(Manufacturing Engineering and Materials Processing 59) Suresh G. Advani, E. Murat Sozer-Process Modeling in Composites Manufacturing-Marcel Dekker (2003)

Process Modeling
in Composites Manufacturing
Suresh G. Advani
University of Delaware
Newark, Delaware
E. Murat Sozer
Koc University
Istanbul, Turkey
MARCEL DEKKER, INC. NEW YORK • BASEL

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MANUFACTURING ENGINEERING AND MATERIALS PROCESSING
A Series of Reference Books and Textbooks
EDITOR
loan Marinescu
University of Toledo
Toledo, Ohio
FOUNDING EDITOR
Geoffrey Boothroyd
Boothroyd Dewhurst, Inc.
Wakefleld, Rhode Island
1. Computers in Manufacturing, U. Rembold, M. Seth, and J. S. Weinstein

2. Cold Rolling of Steel, William L. Roberts
3. Strengthening of Ceramics: Treatments, Tests, and Design Applications, Harry P.
Kirchner
4. Metal Forming: The Application of Limit Analysis, Betzalel Avitzur
5. Improving Productivity by Classification, Coding, and Data Base Standardization: The
Key to Maximizing CAD/CAM and Group Technology, William F. Hyde
6. Automatic Assembly, Geoffrey Boothroyd, Corrado Poll, and Laurence E. Murch
7. Manufacturing Engineering Processes, Leo Alting
8. Modern Ceramic Engineering: Properties, Processing, and Use in Design, David W.
Richerson
9. Interface Technology for Computer-Controlled Manufacturing Processes, Ulrich
Rembold, Karl Armbruster, and Wolfgang Ulzmann
10. Hot Rolling of Steel, William L. Roberts
11. Adhesives in Manufacturing, edited by Gerald L. Schneberger
12. Understanding the Manufacturing Process: Key to Successful CAD/CAM
Implementation, Joseph Harrington, Jr.
13. Industrial Materials Science and Engineering, edited by Lawrence E. Murr
14. Lubricants and Lubrication in Metalworking Operations, Elliot S. Nachtman and
Serope Kalpakjian
15. Manufacturing Engineering: An Introduction to the Basic Functions, John P. Tanner
16. Computer-Integrated Manufacturing Technology and Systems, Ulrich Rembold,
Christian Blume, and Ruediger Dillman
17. Connections in Electronic Assemblies, Anthony J. Bilotta
18. Automation for Press Feed Operations: Applications and Economics, Edward Walker
19. Nontraditional Manufacturing Processes, GaryF. Benedict
20. Programmable Controllers for Factory Automation, David G. Johnson
21. Printed Circuit Assembly Manufacturing, Fred W. Kear
22. Manufacturing High Technology Handbook, edited by Donates Tijunelis and Keith E.
McKee
23. Factory Information Systems: Design and Implementation for CIM Management and
Control, John Gaylord
24. Flat Processing of Steel, William L. Roberts
25. Soldering for Electronic Assemblies, Leo P. Lambert
26. Flexible Manufacturing Systems in Practice: Applications, Design, and Simulation,
Joseph Talavage and Roger G. Hannam
27. Flexible Manufacturing Systems: Benefits for the Low Inventory Factory, John E. Lenz
28. Fundamentals of Machining and Machine Tools: Second Edition, Geoffrey Boothroyd
and Winston A. Knight
29. Computer-Automated Process Planning for World-Class Manufacturing, James Nolen
30. Steel-Rolling Technology: Theory and Practice, Vladimir B. Ginzburg
31. Computer Integrated Electronics Manufacturing and Testing, Jack Arabian

32. In-Process Measurement and Control, Stephen D. Murphy
33. Assembly Line Design: Methodology and Applications, We-Min Chow
34. Robot Technology and Applications, edited by Ulrich Rembold
35. Mechanical Deburring and Surface Finishing Technology, Alfred F. Scheider
36. Manufacturing Engineering: An Introduction to the Basic Functions, Second Edition,
Revised and Expanded, John P. Tanner
37. Assembly Automation and Product Design, Geoffrey Boothroyd
38. Hybrid Assemblies and Multichip Modules, Fred W. Kear
39. High-Quality Steel Rolling: Theory and Practice, Vladimir B. Ginzburg
40. Manufacturing Engineering Processes: Second Edition, Revised and Expanded, Leo
Alting
41. Metalworking Fluids, edited by Jerry P. Byers
42. Coordinate Measuring Machines and Systems, edited by John A. Bosch
43. Arc Welding Automation, Howard B. Cary
44. Facilities Planning and Materials Handling: Methods and Requirements, Vijay S.
Sheth
45. Continuous Flow Manufacturing: Quality in Design and Processes, Pierre C.
Guerindon
46. Laser Materials Processing, edited by Leonard Migliore
47. Re-Engineering the Manufacturing System: Applying the Theory of Constraints,
Robert E. Stein
48. Handbook of Manufacturing Engineering, edited by Jack M. Walker
49. Metal Cutting Theory and Practice, David A. Stephenson and John S. Agapiou
50. Manufacturing Process Design and Optimization, Robert F. Rhyder
51. Statistical Process Control in Manufacturing Practice, Fred W. Kear
52. Measurement of Geometric Tolerances in Manufacturing, James D. Meadows
53. Machining of Ceramics and Composites, edited by Said Jahanmir, M. Ramulu, and
Philip Koshy
54. Introduction to Manufacturing Processes and Materials, Robert C. Creese
55. Computer-Aided Fixture Design, Yiming (Kevin) Rong and Yaoxiang (Stephens) Zhu
56. Understanding and Applying Machine Vision: Second Edition, Revised and
Expanded, Nello Zuech
57. Flat Rolling Fundamentals, Vladimir B. Ginzburg and Robert Bellas
58. Product Design for Manufacture and Assembly: Second Edition, Revised and
Expanded, Geoffrey Boothroyd, Peter Dewhurst, and Winston Knight
59. Process Modeling in Composites Manufacturing, Suresh G. Advani and E. Mural
Sozer
60. Integrated Product Design and Manufacturing' Using Geometric Dimensioning and
Tolerancing, Robert G. Campbell and Edward S. Roth
Additional Volumes in Preparation
Handbook of Induction Heating, Valery Rudnev, Don Loveless, and Ray Cook

Dedication
to our families:
Yolanda Chetwynd, Madhu and Diana Advani;

and
Hanife, Zehra and Eray Sozer.

Preface
Properties and performance of products made from fiber reinforced composites depend on
materials, design, and processing. This book is about polymer composites processing. Three
decades ago our understanding of mass, momentum, and energy transfer during composites
processing was nonexistent. As a result, almost all manufacturing was based on experience,
intuition and trial and error. We have come a long way since then. Many researchers did
delve into this difficult and poorly understood area to uncover the physics and chemistry of
processing and to develop the fundamental and constitutive laws to describe them.
There is currently a wealth of literature on modeling and simulation of polymer com-
posite manufacturing processes. However, we felt that there was a need to systematically
introduce how one would go about modeling a composite manufacturing process. Hence,
we focused on developing a textbook instead of a researcher's reference book to provide an
introduction to modeling of composite manufacturing processes for seniors and first-year
graduate students in material science and engineering, industrial, mechanical, and chemical
engineering. We have explained the basic principles, provided a primer in fluid mechanics
and heat transfer, and tried to create a self-contained text. Many example problems have
been solved to facilitate the use of back-of-the-envelope calculations to introduce a scientific
basis to manufacturing. The end of each chapter has questions and problems that reinforce
the content and help the instructor. "Fill in the Blanks" sections were created by Murat
Sozer to add to the qualitative knowledge of process modeling of composites manufacturing
that will develop the "experience base" of the manufacturing, materials, and design engineer
or scientist.
A project of this magnitude obviously cannot be realized without the help of others.
First, we thank Mr. Ali Gokce, graduate student at the University of Delaware, who created
many of the graphics in this book. Diane Kukich helped in technical editing. Of course we
thank all the graduate students in our research group who over the years have helped create
the research and the science base to develop models of composite manufacturing processes.
We would especially like to mention Petri Hepola, Steve Shuler, Terry Creasy, Krishna
Pillai, Sylvia Kueh, Simon Bickerton, Hubert Stadtfeld, Pavel Nedanov, Pavel Simacek,
Kuang-Ting Hsiao, Gonzalo Estrada, Jeffery Lawrence, and Roopesh Mathur. Some of the
examples and figures used in the book were first developed with their help.
The book contains eight chapters. The first two introduce the composite materials and
manufacturing processes. Chapters 3-5 provide the tools needed to model the processes,
and Chapters 6—8 apply these tools to some of the well known manufacturing processes.

Contents
Preface
1 Introduction
1.1 Motivation and Contents
1.2 Preliminaries
1.3 Polymer Matrices for Composites
1.3.1 Polymer Resins
1.3.2 Comparison Between Thermoplastic and Thermoset Polymers
1.3.3 Additives and Inert Fillers
1.4 Fibers
1.4.1 Fiber-Matrix Interface
1.5 Classification
1.5.1 Short F
1.5.2 Advanced Composites
1.6 General Approach to Modeli
1.7 Organization of the Book
1.8 Exercises
1.8.1 Qu
1.8.2 Fill in the Blanks
2 Overview of Manufacturing Processes

2.1 Background
2.2 Classificatio
2.3 Short Fiber Suspension Manufacturing Methods
2.3.1 Injection Molding
2.3.2 Extrusion
2.3.3 Compression Molding
2.4 Advanced Thermoplastic Manufacturing Methods
2.4.1 Sheet Forming
2.4.2 Thermoplastic Pultrusion
2.4.3 Thermoplastic Tape Lay-Up Process
2.5 Advanced Thermoset Composite Manufacturing Methods
2.5.1 Autoclave Processing
2.5.2 Liquid Composite Molding
2.5.3 Filament Winding
2.6 Exercises
2.6.1 Questions

3 Transport Equations for Composite Processing
3.1 Introduction to Process Models
3.2 Conservation of Mass (Continuity Equation)
3.2.1 Conservation of Mass
3.2.2 Mass Conservation for Resin with Presence of Fiber
3.3 Conservation of Momentum (Equation of Motion)
3.4 Stress-Strain Rate Relationship
3.4.1 Kinematics of Fluid
3.4.2 Newtonian Fluids
3.5 Examples on Use of Conservation Equations to Solve Viscous Flow Problems
3.5.1 Boundary Conditions
3.5.2 Solution Procedure
3.6 Conservation of Energy
3.6.1 Heat Flux-Temperature Gradient Relationship
3.6.2 Thermal Boundary Conditions
3.7 Exercises
3.7.1 Questions
3.7.2 Problems
4 Constitutive Laws and Their Characterization

4.1 Introduction
4.2 Resin Viscosity
4.2.1 Shear Rate Dependence
4.2.2 Temperature and Cure Dependence
4.3 Viscosity of Aligned Fiber Thermoplastic L
4.4 Suspension Viscosity
4.4.1 Regimes of Fib
4.4.2 Constitutive Equations
4.5 Reaction Kinetics
4.5.1 Techniques to Monitor Cure: Macroscopic Characterization
4.5.2 Technique to Monitor Cure: Microscopic Characterization
4.5.3 Effect of Reinforcements on Cure Kinetics
4.6 Crystallization Kinetics
4.6.1 Introduction
4.6.2 Solidification and Crystallization
4.6.3 Background
4.6.4 Crystalline Structure
4.6.5 Spherulitic Growth
4.6.6 Macroscopic Crystallization
4.7 Permeability
4.7.1 Permeability and Preform Parameters
4.7.2 Analytic and Numerical Characterization of Permeability
4.7.3 Experimental Characterization of Permeability
4.8 Fiber Stress
4.9 Exercises
4.9.1 Questions
4.9.3 Problems

5 Model Simplifications and Solution
5.1 Introduction
5.1.1 Usefulness of Models
5.2 Formulation of Models
5.2.1 Problem Definition
5.2.2 Building the Mathematical Model
5.2.3 Solution of the Equations
5.2.4 Model Assessment
5.2.5 Revisions of the Model
5.3 Model and Geometry Simplifications
5.4 Dimensionless Analysis and Dimensionless Numbers
5.4.1 Dimensionless Numbers Used in Composites Processing
5.5 Customary Assumptions in Polymer Composite
Processing
5.5.1 Quasi-Steady State
5.5.2 Fully Developed Region and Entrance Effects
5.5.3 Lubrication Approximation
5.5.4 Thin Shell Approximation
5.6 Boundary Conditions for Flow Analysis
5.6.1 In Contact with the Solid Surface
5.6.2 In Contact with Other Fluid Surfaces
5.6.3 Free Surfaces
5.6.4 No Flow out of the Solid Surface
5.6.5 Specified Conditions
5.6.6 Periodic Boundary Condition
5.6.7 Temperature Boundary Conditions
5.7 Convection of Variables
5.8 Process Models from Simplified Geometries
5.8.1 Model Construction Based on Simple Geometries
5.9 Mathematical Tools for Simplification
5.9.1 Transformation of Coordinates
5.9.2 Superposition
5.9.3 Decoupling of Equations
5.10 Solution Methods
5.10.1 Closed Form Solutions
5.11 Numerical Methods
5.12 Validation
5.12.1 Various Approaches for
5.13 Exercises
5.13.1 Questions
5.13.2 Problems
6 Short Fiber Composites

6.1 Introduction
6.2 Compression Molding
6.2.1 Basic Processing Steps [1
6.2.2 Applications [1]
6.2.3 Flow Modeling
6.2.4 Thin Cavity Models
6.2.5 Hele-Shaw Model

6.2.6 Lubricated Squeeze Flow Model
6.2.7 Hele-Shaw Model with a Partial Slip Boundary Condition [2]
6.2.8 Heat Transfer and Cure
6.2.9 Cure
6.2.10 Coupling of Heat Transfer with Cure
6.2.11 Fiber Orientation
6.3 Extrusion
6.3.1 Flo
6.3.2 Calculation of Power Requirements [3]
6.3.3 Variable Channel Length [3]
6.3.4 Newtonian Adiabatic Analysis [3]
6.4 Injection Molding
6.4.1 Process Description
6.4.2 Materials
6.4.3 Applications
6.4.4 Critical Issues
6.4.5 Model Formulation for Injection Molding
6.5 Exercises
6.5.1 Questions
6.5.3 Problems
7 Advanced Thermoplastic Composite Manufacturing Processes

7.1 Introduction
7.2 Composite Sheet Forming Processes
7.2.1 Diaphragm Forming
7.2.2 Matched Die Forming
7.2.3 Stretch and Roll Forming
7.2.4 Deformation Mechanisms
7.3 Pultrusion
7.3.1 Thermoset Versus Thermoplastics Pultrusion
7.3.2 Cell Model [4]
7.4 Thermal Model
7.4.1 Transient Hea
7.4.2 Viscous Dissipation
7.5 On-line Consolidation of Thermoplastics
7.5.1 Introduction to Consolidation Model
7.5.2 Importance of Process Modeling
7.5.3 Consolidation Process Model
7.5.4 Model Assumptions and Simplifi
7.5.5 Governing Equations
7.5.7 Rheology of the Com
7.5.8 Model Solutions
7.5.9 Inverse Problem of Force Control
7.5.10 Extended Consolidation Model
7.6 Exercises
7.6.1 Questions

8 Processing Advanced Thermoset Fiber Composites
8.1 Introduction
8.2 Autoclave Molding
8.2.1 Part Prepar
8.2.2 Material and Proc
8.2.3 Processing Steps
8.2.5 Flow Model fo utoclave Proces
8.3 Liquid Composite Molding
8.3.1 Similarities and Dif
8.3.2 Important Components of LCM Processes
8.3.3 Modeling the Process Issues in LCM
8.3.4 Process Models
8.3.5 Resin Flow
8.3.6 Heat Transf d Cure
8.3.7 Numerical Simulation of n LC
8.4 Filament Winding of Thermosetting Matrix Composites
8.4.1 Introduction
8.4.2 Process Model
8.5 Summary and Outlook
8.6 Exercises
8.6.1 Qu
8.6.2 Fill in the
8.6.3 Problems
Bibliography

Chapter 1
Introduction
1.1 Motivation and Contents

Polymer Composites have been in use for a few decades now. Their advantages over other
materials for high-performance, lightweight applications have attracted many industries
such as aerospace, automobile, infrastructure, sports and marine to explore and increase
their usage. The path to the design and manufacturing of composite structures was pur-
sued in evolutionary as well as revolutionary ways. They ranged from using hand layup
with labor and cost intensive autoclave processing to the use of automated processes such
as injection molding and extrusion, traditionally employed by the polymer processing in-
dustry. Many new manufacturing techniques were invented and introduced during the last
two decades, and some of them were incrementally improved to increase the yield of man-
ufactured composite parts. The process engineer has relied on experience and "trial and
error" approaches to improve the manufacturability of a prototype. Very little analysis of
process physics and back-of-the-envelope calculations were done to approach a prototype
development of a composite structure. Even the choice of the process was dictated by fa-
miliarity and experience rather than appropriateness and methodology. This has proved to
be very expensive. However, in the last decade the composites manufacturing industry has
come under intense pressure to be cost-effective and focus on cost avoidance in prototype
development. Design and manufacturing engineers have resorted to use of process modeling
and simulations to address some of these concerns. The virtues of virtual manufacturing
are becoming more obvious to the manufacturing engineer when formulating the guidelines
and methodology for the design and manufacturing of composites.
As a result, many books on composites manufacturing have been written in the last
few years. They have served as good research references for the composites manufacturing
engineers and personnel. The underlying science for many of these manufacturing processes
is described by a process model and incorporated into simulations to allow one to perform
trial and error experiments in virtual space instead of the laboratory space. Currently, the
available books are either chapters written by multiple authors on different processes which
summarize the state of the art in the field and are excellent research reference materials
[5, 6, 7] or they paint a broad brush on the qualitative aspects of manufacturing of composite
materials with polymer, ceramics and metal matrices [8]. Thomas Astrom's book [9] is an
excellent book to get practical information about the manufacturing process as well as a
great resource for property data. The book gives a very detailed qualitative insight into
the materials and processes addressing the issues encountered from designing to shop floor
manufacturing.

Our book will have two complementary focuses as compared to the recent books written
on composites manufacturing. First, this book will introduce to the reader the approach to
model the processing operation during composite manufacturing using fundamental prin-
ciples. The most important aspect will be to identify the key transport phenomena that
surface during the manufacturing process and the approach to incorporate them in a process
model. Thus, it will reduce the reliance on the trial and error methodology used to achieve
an acceptable composite part and will increase the use of science base in the manufactur-
ing process. Second, as the reader or practitioner understands more about the physics of
the process and the transport phenomena that drive the process, he or she will be in a
position to invent a novel composite processing method that can improve upon the existing
manufacturing methods. This could attract many more industries to accelerate insertion of
composite materials into their products.
In this book, we will restrict ourselves to modeling the processing step of the poly-
mer composite fabrication process, although the modeling philosophy could be extended to
manufacturing processes with other materials. The book is written with the undergraduate
senior and the first year graduate student in mind who has some understanding of the basics
of fluid mechanics and heat transfer and ordinary and partial differential equations. A brief
introduction of useful equations in fluid mechanics and heat transfer will be presented as a
primer for those unfamiliar with the subject and should serve as a refresher for those who
can't quite recall the details.
1.2 Preliminaries
Composite materials generically consist of two different materials that are combined to-
gether. In engineering, the definition can be narrowed down to a combination of two or
more distinct materials into one with the intent of suppressing undesirable constituent
properties in favor of the desirable ones. Atomic level combinations such as metal alloys
and polymer blends are excluded from these definitions [9]. However, with the invention
of nanocomposites, one can probably group alloys and blends also under the umbrella of
composites.
In polymer composites, the individual constituents are polymer resin and fibers as shown
in Figure 1.1. The role of the polymer resin, which is also called the matrix phase of
the composite, is to primarily bind the fibers together, give the composite a nice surface
appearance in addition to environmental tolerance and provide overall durability. The fibers,
also known as the reinforcing phase, carry the structural load, reduce thermal stresses and
provide macroscopic stiffness and strength [8, 9]. The polymer matrix is either a thermoset
or a thermoplastic material. The fibers are made from glass, carbon or polymer. Some of
the fiber forms are shown in Figure 1.2.
From the processing and manufacturing viewpoint, the type of matrix plays an important
role. Thermoset materials are only 50 to 500 times more viscous than water and can
impregnate the empty spaces between the fibers readily. They do require an additional
processing step which involves chemical reaction of cross-linking the polymer chains known
as curing. This is schematically shown in Figure 1.3. On the other hand, thermoplastic
materials do not require this step but are highly viscous. Their viscosity can be as high
as a million times more than that of water. Hence, it is difficult to make them flow and
fill the tiny empty spaces between the reinforcing fibers. Figure 1.4 displays the important
differences between thermoplastics and thermosets. The constitutive equations that describe
the chemorheology of the matrix materials such as the influence of temperature, shear rate
and degree of cure on the viscosity will play an important role in the processing step during

, <*%•
I + f„
•
M» JjnK
•""• X"» -
Fabric
\ Resin
Composite
Figure 1.1: Fiber composite made from fibers and resin.
FIBERS
Carbon Tapes and Fabric
Figure 1.2: Different fiber forms.

liquid solid
• Chemical reaction
• Heat evolution
• Volatiles evolution
• Increase in viscosity
• Gelation
• Vitrification
Figure 1.3: Curing is the process of cross-linking a thermoset polymer.
Thermoplastics Thermosets
Recycles Cures
High Viscosity Low Viscosity
Figure 1.4: Polymer resin types used to make composites.
the composite manufacturing process.

Glass and carbon are the most common materials used for the fibers. The fiber material
usually will not influence the modeling of the manufacturing process in a very significant
way. However, whether the fibers are discontinuous or continuous will influence the modeling
approach. Also, if the fibers are discontinuous, their aspect ratio (the ratio of fiber length
to its diameter) will be important during processing, and if the fibers are continuous then
their fiber architecture will play a major role in the manufacturing process. The continuous
fibers can be introduced into the polymer matrix as unidirectional fiber arrays or by utilizing
appropriate fabrication methods, e.g. weaving, braiding, knitting, or stitching, shaped
into 2-D or 3-D reinforcing fabrics before being embedded. Some of these structures are
displayed in Figures 1.5 and 1.6. In general, the ease of processing decreases as we move
from discontinuous short fibers to continuous fiber preforms that are woven or stitched as
schematically shown in Figure 1.7.
1.3 Polymer Matrices for Composites
The polymer matrix in a composite will consist mainly of a thermoplastic or thermoset

resin. In addition, it may contain small quantities of additives, inert fillers and adhesives.

Random fabric Stitched Fabric
i: v
.-.:§V^:5
; '";£ vi* f$K£ V-i
V /* • ". •• • i *& ?'.' •* -..-"^^x
, • ** ».**•**. «"T »*«. ^t* '• I'.*'*""»•'• *."* •*- IT
Weave Fabrics:
Plain
(1 over, 1 under)
8 Harness 5 Harness
(7 over, 1 under) (4 over, 1 under)
I I I I 1
Figure 1.5: Typical fabrics and schematics with continuous fibers.

Biaxial Triaxial Knit Multiaxial Multilayer
Weave Weave Warp Knit
3-D Cylindrical 3-D Braiding 3-D Orthogonal Angle-Interlock

Construction Fabric Construction
Figure 1.6: More detailed architectures of reinforcing fiber preforms [10].
Relative
0) Processability
o
c
o Relative
o Performance
(Strength/Stiffness)
I
o
0)
0)
(0
LU
Melt Flow Random Discontinuous Continuous

Oriented Chopped Collimated Fiber
(Injection Strands Fibers System
Molded) (SMC)
Figure 1.7: Schematic of role of fiber form on processing and performance [11].

1.3.1 Polymer Resins
Polymers or plastics are high molecular weight (MW) compounds consisting of many (poly)
repeated small segments (mers). They possess the characteristic of a chemical reaction
utilizing the smallest building block, the monomer, and assembling approximately 103 up
to 106 of these blocks into a polymer. There are two different types of reactions that can
be used to create all modern polymers: poly-condensation and poly-addition. They can all
produce linear or branched polymers. The primary bonds formed between the molecules
are the strong covalent bonds. However, the molecules also form secondary bonds which
are an order of magnitude weaker than the covalent bonds. These bonds are due to van der
Waals' forces.
Polymers are classified as thermoplastics or cross-linked polymers such as elastomers or
thermosets. Thermoplastic polymers can be either amorphous (without regular structure),
see Figure 1.8(a), or semicrystalline (amorphous base structure with embedded regular
substructures), displayed in Figure 1.8(b).
" r"* ,'- f- -" f~ '
(c) A
<•»'
Figure 1.8: Schematic of the molecular structure: a) Amorphous Thermoplastic, b) Semi-

crystalline Thermoplastic, c) Elastomer and d) Thermoset [12].
The thermoplastic properties are determined by the resulting microstructure, which is

strongly influenced by the cooling dynamics. In general, an amorphous polymer is trans-
parent, has lower mechanical properties and is less resistant to other chemicals than the
semicrystalline thermoplastics. Thermoplastic polymers can be best compared to a plate
of spaghetti. Each noodle can be thought of as a long chain of repetitive molecules. When
it is heated, the molecules can move around. If cooled quickly, the current arrangement of
the noodles or molecule chains can be frozen due to the van der Waals' forces. If cooled
slowly, the molecules align themselves in regular crystal formation which is the lowest pos-
sible energy state for the arrangement of molecules. As there are only secondary bonds
between the molecules, thermoplastics can be melted and reformed. If the molecules are
in an orderly form they are known as semicrystalline. If they are randomly organized they
are known as amorphous. Hence thermoplastics can be cooled in amorphous form or with
various degrees of crystallinity. Crystalline state packs better than the amorphous state.
However, it is not possible to get 100% crystalline state. The resulting degree of crystallinity
depends on pressure, molecular weight, temperature and most importantly cooling rate, as
shown in Figure 1.9. Note that Tg in the figure refers to the glass transition temperature.
At this temperature, one expects the secondary bonds to initiate breaking. The molecules

continue to slide over one another with relative ease, and flow is possible. The softening
occurs over a temperature range of 50-80°C. When a shear force is applied to the bulk
material, the long chain molecules will start to slide relative to each other, in response to
the applied force. Thus most thermoplastic resins exhibit shear thinning behavior, which is
an important property to consider when one develops the process model. This causes the
thermoplastic resin viscosity to decrease with temperature and applied shear as shown in
Figure 1.10.
o
Tm Temperature
Figure 1.9: Change in crystallization rate as a function of temperature. Tg is the glass

transition temperature and Tm is the melting temperature.
10
CD
CL
10
10
Y(s 1 )
Figure 1.10: Change in viscosity as a function of temperature and applied shear for
polypropylene resin [9].
In Figure 1.8(c), one can notice the slightly cross-linked structure of an elastomer. Its
structure can be compared and modeled as a network of springs to capture their rubber
like character. Figure 1.8(d) shows the molecular structure of the family of thermosets.
Both thermosets and elastomers always cure to form an amorphous structure. Thermosets
initially consist of long chain molecules with weak bonds. Chemical reactions can initiate
covalent bonds that cross-link and cannot be melted. The high density of cross-linking
within the thermoset structure is responsible for the superior thermal stability and the

mechanical properties, as can be seen in Table 1.1 [13]. The materials selected in Table 1.1
reflect the most commonly used thermoplastics and thermosets. Thermoplastics are listed
first followed by the thermosets.
Table 1.1: Properties and typical applications for commonly used polymers [14].
Name / Abbreviation Material Application Important Application
Family Temperature Properties Examples
Range (C)
Polyethylene / PE Thermoplastic 100 Low strength, high Bottles, fuel tanks,
ductility, resists most sealing material, tub-
chemicals ing, plastic films
Polypropylene / PP Thermoplastic 110 In general, better Suitcases, tubing, en-
properties than PE closures, bottles
Polyvinylchloride / PVC Thermoplastic 60 Good chemical resis- Flooring material,
tance plastic films, tubing
Polytetrafluorethylen / PTFE Thermoplastic -200 to +270 Highest chemical Lab. Equipment,
resistance, strongest coatings (pans, etc.)
anti-adhesive
Poliamide / PA Thermoplastic -40 to +120 High strength and Ropes, bearings,
ductility gears, dowels
Polyethylentherephthalate / PET Thermoplastic 110 Low creeping ten- Most soda bottles,
dency, clear miniature parts,
parts with small
tolerances
Polycarbonate / PC Thermoplastic -100 to +130 High strength and Visors for helmets,
ductility, clear safety glasses, quality
flatware
Polyacrylate / PMMA Thermoplastic 70 Excellent optical Magnifying glasses,
properties (organic lenses of all kind,
glass), easy bonding showcases
Polystyrole / PS Thermoplastic 60 High strength, brit- Wrapping film, low
tle, glass clear, low quality cutlery and
chem. resistance plastic cups
Unsaturated Polyester / UP Thermoset 100 to 180 High tensile strength Structural parts for
(close to steel), good boats and cars, fish-
chemical resistance ing rods
Epoxy / EP Thermoset 80 to 200 Structural parts in Helicopter rotor
airplanes with high blades, fuselage,
demands for stiffness commonly used as
and strength adhesive
Phenolics / PF Thermoset 150 High strength and Enclosures, printed
stiffness, brittle circuit boards
Vinylesters / VE Thermoset 200 Room curing, high Applications in ma-
chem. resistance, rine industry, corro-
good strength and sion resistant tanks
ductility and pipes
1.3.2 Comparison Between Thermoplastic and Thermoset Polymers

A key difference between thermoplastics and thermosets is that one needs to apply heat to
melt a thermoplastic and hence initiate a phase change from solid to liquid before or during
processing, whereas thermosets are generally provided by the manufacturer in the liquid
phase. However, some thermosets such as phenolics and unsaturated polyesters are solid at
room temperature and need to be heated to convert them into liquids. A diluent/solvent
is added to thermosets to lower their viscosity. After processing, the thermoplastic melt

must be cooled down to solidify it, whereas the thermoset will turn into a solid after it is
chemically and thermally activated to form the cross-linked network which is also referred
to as curing. If the material viscosity is low, it is easy to get it to flow in the empty
spaces between the fibers and/or into a mold. Thermoset viscosity is usually between 0.050
to 0.500 Pa.s. Thermoplastics at room temperature are solid, but their viscosity around
the processing temperature range is between 102 and 106 Pa.s. Also, thermoplastics exhibit
non-Newtonian behavior such as shear thinning of the viscosity with applied stress, whereas
thermosets are relatively insensitive to shear. All polymers exhibit reduction in viscosity
with temperature, although thermoplastics can exhibit a steeper reduction than thermosets.
A variety of different material viscosities are compared in Table 1.2.
A general comparison between thermoplastic and thermoset matrices is depicted in Table
1.3.
Table 1.2: Comparison of different material viscosities [13].

Material Viscosity [Pa.s] Consistency
Air io-53 Gaseous
Water io- Thin-bodied
Glycerin 1 Liquid
Thermosets 0.05 to 0.5 Liquid
Molten thermoplastics at
IO 2 to IO6 Thick-flowing
processing temperature
21
Glass IO Solid
Table 1.3: Summary of differences between thermoplastics and thermosets from processing
viewpoint.
Characteristic Thermoplastics Thermosets
Viscosity High Low
Initial state Usually solid Usually liquid
Post processing None Heat necessary
Reversibility Can be remelted and re- Once formed, vir-
formed gin state cannot be
recovered
Heat transfer requirement Heat needed to melt it Heat may be need to ini-
tiate cure
Processing temperature Usually high Can be at room temper-
ature
Usage Large volumes in injec- Mainly used in ad-
tion molding vanced composites
Solidification Cooling for change of Extraction of exother-
phase mic heat during curing

1.3.3 Additives and Inert Fillers
Additives are added to the matrix to change processibility, shrinkage, and mechanical and
optical properties. For thermosets, small amounts of additives are added which are cross-
linking agents that can initiate, inhibit or accelerate the reaction. For thermoplastics,
plasticizers are added which are low molecular weight compounds to lower the viscosities.
Inert fillers are added to the resin to improve stiffness, electrical properties, decrease
shrinkage, provide resistance to ultraviolet radiation, and reduce resin usage for low cost
applications. Fillers as colorants do not require expensive painting.
1.4 Fibers
Reinforcements carry structural loads and provide stiffness and strength to the composite.
They can be in the form of particles, whiskers or fibers. Particles or flakes have a low aspect
ratio of the diameter to the length, whiskers are usually 0.1 micron in diameter and made
from a single crystal. Particles do not provide a substantial change in mechanical properties
and whiskers are too expensive to manufacture.
Fibers are usually spun from a solution or a melt which orients the molecules of the
material. They are made from either glass, carbon or polymer. Their diameter is usually
less than 10 /um. Fibers come in various forms, shapes and materials and are primarily
used for reinforcements. Composites containing continuous fibers are known as advanced
composites. Composites containing discontinuous fibers are called short fiber or long fiber
reinforced plastics.
For advanced composites, the fibers are used in the form of rovings, yarns, strands and
tows. These yarns or tows can be combined in various forms to create a preform. Some of
these structures are shown in Figures 1.5 and 1.6.
Figure 1.11: A network of fiber tows containing 1000 to 2000 fibers in each tow stitched
together to form the fabric.
Many preforms are formed using fabric reinforcements. Fabrics are formed from a net-
work of continuous fibers. One large class of fabrics is manufactured by either weaving or
stitching together bundles ("tows") of fibers. These tows are generally elliptical in cross
section, and may contain from 100 to 48000 single fibers as can be seen in Figure 1.5. The
cross sectional width and thickness of tows are of the order of millimeters, as can be seen
in Figure 1.11. Another large class of preform fabrics include "chopped" and "continuous
strand" random mat also shown in Figure 1.5. These fabrics are typically formed from
low cost E-glass fibers, cheaper than woven and stitched fabrics, and used for low-strength

applications. These fabrics are formed using smaller tows (approximately 100 fibers), and
have a structure which is more random in nature than woven or stitched fabrics. Random
mats are typically isotropic in their structural and flow properties, which is often untrue
for woven or stitched fabrics.
Fiber tows can be formed into three dimensional shapes using braiding and weaving
techniques. Tows can be oriented at different angles in 3-dimensional space, providing
structural support in a multitude of directions, depending upon the application. A fiber
preform is an assembly of fabrics. Figure 1.12 shows a complex preform constructed from
woven fabric that forms the skeleton of the shape of the composite part. Such preforms
are typically used for advanced composites. From the mold filling process viewpoint, the
architecture of the preforms dictates the resistance to the flow of resins.
>j<£^££--' >•••••• •'• •••^.«'v,;, ./W..W.,,,,
Figure 1.12: Fiber preform constructed from woven fabrics and placed in a mold that forms
a skeleton of the composite part.
It is difficult to stack the layers in a desired orientation when draping multi-layers of

a dry fabric preform over a tool surface. Use of preimpregnated fabrics (prepregs) or a
tackifier (a binder that holds various layers together) eases the preforming and draping
process for various net-shape structures [15]. This also reduces the chance of fiber wash
(movement of the fibers) during the resin injection.
1.4.1 Fiber-Matrix Interface

A strong bond between the fiber and the matrix will improve the interlaminar shear strength,
delamination resistance, fatigue properties and corrosion resistance. However a weak bond
is useful for damage tolerance and energy absorption. The interface area between the fibers

and the resin is given approximately by four times the volume fraction of the fibers divided
by the diameter of the fiber. The interface area for a small volume of 1 meter by 1 meter by
2 centimeter composite part containing 50% fibers can be the size of a baseball field (about
10,000 square meters) if the fiber diameter is a few microns [6].
A good bond between the fiber and the matrix is created by wetting of the fiber by the
resin. The thermodynamics of wetting states that low energy liquids wet high energy solids.
The surface energy for glass is around 500 dynes/cm2 and for the polymers it is around
30-40 dynes/cm2. Hence, glass is a great wetting agent. Carbon has a surface energy of
around 50 dynes/cm2 and can still be easily wetted by the resin. Addition of sizing to the
fibers promotes handling but can inhibit wetting. Thermodynamics can tell you if the resin
will wet the fibers but does not tell you the rate of wetting and if we can get the resin to
reach the fiber surface. For this we have to understand how the resin flows and impregnates
between the fiber surfaces.
1.5 Classification
Thermosets have been around much longer than thermoplastic materials; hence almost all
manufacturing techniques developed for thermoplastics today were originally derived from
the processes that used thermoset matrices, and the most important ones are listed in Table
1.4. The practice of choosing an appropriate manufacturing method is usually based on the
actual part size and geometry, the unit count, the precursor material (initial state of the
composite material), the selected components of the composite, i.e. the reinforcement and
the matrix, and the cost.
1.5.1 Short Fiber Composites

The fibers can be cut or chopped and compounded in an extruder with any polymer to
form a pellet consisting of short fibers or could be pultruded consisting of aligned fibers as
shown in Figure 1.13.
cut or chopped fibers , aligned fibers
(a) compounded pellet (b) pultruded pellet
Figure 1.13: Schematic of pellets for injection molding.
The first generation of composites used chopped or short fibers preimpregnated with
the thermoplastic polymer matrix in the form of pellets. The pellets are usually a few
centimeters in length and a few millimeters in diameter.
The composite types can be broadly divided into composites made from short fibers
(aspect ratio less than 100) and continuous fibers. The three most common mass produc-
tion processes for short fiber composites manufacturing are injection molding, compression

Table 1.4: Examples of composite manufacturing processes.
Process Precursor Tooling Production
Materials
Injection Molding Pellets with short Aluminium or Small complex
fibers steel molds shape parts, high
volume
Extrusion Pellets with short Dies for continu- Tubes, T-
fibers ous operation sections, any
cross-sectionally
long part
Compression Molding Laminates with Aluminium or Large net shape
long discontin- steel molds parts such as
uous fibers or wind deflectors
continuous fibers
Wet layup and Tape Layup Unidirectional One sided steel Small low curva-
continuous fiber mold ture parts.
prepregs
Autoclave Unidirectional One sided steel Part size limited
continuous fiber mold by autoclave size
prepregs
Filament Winding Prepregs or fiber Open mold Usually axi-
rovings process over symmetric parts
a mandrel with hollow cores
(steel/aluminum)
Liquid Molding Random, woven, Closed mold Near-net shape
knitted fabric pre- process with alu- parts
forms in any form minium or steel
mold
Pultrusion Uni-directional Closed die made Continuous cross-
tape or fabric of steel section parts
rovings
Sheet Forming Pre-impregnated Metal mold Parts with slight
sheets curvatures

molding and extrusion. These processes were adopted from the polymer processing industry
that had developed the equipment to produce parts in high volumes with polymers.
These pellets were fed into the hopper of either an injection molding machine or an
extruder. The polymer contained in the pellets melts inside the barrel of the machine
because of the heating and viscous dissipation due to the shearing of the polymer against
the barrel and the screw. The short fibers suspended in the molten polymer are forced into a
mold cavity along with the polymer in the case of discontinuous operations, such as injection
molding, and through a die in the case of continuous operations, such as extrusion. Thus, the
existing machines used for polymer processing could be easily adopted for fiber reinforced
polymers. The advantages were stiffer and stronger components with lower degrees of
warpage and shrinkage. The disadvantage was no control on the fiber orientation in the
component and fiber attrition.
1.5.2 Advanced Composites
From the analysis, it was evident that composites with continuous fibers could enhance
the mechanical properties by one to two orders of magnitude as compared to short fiber
composites. These composites are referred to as advanced composites. There are several
primary steps that are common in manufacturing of advanced composites. First, all ad-
vanced composites require a skeleton structure of the fibers or fiber network that is tailored
for the particular part geometry and the property requirements. Second, this fiber structure
must be covered and impregnated by the liquid resin in some way. Finally, the part should
be supported by a rigid tool to allow the resin to solidify or cross-link, permanently freezing
the microstructure created by the fiber network.
Many fiber structures are available as seen from Figures 1.2, 1.5 and 1.6. Broadly, they
can be divided into two groups. The first group consists of continuous fibers in sheets, tapes
or tows aligned in one direction. These fibers may be prewet with the resin and then laid in
different directions by hand or by a machine to construct the desirable structure. Aligned
fibers allow for creation of very high fiber volume fraction and hence high specific in-plane
strengths and stiffnesses. The second group uses fiber interlacing to create two-dimensional
and three-dimensional interlocked textile structures as shown in Figure 1.6. This can allow
the composite to achieve higher stiffness and strength both in and out of plane directions,
and potentially allow the designer to tailor the mechanical or physical properties to the
desired application. However, as shown in Figure 1.14, the degree of complexity that can
be handled with short fiber composites cannot be duplicated with advanced composites.
Thus, the material manufacturers started to make resin impregnated prepregs with
continuous aligned fibers that could be bonded and fused together to make an advanced
composite. Textile preforms were being made where the fiber tows could be woven, stitched
or braided together to create the underlying microstructure to provide strength to the com-
posite. Various techniques were invented to induce the resin to wet the fibers and infiltrate
the empty spaces between the fibers to retain the integral structure of the composite. This
started the evolution of new composite manufacturing processes to make advanced com-
posites. The details of all the processes are explained very well in [9]. Here, we will briefly
introduce the general approach to model the processing step of composites manufacturing,
and in the next chapter we will briefly introduce some of the important manufacturing
processes and identify the underlying physics of transport of mass, momentum and energy
in these processes.

1.6 General Approach to Modeling
(a)
(b)
Figure 1.14: (a) Injection molded short fiber component with very high degree of geomet-
ric complexity [16]. (b) Resin transfer molded advanced composite with modest level of
geometric complexity [17].
The manufacturing process physics and modeling are greatly influenced by the type of
fibers being used: short or long, continuous or discontinuous, aligned or interlaced, etc. The
type of resins being used, thermoplastic or thermoset, also influences the process. Thus,
the fiber form and the matrix type play a key role in the selection of the manufacturing
process. The geometry of the part to be manufactured influences the decision and also if
the process is carried out in an open mold or a closed mold. These choices influence the
physics of mold filling.
The process modeling step in composite manufacturing is generally approached by re-
searchers on two scales. The macroscale is usually the order of the smallest dimension of
the composite being manufactured (millimeters). The microscale scale is more on the order
of a fiber or tow diameter (microns). At the macroscale, the modeler is generally inter-
ested in the overall relationship between the process parameters (such as pressure, flow rate
and temperature) and global deformation of the composite material that is being formed.
One can use a continuum mechanics approximation to describe this physics. However, as
composite materials are heterogenous materials by definition, macrolevel physics cannot
capture phenomena that occur on the scale of a fiber diameter (usually a few microns).
Hence one may need to model this physics separately and find an approach to couple it
with the macroscale physics.

Broadly, one can divide the manufacturing processes into three different categories on
the macroscale. The first category deals with materials that contain either thermoplastic
or thermoset resin but in.which the precursor material is formed into pellets with short
or chopped fibers. In such cases, once the resin is melted, the fibers and the resin flow
together as a suspension either into a mold or through a die. Hence, the key physics here
is the flow physics of fiber suspensions and the rheology of such suspensions as they deform
under the applied pressure to occupy the mold or the die. Rhelogy is usually defined as the
deformation science of materials. It becomes important to model the transport, attrition
and orientation of the fibers during the flow as the final microstructure is decided by the
resulting frozen-in fiber distribution and orientation. Processes such as extrusion, injection
molding and compression molding fall under this category.
The second category involves long, discontinuous fibers or continuous fibers preimpreg-
nated with viscous thermoplastic resin. In such cases, heat and pressure are applied to form
and consolidate the composite part. Here the physics of squeeze flow with anisotropic vis-
cosity of the composite is used to model the flow process. The heat transfer during heating
and cooling of the material and the mold are also important aspects. The non-Newtonian
and shear thinning nature of the composite complicates the rheology but needs to be ad-
dressed. Thermoplastic sheet forming, thermoplastic pultrusion and fiber tow placement
are some examples of processes that can be modeled in this manner.
The third category involves thermosets of low viscosity resins and continuous fibers in
the form of aligned, woven, or stitched fibers. In almost all thermoset resins, the approach to
modeling uses resin infiltration into a porous network of fibers. Here the flow through porous
media physics allows one to model the impregnation process. Heat transfer is also important
along with the cure kinetics which cross-links the resin, rapidly changes the viscosity and
also introduces heat into the composite. Resin transfer molding, thermoset pultrusion,
thermoset filament winding and autoclave processing are examples of such manufacturing
processes.
Thus, depending on the category, the modeling physics on the macroscale will differ,
and in this book we will introduce approaches and philosophy to model these processes. On
the macroscale, our goal is to find processing conditions such as flow rates, pressures and
rates of heating and cooling to manufacture a successful part. However, as composites are
quite heterogenous materials on a macroscale, one is forced to address microlevel isssues
such as creation of micro voids due to volatiles or air entrapped in the resin that does not
escape from the mold cavity. Interface adhesion between the fibers and resin is decided by
the type of sizing1 on the fibers and their compatibility with the resin. Changes in cure
kinetics and rheology may also occur due to the presence of the sizing on the fibers. In this
book we also discuss how to address some of these microscale issues.
The important challenge in modeling is how one can couple what occurs at the microscale
to the physics that gets influenced at the macroscale. This may not be intuitively obvious in
all cases, but we will present a few examples of how one can endeavor to approach it. Usually
constitutive equations are formulated to bridge this gap. This is a fertile area of research,
especially in areas of material processing in which the modeler tends to use continuum
mechanics principles to describe the macroscale physics for heterogenous materials and
ignores the associated microlevel physics.
1
Sizing is a chemical coating that is applied on the surface of the fibers, sometimes by grafting the
molecules on the surface in order to improve the adhesion between the resin and the fiber.

1.7 Organization of the Book
Chapter 2 will discuss briefly grouping the composite manufacturing processes with the
underlying theme of processing. The philosophy in modeling these processes will be out-
lined, along with a brief introduction to the important manufacturing methods. Issues
important for modeling the transport processes will be highlighted at the micro and macro
scales. Chapter 3 will review the basics of fluid mechanics and heat transfer as required for
processing of polymers and polymer composites. Fundamental principles involved in mod-
eling and the approach that couples the physical laws and the constitutive laws to describe
the physics with the help of appropriate boundary conditions will be outlined. Thus, it will
introduce the transport equations necessary for modeling along with boundary conditions
and examples. Chapter 4 will delve into details of constitutive laws and relationships based
on phenomenological behavior. Chapter 5 will discuss details on the tools necessary for
modeling these processes. The usefulness of tools such as dimensionless analysis and simple
back of the envelope calculations will be illustrated with the help of examples. As there are
different scales involved in polymer composite manufacturing and as the material behavior
at the microscale can influence the issue at the macroscale, coupling of microscale physics
with the phenomena at the macroscale will be discussed. Different phenomenology involved
in characterization of material parameters required in modeling will be introduced, and their
usefulness, challenges and uncertainties will be unveiled. Chapters 6-8 will apply the tools
and the fundamental principles studied in earlier chapters to model composite manufactur-
ing processes. We will illustrate how the modeling principles can be incorporated in some
of the composite manufacturing processes to reveal some of the understanding based on
scientific principles rather than trial and error approaches. Solved examples are presented
in all chapters to enhance the physical understanding of processing these complex hetero-
geneous materials. The questions, fill in the blanks and some problems are formulated to
reinforce qualitative understanding of transport phenomena in various processes and also
understanding the key manufacturing issues in composites manufacturing with seniors and
general practitioners of composites in mind. The analysis and some problems are introduced
for graduate and advanced students who would like to delve further on understanding and
modeling of such processes.
1.8 Exercises
1.8.1 Questions
1. What are the advantages of polymer composites over other materials?
2. List a few industries that use polymer composites.
3. When polymer composites were used a few decades ago, did the process engineers
rely on (i) experience and trial and error approaches, or (ii) accurate mathematical
modeling of process physics, in order to improve the manufacturability of a certain
prototype?
4. What are the two major ingredients of a composite material? How do they enhance
the properties of the composite?
5. What are the two types of polymer resins used in composites processing? What are
major differences between them?

6. What are the three different type of materials used to manufacture fibers?
7. Is it easier to inject a thermoplastic or thermoset resin through a tightly knit fiber
preform?
8. What are the typical viscosities of thermoplastic and thermoset resins relative to the
viscosity of water?
9. Which one of the following has more influence on the mathematical modeling of the
manufacturing process: (a) the fiber material (e.g., glass or carbon) or (b) whether
the fibers are discontinuous or continuous? Why?
10. Although in general the ease of processing decreases as we move from discontinuous
short fibers to continuous fiber preforms that are woven or stitched, why are continuous
fiber preforms preferred in some composite parts instead of discontinuous short fibers?
11. List various manufacturing processes that use continuous fibers.
12. What is the smallest building block in plastics? How many of them are there in a
polymer?
13. What are the different types of reactions that can be used to create all modern poly-
mers?
14. What are the main differences between thermoplastic and thermoset resins in terms
of processing?
15. What are the criteria used to choose an appropriate composite manufacturing method?
16. What is a pellet?
17. What are the advantages and disadvantages of short fiber composites?
18. What composites are referred to as advanced composites? Why?
19. What is a prepreg fabric?
20. What are the two scales used to model composite manufacturing processes? Why do
we need to couple them?
21. List the modeling approaches for manufacturing processes on the macroscale? Why
do we need to model them differently?
22. What are fiber sizings and why are they necessary?

1. The thermoplastic properties are determined by its resulting , which is
strongly influenced by the dynamics.
2. In general, an amorphous polymer is transparent, has mechanical properties
and is resistant to other chemicals than the thermo-
plastics.

3. When a shear force is applied to thermoplastic polymers, the long chain molecules
will start to relative to each other, in response to the applied force. Thus,
most of them exhibit shear behavior, which is an important property to
consider when one develops the process model.
4. The high of cross-linking points within a thermoset structure is responsible
for the superior stability and properties.
5. is applied to a thermoplastic and hence initiate a
change from to before or during processing.
6. Thermosets are generally provided by the manufacturer in phase.
7. After processing, the thermoplastic melt must be cooled down to it, whereas
the thermoset will turn into a after it is chemically and thermally activated
to form the cross-linked network, which is also referred to as
8. Fiber diameter is usually less than Fibers are cut or chopped and com-
pounded in an extruder with any to form consisting of
fibers, or could be pultruded consisting of fibers.
9. Fabrics are laminate structures having fibers aligned in the directions. One
large class of fabrics is manufactured by either or together bun-
dles, or " ", of fibers. These bundles are generally in cross section,
and may contain from to single fibers.
10. Random mats are typically in their structural and flow properties, which
is often untrue for woven or stitched fabrics.
11. Fiber tows can be formed into three-dimensional shapes using and weaving
techniques.
12. Use of preimpregnated fabrics (prepregs) enables these two: (i) it eases the
process during placement over a tool surface, (ii) it reduces the chance of fiber
during the resin injection.
13. The existing machines used for polymer processing could be adopted easily for fiber
reinforced polymers. The advantages would be and compo-
nents with low degrees of and The disadvantage would be no
on the fiber in the component and fiber attrition.
14. Composites with fibers could enhance the mechanical properties by one to
two orders of magnitude as compared to fiber composites. These composites
are referred to as
15. There are several primary steps that are common in manufacturing of advanced com-
posites. First, all advanced composites require a skeleton structure of that
is tailored for the particular part and the property requirements. Second,
this structure must be by the liquid in some way. Finally, the
part should be supported by a rigid to allow the to solidify or
cross-link, permanently freezing the microstructure created by the fiber network.
16. Aligned fibers allow for creation of very high fiber and hence high
stiffness and strength in directions.

17. Two- and three-dimensional interlocked textile structures can allow the composite to
achieve high stiffness and strength in and directions and poten-
tially allow the designer to tailor the mechanical or physical properties to the desired
application.
18. The manufacturing process physics and modeling are greatly influenced by the types
of and
19. The geometry of the part to be manufactured influences the decision if the process is
carried out in an open or closed
20. The process modeling step in composite manufacturing is generally approached by
researchers on two scales. The scale is usually the order of the smallest
dimension of the composite part being manufactured which is in The
scale is more on the order of a diameter which is in microns.
21. Broadly, one can divide the manufacturing processes into three different categories on
the scale from the flow viewpoint, (i) Once the solid pellets are heated,
and short or chopped , which are the two ingredients of pellets,
flow together as a (ii) Long fibers or fibers are preim-
pregnated with viscous resin by applying heat and (iii) The flow
of low viscosity resins through fibers is modeled as infiltration of
resin into a network of fibers.
22. On the macroscale, a modeler's goal is to find processing conditions such as ,
and rates of and to manufacture a successful part.
However, as composites are heterogeneus materials on a macroscale, one is forced to
address microlevel isssues such as creation of micro due to or
entrapped in the resin that does not escape from the mold cavity.
23. Interface adhesion between the fibers and resin is decided by the type of ,
which is a chemical that is applied on the surface of the fibers, sometimes
by grafting the molecules on the surface in order to improve the between
the resin and the fiber.

Chapter 2
Overview of Manufacturing
Processes
2.1 Background
Several industries have been using fiber reinforced composite materials for a few decades
now. Glass fibers were available commercially in the 1940s. Within a decade, composites
were being used by several industries; for example the automobile industry was producing
polyester panels with approximately 25% glass fibers [18].
Manufacturing with composite materials is very different from metals. This is because
when making a metal part, the properties of the virgin material and the finished part
are fundamentally unchanged. For composites, the manufacturing process plays a key role.
During composite processing, one makes not only the part of the desired shape, but also the
material itself with specific properties. In addition, the quality of the composite material
and the part fabricated depends on the manufacturing process, because it is during the
manufacturing process that the matrix material and the fiber reinforcement are combined
and consolidated to form the composite.
In early stages of development, the' cost of composite materials was very high and only
selected industries, for which the importance of the property of the material greatly out-
weighed the cost factor, were willing to use them. These industries were primarily aerospace
and the aeronautical industries. They valued the properties of the composites greatly and
could justify the higher costs because of the weight savings. Both industries took advan-
tage of the light weight and, in the case of defense oriented projects, the stealth properties.
The lack of automated and repeatable manufacturing processes drove the cost of composite
parts up and limited the number of potential users. Another industry that has been using
composites since the 1970s is the marine industry. It could deal with low production volume
and relatively high costs while taking advantage of the corrosion resistance properties of
composites. The majority of the manufacturing work done in these industries in the 1970s
was very labor intensive and not very cost effective as the manufacturing modus operandi
was "experience" and trial and error.
It was imperative that in order for composites to be widely used, especially by the con-
sumer goods industry, such as the automotive and sports industry, two major goals had to
be achieved. First of all, the cost of raw materials had to go south. Secondly, and most
importantly, manufacturing methods had to be developed to achieve high-volume produc-
tion that relied more on the fundamental understanding of the physics of the process rather

than the accepted trial and error practice ingrained on the shop floor of the manufacturing
sites. Over the last two decades, composites research has moved in this direction, and the
development and improvement of several manufacturing methods has been achieved.
The objective of this chapter is to briefly outline the different composites manufacturing
techniques that are commonly used today. Details are described in other books mentioned
in the introduction chapter. As the emphasis of this book is process modeling, the man-
ufacturing methods will be categorized in groups that involve similar transport process
physics. The dominant transport processes will be identified in each process to help clarify
the physics. In addition, a brief evaluation of each method, emphasizing its advantages and
disadvantages, will be listed to help the users identify the best possible method for their
applications.
2.2 Classification Based on Dominant Flow Process

Transport processes encompass the physics of the phenomena of mass, momentum and en-
ergy transfer on all scales. As composites are heterogeneous materials, there is simultaneous
transfer of heat, mass and momentum at micro-, meso- and macroscales, often along with
chemical reaction, in a multiphase system with time-dependent material properties and
boundary conditions.
Composite manufacturing processes are generally grouped into two general classes: open
mold and closed mold. Open mold are those processes in which the part is not inside the
mold during the complete duration of the manufacturing process such as pultrusion or
filament winding. In closed mold processes, the preform is placed in a mold, the mold is
closed, and when it is reopened the part is fabricated. However, as the focus of this book is
transport phenomena in composites processing, instead of classifying processes as open and
closed mold, we will use the mechanisms of transport processes as the yardstick to group
them.
One may broadly group composites manufacturing processes into three categories. The
first category consists of manufacturing processes that involve the transport of fibers and
resin as a suspension into a mold or through a die to form the composite. In such processes,
the fibers in the molten deforming resin can travel large distances and are usually free to
rotate and undergo breakage; thus the microstructure of the final product is linked with the
processing method and the flow of the suspension in the mold. We will describe injection
molding, compression molding and extrusion processes in this category. The reinforcements
are usually discontinuous glass, kevlar or carbon fibers, and the resin may be either ther-
moset or thermoplastic. We will call this category short fiber suspension manufacturing
methods.
The second category, which we will refer to as squeeze flow manufacturing methods or
Advanced Thermoplastic Composites Manufacturing Methods, usually involves continuous
or long aligned discontinuous fibers preimpregnated with thermoplastic resin either partially
or completely. In these processes, the fibers and the resin deform together like the dough
containing strands of continuous wires or wire screens under applied stress to form the
composite shape. However, the presence of fibers creates anisotropic resistance to the
applied load, and the viscosity can be over a million times that of water, preventing large
bulk movements of the composite. Thermoplastic sheet forming, thermoplastic pultrusion
and fiber tape laying methods can be described by this physics. The precursor materials can
be in various forms such as the thermoplastic tapes impregnated with aligned and continuous
or long discontinuous fibers (for example, APC2 and LDF materials, respectively) [19, 20,
21]. The other popular form is to weave a preform of the polymer fibers commingled with

glass or carbon fibers. Thus under applied heat and pressure, the polymer fibers melt
and occupy the space in between the reinforcing fibers [22]. The polymer could also be
in powder form attached to the fibers during the initial stages, which the heat will melt
and the pressure will help fuse and consolidate the fiber assembly [23, 24]. The reality of
thermoplastic resins is that they cannot travel and infiltrate large distances due to their
very high viscosity. Thus the precursor material form has to accommodate a distributed
resin percolation among the fiber architectural network.
The third and final group, which we will term porous media manufacturing methods
or advanced thermoset composite manufaturing methods, involves usually continuous and
nearly stationary fiber networks into which the resin will impregnate and displace the air,
forming the composite in an open or a closed mold. The resin in such processes is almost
always a thermoset due to its low viscosity. But one does have to account for complex
chemical reactions that are prevalent in these methods. We will discuss liquid composite
molding, filament winding and autoclave processing under this category. The precursor
material here can take various forms from partially impregnated prepregs to applying the
liquid thermoset resin to the fibers during the process or impregnating the resin in a sta-
tionary network of fibers. The low viscosity of thermoset resin allows for this versatility.
However, the disadvantage is the introduction of complex chemical reaction and the gelling
and curing phenomena. In addition, thermosets are environmentally unfriendly, and it is
difficult to repair and recycle them.
Figure 2.1 schematically shows the type of flows one expects in these categories. In the
section below, we will describe the commonly used composite methods under the categories
created.
2.3 Short Fiber Suspension Manufacturing Methods

The underlying transport process here during manufacturing is the flow of the resin along
with the discontinuous fibers. Mechanical and physical property control is a primary issue
in this process. Denton [25] showed that tensile strength and the elastic modulus of the
samples made by compression molding of short fiber composites in a carefully controlled
laboratory environment exhibited a standard deviation of about 50% around their mean
value. The properties vary due to two main reasons: precursor material variability and
fiber orientation variability. It is well known that flow will change the orientation of fibers,
which, in turn, will influence the properties. In this book, in addition to developing process
parameters which influence manufacturing, we will try to quantify this effect in an attempt
to tailor the properties of such materials.
The three processes, injection molding, extrusion and compression molding, which evolved
as composite processes from polymer processing techniques and the transport issues associ-
ated with them, will be discussed here. The precursor materials (material form used as the
initial input to the process) in injection molding and extrusion are polymer pellets contain-
ing short fibers, and for compression molding it is usually a charge of material containing
resin, fillers and fibers.
2.3.1 Injection Molding

Process
Injection molding is the most common and widely used manufacturing process for high-
volume production of thermoplastic resin parts, reinforced with fibers or otherwise. Solid
pellets of resin (usually the size of a small piece of chalk) containing the fibers and sometimes

a) Short Fiber Suspension Flow
Force
b) Squeeze Flow in Advanced Thermoplastic

Manufacturing Methods
Macroscopic (Volume Averaged)

Microscopic Velocity i Velocity
Process sfe V_. "i—x_ i—f—*"* ?—*—i Model
Fluid Phase
Solid Phase
c) Darcy Flow for Advanced Thermoset

Manufacturing Methods
Figure 2.1: Schematic of types of flows expected in composites processing: (a) Short fiber
suspension flow, (b) Advanced thermoplastic flow, and (c) Flow through porous media.

fillers are fed through a hopper into a heated barrel with a rotating screw. The function of
the screw is to mix the reinforcements and the resin and also to generate heat by viscous
shearing against the barrel. This melts the resin. The screw then acts as a piston and
forces the mixture of fibers, fillers and molten resin under high pressure through sprues and
runners into a matched-metal mold where the polymer solidifies, freezing the orientation
and distribution of fibers and fillers in the part. The mold cavity is then opened and the
composite part is ejected. As the fabrication of metal molds can run into thousands of
dollars, one can justify the use only for high-volume production parts such as laser disks,
etc. Recently, researchers have begun to explore the use of plastic molds reinforced with
metal powder for small-volume production or for prototype development with the use of
rapid prototype technology [26].
Mold
Part
, ,TT^ 77" J Injection process

I
Figure 2.2: Schematic of injection molding process.
zoom
Figure 2.3: Details of injection molding machine [16].

The injection molding is a cyclic process in which a molten polymer along with reinforce-
ments and fillers is injected into a closed mold cavity where it takes the shape of the mold
cavity and solidifies because the mold is usually cold with high thermal inertia (see Figures
2.2 and 2.3). The molding time is usually of the order of few seconds, and parts can be
complex and precise as shown in Figure 1.14. The mold is then opened, the part is ejected

with ejector pins and the cycle is repeated. Since the first hand operated injection molding
machine was introduced over seven decades ago, it has evolved into a complex, sophisticated
and automated process that can produce many thousands to millions of parts.
The injection machines can be as simple as a plunger and a torpedo unit to a recip-
rocating single or double screw injection unit. Description of complex machines can be
found in various other books on injection molding [27, 28, 29]. Some of these units can be
modified to handle thermoset materials with reinforcements as well. However, as the shear
rates experienced by the material can be of the order of 104 to 106 s"1, the thermoplastic
viscosities can decrease rapidly due to their shear thinning nature, allowing rapid molding
of such materials.
The important process parameters that can be controlled on the injection units are the
melt temperature, injection and screw speed, injection pressure and in some instances, the
mold temperature. The material parameters that will influence the manufacturing process
and the final properties of the part are the resin rheology and the filler type and content.
The geometric parameters that will play a key role are the mold cavity shape and size, and
the locations of injection gates, through which the resin enters the cavity, and the vents
that allow the air to escape.
Precursor Materials
The filled thermoplastic pellets usually contain a second, discontinuous, usually more rigid
phase blended into the polymer. When the aspect ratio (ratio of largest to smallest di-
mension) of the second component is around one, it is referred to as a filler. If the aspect
ratio is one to two orders of magnitude larger, then it is called a reinforcement. The most
commonly used reinforcements are particles, wiskers and short fibers usually less than one
inch in length. The parts obtained usually have a fiber volume fraction between 30% and
40%. Filled or reinforced materials provide much different properties than the base resin.
For example, reinforced polypropylene provides higher rigidity and lower warpage charac-
teristics than neat polypropylene. Also, the viscosity of the filled resin will be different in
magnitude and sometimes anisotropic as compared to the neat resin. In practice, fibrous
reinforcements used with glass fibers dominate the market although the carbon and aramid
fibers provide higher stiffness and strength but are seldom used due to the high cost of raw
materials.
The traditional injection molding process limits the fiber length that solidifies in the final
part since the high shear rates in the barrel and the passage of fibers through narrow gates
and openings in the mold cause significant fiber attrition. Usually, the fiber diameter is of
the order of a few microns, and the final length distribution, irrespective of the starting
fiber length, is of the order of 50 to 500 /mi. The starting length of these fibers in the
log-like pellets is usually of the order of 1 to 3 mm. As a result, new methods to produce
pellets containing longer fibers were developed in which the fibers were pultruded and stayed
bundled together and were not dispersed in the pellet by the action of compounding. These
pellets (see Figure 2.4) produced final parts that retained a higher percentage of longer
fibers and consequently showed a significant increase in modulus and impact toughness.
The thermoplastic matrix material selected also plays a role in the final physical and
optical properties. Most thermoplastic materials when they solidify do so as an amorphous
matrix or exhibit various degrees of crystalline behavior depending on the thermal history
the material undergoes during the injection molding process. Samples of crystalline and
amorphous materials are shown in Figure 2.5. More details on crystallization of thermo-
plastics will be discussed later.

Creel Racks
Impregnation Cutter
\, Die
o
Fibers Pellets
o Resin (length = 11 mm,
diameter = 2 mm)
Puller
Figure 2.4: Schematic to make pultruded pellets.
Figure 2.5: Crystalline and amorphous materials, (a) Spherulite in malonamide containing
10% d-tartaric acid (low crystallinity). (b) Spherulite grown in mixture of isotactic and
atactic polypropylene (high crystallinity) (redrawn from [30]).
Transport Issues
The issues that relate to transport phenomena in this process are the flow of fiber suspen-
sions as they occupy the closed mold, the orientation of the fibers during flow, fiber length
distribution, fiber breakage and the heat transfer that changes the microstructure of the
resin. So, if we consider mass conservation, we have to account for the mass balance of
the suspension which can be treated as a continuum material at least for the short fiber
materials as the fiber length is of much smaller scale as compared to the domain dimen-
sions. One also needs to characterize and describe the orientation of the fibers in a flowing
suspension. The physical concept that one may have to invoke here is the conservation
of the orientation field, which simply states that if the orientation of the fibers disappears
in one direction, it should reappear in some other direction. One also needs to conserve
the momentum to describe the flow and the pressure field during the flow process. This
requires one to describe the constitutive equation between the stress applied and the strain
rate experienced by the material. For Newtonian fluids, this is usually constant and the
constant of proportionality is called viscosity. However, as the thermoplastic melts are shear
thinning, the viscosity is known to decrease with shear rate, and the addition of fibers can
change the stress strain rate behavior and even make it anisotropic. One needs a rheologi-
cal equation to describe this behavior. The energy conservation allows one to describe the
temperature history of the melt in the channel between the screw and the barrel, where it
gets its heat input from the heaters on the barrel and due to viscous dissipation caused by
the shearing of the suspension. It also allows one to keep track of the cooling history in

the closed mold as the suspension enters it. The cooling dynamics play a crucial role in the
resulting microstructure.
The transport phenomena modeling also requires one to consider initial and boundary
conditions; hence the physical laws of mass, momentum and energy balance need to be ap-
plied at the boundaries along with imposed external conditions which we refer to as process
parameters. The material parameters enter into the modeling through the description of
the constitutive equations.
There are other microscale phenomena occurring simultaneously such as the molecular
orientation and spherulitic growth of polymers during solidification and fiber breakage due to
shearing action in the screw that results in a length distribution. For long fiber suspensions,
the constitutive equation may change, and issues such as fiber clustering may also need to
be addressed, as seen in Figure 2.6 [31].
Clusters
Figure 2.6: Schematic of fiber clustering for long fiber suspensions [31].
The coupling between the energy transport and the momentum creates a fountain flow
mechanism in injection molding. As the walls are cooler than the core, the suspension
viscosity is higher near the walls (polymer viscosity increases as temperature decreases) as
compared to the core. Hence, under the same pressure, the suspension in the core moves
ahead of the suspension near the walls, spreading from the center outwards like a fountain,
as shown in Figure 2.7.
Flow
direction
Figure 2.7: Schematic of fountain flow effect encountered during filling (redrawn from [32]).
The fibers align in the direction of shearing and also in the direction of stretching as
shown in Figure 2.8. The shear flow near the mold walls aligns the fibers in the direction of

the flow and is called the skin. Below this layer, the suspension continues to experience shear
and fibers orient along the shear lines; this layer is known as the shear layer. Finally, the core
has fibers that are influenced by the bulk deformation of the flow in the mold which usually
has an elongated component, causing the material to stretch in and out of the paper direction
aligning the fibers. This skin core structure is a common microstructural observation, and
it is the study of the coupling between flow, heat transfer and fiber orientation which will
allow us to understand this phenomena.
I
s<n
''
Flow
direction / \/ \ / / \ \ / \ / / \ / \ / \/ \\ )
i i i \
core
} skin
Skin: fibers are mostly aligned along the flow direction

Core: fibers are mostly aligned transverse to the flow direction
Figure 2.8: Influence of flow on fiber orientation.
Another phenomenon associated with flow and fibers at the micro level has been that
the fibers at the flow front tend to align along the flow boundary and not across it. This may
have to do with the surface tension phenomena between a solid, polymer and air. However,
because of this phenomenon, whenever two flow fronts meet, the boundary is called a weld
line and is usually the weak link for the mechanical properties because the fibers align along
the weld line and not across it, as shown in Figure 2.9. Thus, understanding of this issue
could help modelers address and develop flow management techniques to create strength
along the weld lines.
Applications
Nearly 20% of the goods manufactured nowadays use injection molding due to its versa-
tility and low cost. However as short fiber composites can improve the desired physical,
optical and mechanical properties, structural integrity and dimensional stability, injection
molding machines and the screw geometry were modified to handle fibers along with the
polymer. Many applications such as housing for electric tools, automotive parts under the
hood, plastic drawers, metal inserts and attachments, seats in airplanes, etc. are routinely
manufactured using injection molding with thermoplastic pellets containing discontinuous
fibers.
The fundamental advantage of injection molding is the ease of automating the process
and the short cycle times, which together allow for the possibility of high volume production.
In addition, molds can also be constructed to make more than one part at a time. The
major disadvantages are the high initial costs of the capital equipment and the molds and
the variation in part properties due to lack of control of fiber orientation and distribution.

Flow
fronts,
,• Weld line
Injection (Fibers are aligned
gate —> parallel to weld line)
Figure 2.9: Schematic of flow front locations and weld line with fibers aligning along them
during injection molding.
2.3.2 Extrusion
Extrusion resembles injection molding because it contains a screw. The main difference
is that there is no closed mold in extrusion. Instead .a die is used to shape the polymer
suspension into specific cross sections. This process is used to plasticize and compound
polymer pellets containing short fibers and also for manufacturing continuous parts with
different cross sections. As in the case of injection molding, the screw melts the polymer and
acts as a piston to push the suspension into the die geometry. Inside the die, the suspension
takes the form of the die cross section and exits from the other side of the die and can be
continuously pulled to make long tubes, I-beams and reinforced pipes.
Solid pellets
Hopper
k) . .
Extr jder 1pie|
Sizer Cooler
to Cutter
Puller
Figure 2.10: Schematic of extrusion process line [33].
Process
Figure 2.1C shows a simple sketch of an extrusion line. The process starts with a hopper
into which one pours solid pellets. The extruder melts the plastic (resin or polymer) and
may seriously cause fiber attrition. It pumps the fiber suspension through a die hole of the
desired shape. It then enters a sizing and cooling trough where the correct size and shape
are developed. Next, the formed product enters a puller which pulls it through the sizer.

At the end of the line, a cutter or coiler does the handling of the product. Thus, it is a
continuous process, and as long as the operator makes sure that the hopper is filled with
pellets and the final product is moved away for storage and shipment, it can operate for
days without much attention, which makes it very cost effective.
The heart of the extruder is a barrel and the screw that turns in it. A sketch of the
extruder is given in Figure 2.11. The screw channel connects the hopper at the rear and to
the die at the front of the extruder. The screw is the moving part that melts and pumps
the plastic. The extruder screw is turned in the barrel with the power supplied by the
motor operating through a gear reducer. The screw is usually machined from a solid steel
rod and fits within the barrel with less than a millimeter clearance. It is hardened and
chrome plated to resist corrosive action of some resins. To pump a suspension through
a die, the screw is designed to generate over 100 to 200 atmospheres of pressure in the
suspension. The barrel of the extruder resembles the barrel of a cannon. It is made of steel
and has thick walls to withstand very high internal pressures. The inside of the extruder is
made of a hard steel alloy for corrosion resistance, and the inside dimension of the barrel
determines the extruder size. The power to turn the screw comes from an electric motor.
Usually, the power requirements are large due to the pumping pressure and rate required.
The pellets are usually fed through the hopper by gravity. The outside of the barrel is
equipped with heating and cooling systems to maintain the barrel at a desired temperature.
We will consider the details of the working of the screw later, but for a simple and crud,e
explanation, one may think of a bolt as the screw, the nut as the pellet and the wrench as
the barrel. Now if one turns the bolt (screw) and holds the wrench (barrel) in place, the
nut (pellet) will move forward. The heat from the heaters and the mechanical frictional
work will melt the polymer and push it forward along with the short fibers. This action is
usually called plasticating. Most of the heat needed for softening and melting comes from
the viscous dissipation due to the turning of the screw inside a stationary barrel. This heat
generated from mechanical work is sometimes more than sufficient to operate an extruder
with its heaters turned off, but sometimes the cooling system has to be turned on to avoid
overheating of the resin.
' Powder
Screw , Flight
Breaker plate
Figure 2.11: A schematic of the extruder (redrawn from [34]).
Transport Issues
The action of the screw as a pump is a complex process and involves drag flow and pressure
driven flow acting against each other. Hence the important transport issues are to under-
stand the interaction between the drag and pressure driven flow and their role in calculation

of the pumping rate and the power requirement for the turning of the screw. Another trans-
port phenomenon is the interaction of the viscous dissipation in the momentum transport
with the heat transport which helps understand and control the heating and cooling system.
As the suspension is non-Newtonian when it exits the die, the normal stresses can distort
the cross section by causing a phenomenon known as die swelling as shown below.
Dn,
Figure 2.12: Schematic of die swelling.
Die swelling (see Figure 2.12) and melt fracture are significant processing issues for ex-
truded structures and with the addition of fibers can distort the final cross section. Trans-
port processes and their interaction with surface tension and normal stresses will allow one
to study and hopefully understand this relationship.
Applications
Extrusion is considered as the positive displacement pump for producing over six billion
polymer products each year. A partial list of extruded products includes films, pipes,
tubing, insulated wire, filaments for brush bristles, profiles for home siding, storm windows
and gaskets, etc. [35]. The process of making these products is termed extrusion. The
processing physics of flow and heat transfer of plastic melts in an extruder have been
studied in detail by many researchers [36, 37]. In the last few years, the process has been
slightly modified to allow extrusion of polymers containing reinforcements.
2.3.3 Compression Molding

The principle in compression molding is very simple. The material (called the charge) is
placed inside the mold cavity. The mold is closed by applying pressure. The material
deforms to take the shape of the cavity. The mold is opened and the part is ejected.
Although conceptually simple, there are many critical issues that need to be resolved before
one can produce a part without defects.
Compression molding has been around for decades and was used for a long time as a
standard method for molding phenolics and similar thermosets. Injection molding partially
replaced it primarily because of its ease in material handling and automation. However,
compression molding offers a distinct advantage when processing composites. As compared
to injection molding, in compression molding the material undergoes very modest amount
of deformation and there are no regions of very high stress, as in a gate of an injection mold.
Also as there is no gate through which the fibers have to enter the mold, the reinforcing fibers
are not damaged by the flow during mold filling, and longer fibers and higher fiber volume
fractions can be used to make composites. The other advantages of compression molding
are that it is fairly simple, cycle times can be relatively fast, repeatability is excellent, high-
volume production is easily obtained and parts with tight tolerances can be produced. In
addition, mixing the resin and fibers before the compression allows for good control over
the chemistry and the mix of the final product. The major disadvantages are that a large

initial investment in molds and presses is necessary, the material must be stored under
certain environmental conditions and must be used within a certain time for thermosets,
and flow related problems can arise during the process so mold design is difficult and tedious.
Several minor defects can arise in the part such as residual stresses, delamination, warpage,
and flow orientation of fibers; all these give the process a large number of variables that can
influence the process and hence the part quality [38].
Precursor Material Forms

A wide variety of composite materials are compression molded. The most commonly used
material for compression molding of composites is sheet molding compound (SMC). This
material consists of a thermoset matrix with short fibers dispersed through it. This may
involve compounding a resin, combining it with fillers and fibers or impregnating a fiber
preform with a resin. Subsequently, thickening of the resin or B-staging of the resin is carried
out for proper bonding between the fibers and the resin. Figure 2.13 shows schematically
how SMC is made.
Continuous Strand Roving
Continuous o
Strand Roving Chopper
Resin/Filler
10 Paste ^ Carrier Film
Resin/Filler Chain Link Compaction Belt

Paste
n mb^JD
Carrier Filmy
^ Take-up Roll
Figure 2.13: Schematic of sheet molding compound (SMC) production (redrawn from [38]).
To form the sheets of SMC material a specific procedure is used as shown in Figure 2.13.
A thin layer of resin is placed on a sheet of nonporous material, such as nylon. As the
nylon moves along the production line, fibers are added to it; these can be in random,
unidirectional, or other orientations. Next a layer of resin, placed on a cover sheet, is
applied onto the fibers so that the resin is in contact with the fibers. This sheet, enclosed
between the nylon sheet and the cover sheet, is then passed through several compaction
rollers. These serve two main purposes: they mix the resin and fibers together, and they
compact the sheets. The resin is now in a continuously changing state (i.e., it is slowly
curing); it is left to thicken for approximately 5 days, after which the SMC is ready. At
this point the SMC sheet must be used within a certain period of time, which can be
up to several weeks, and must be stored under certain environmental conditions, such as
low humidity. Several types of SMC are currently used in industry: SMC-R (reinforced
with fibers oriented randomly), SMC-C (reinforced with unidirectional continuous fibers),
SMC-C/R (reinforced with both randomly oriented and continuous unidirectional fibers),
SMC-D (reinforced with directional but discontinuous fibers). It is possible to use both
thermoplastics and thermosets in SMC, but the majority of SMC is done using thermosets

[39].
Automobiles have been using SMC in many primary and secondary structures. For
example, Ford Explorers and Rangers used SMC beams in 1995, and their number increased
to 1.75 million by the end of 1996 [40] and has continued to increase despite the fact that
one cannot recycle this material.
Other composite materials that can be compression molded are thermoset matrices with
continuous reinforcing fibers and thermoplastic matrices with continuous random or aligned
fiber reinforcement. Traditional laminates usually with woven or stitched fiber preforms are
also compression molded. The processing of such materials will be discussed under squeeze
flow manufacturing methods for thermoplastic materials and porous media manufacturing
methods for thermoset matrices as categorized by the dominant transport processes. Com-
pression molding of short fiber reinforced materials such as SMC is interesting because the
properties of the finished product are strongly affected by the processing.
Process
The SMC or the thermoplastic material is stacked into the mold cavity. This is referred
to as the initial charge. The initial charge shape and its placement location in the mold
are crucial parameters as they influence the final properties of the product. Sometimes this
charge is preheated using dielectric sensors before closing the mold to initiate the flow. The
temperature field that results from this stage is part of the initial condition for the mold
filling stage. Mold filling begins when the polymer begins to flow and ends when the mold
cavity is filled. The heated top and bottom platen containing the two halves of the mold
cavity are brought together, generating heat and pressure to initiate the flow. Temperature
ranges between 135 and 160 degrees C, pressures between 3.5 and 15 MPa and cycle times
between 1 and 6 minutes. The amount of flow in compression molding is small but critical
to the properties and the quality of the part because the flow controls the orientation of
the short fibers and the final orientation pattern is what will determine the physical and
mechanical properties of the composite.
In-mold curing describes the next stage in compression molding of thermosets, where
the liquid resin starts to gel and cross-link and forms a solid part. The curing may initiate
during mold filling stage but the bulk of the curing takes place after the mold is filled. The
part is removed from the mold as soon as it is solid-like and may be placed in an oven for
post-cure to complete the curing process.
The mold is usually made of steel and it is hardened in key areas where the mold can
wear out more easily. This is important because the mold is subject to high pressures and
temperatures and also undergoes many cycles continuously. For these reasons mold design
is very important, and the overall cost of the molds is usually high. Several different resin
systems can be used in SMC. Vinyl ester and polyester are the most used in the automotive
industry, while epoxy resins are widely used in the aerospace industry [41]. There are several
variations and modifications that different industries have developed over time, in order to
improve the process and to tailor them to their own needs. The automotive industry, for
example, has a specific need for parts with excellent surface finish. For this, a technique
known as in-mold coating was developed.
In in-mold coating, after the part is partially cured inside the mold, the mold is opened
slightly and a resin, such as a urethane, is injected in the mold. Subsequently the mold is
closed again, causing the resin to coat the outside of the part, filling any voids on it. This
greatly improves the surface finish on the part and can save several stages in the painting
process.

Transport Issues
Heat transfer by conduction, interaction between cure and heat transfer, cure and viscosity,
temperature and viscosity, velocity, deformation gradient and fiber orientation, fiber orien-
tation and viscosity are some of the transport phenomena that are important to understand
to model the flow behavior of SMC like materials by compression molding. Part cool down
is the final phase which plays an important role in the distortion of the part and the devel-
opment of residual stresses. A difference in thermal expansion through the thickness and in
different sections of the part is one of the sources that gives rise to residual stresses inducing
distortions as the part cools down to room temperature. Thus, the temperature distribution
and rate of cooling are important in determining how these stresses relax during cool down.
Another issue related to the transport processes is the cycle time it takes to produce a
part from a single mold and press. This is important in high-volume applications. Closing
speed and placement of the charge in the mold can influence the time to fill the mold with
the material. Considerable efforts on trial and error methods have been made to reduce
the cycle time. Understanding of the cure kinetics and its interaction with heat transfer
should provide fruitful avenues for enlightening experiments and methods to improve the
cycle time.
Mold and part design is related to flow and heat transfer and indirectly controls the
quality of the part and the cycle time. For example, thermal design of the mold will
influence the cycle time. Fabrication of molds is an expensive and time consuming task, so
modeling the process, which can virtually verify the design efficiency before the mold or the
tool is built, will be extremely handy.
Process automation is also a critical issue as it will make this process more competitive
with injection molding. Currently the initial charge shape is cut and placed by hand in the
mold cavity. Use of devices to load and unload the part, along with cutting and placement
of the charge as shown in Figure 2.14 will allow this process to handle material in bulk and
for high-volume production.
Robot 1 Robot 2 Robot 3
Press
Finished part
Figure 2.14: Schematic of automated compression molding [9].
Performance of the manufactured part is tied to the flow, heat transfer and chemical
reactions which occur in the mold. For example, initial charge shape and location will change
the flow pattern, which in turn will influence the fiber orientation. The fiber orientation
will influence the physical and mechanical properties.
2.4 Advanced Thermoplastic Manufacturing Methods

Thermoplastic resins are usually solid at room temperature and exhibit some softening
when heated above their crystallization temperature, which is usually above 100°C. Even
at their melt temperature, thermoplastic resins are very viscous. It is not uncommon to

have a resin with a viscosity about a million times that of water (10,000 Poise) at its melt
temperature. It is extremely difficult to process such resins if they have to be forced to
occupy the empty spaces between fibers to form an advanced thermoplastic composite.
Unlike short fiber suspensions, advanced thermoplastics contain continuous fibers or nearly
continuous fibers. However, two mechanisms can help reduce the viscosity of the resin.
The viscosity reduces rapidly with temperature for most thermoplastics. Secondly almost
all thermoplastics are shear-thinning materials, which implies that under high shear their
viscosity reduces. Nevertheless, high processing temperatures translate into higher costs in
cycle times and processing equipment. As the polymer can degrade at higher temperatures,
the window to raise the temperature much higher than the crystallization temperature is
narrow. Also, it is difficult to shear the resin to occupy the spaces between the fibers at
such high viscosity levels. To circumvent this problem, the resin is preimpregnated into
the fiber bundles or is sprayed as commingled powder or resin fibers are woven with the
reinforcing fibers. This ensures that resin does not have to travel far when heat and pressure
are applied to move the resin to occupy the empty spaces between the fibers.
When heat is applied the resin melts, and the applied pressure makes the resin flow
and redistribute. As the resin is viscous, the fibers and the resin on the macro scale will
deform together and consolidate into the shape of the structure being manufactured. Hence,
for such materials practice has converged, from the modeling viewpoint, to treat them as
one material with a viscosity that is modified due to the presence of the fibers. The three
manufacturing methods that may be modeled with this philosophy and will be discussed
in this book are (1) sheet forming, (2) tape laying or advanced fiber placement and (3)
thermoplastic pultrusion. We will give a brief description of these processes below.
2.4.1 Sheet Forming

The processing science for long and short fiber reinforced thermoplastic sheets grew out of
a need for large parts with higher strengths and stiffness over non-reinforced sheets and
monolithic materials with faster processing cycle times than those for thermoset-matrix
composites. In addition to faster forming cycles, thermoplastics have more flexible process-
ing parameters since the viscosity is only a function of temperature — not of cross-linking
or cure as in thermosets. Sheet formed parts also have the potential to reduce the total
part count in a structure by molding in and incorporating reinforced areas.
Process and Precursor Materials

Composite sheet forming is a process well suited for the forming and shaping of thermo-
plastic matrix short and long fiber reinforced composites. The material preform may be in
unidirectional or multi-axial sheets either in stacked or pre-consolidated form. The basic
sheet forming sequence starts with heating the preform to its forming temperature, defined
as the temperature where the viscosity of the reinforcing resin is soft enough to allow the
reinforcing fibers to slide relative to one another and permit easy shaping of the sheet.
Then, using either mechanical or hydraulic pressure, the sheet is formed over a curvilinear
tool surface. The forming step is analogous to several common sheet metal bending and
forming operations and includes deformation of the sheet both in and out of the plane. This
material flow is viscous and is characterized by the flow of both resin and fibers together.
After the forming step is complete, consolidation pressure is maintained on the part until
the part cools below the matrix melt temperature. Once sufficiently cooled, the part is
removed from the tool surface and, if required, an edge trimming step is performed. If
necessary, the reversible solid-liquid phase change characteristic of thermoplastics enables

the once formed part to be transferred to another tool surface and repeatedly re-formed or
incrementally formed until the final desired geometry is attained.
The oldest form of sheet forming exists with the processing of non-reinforced thermo-
plastic sheets. Isotropic in nature, the sheets are usually held in place along the edges over
a tool surface and brought up to their material softening temperature. This is usually some-
where slightly below the actual melt temperature in order to work the material while in a
compliant but not liquid state. The most common forming methods are "hot stamping,"
where the sheet is pressed between matching dies, and "vacuum forming," where a vacuum
is pulled through small holes in the tool face, pulling and spreading the sheet down over
the surface.
The sheet forming process holds several unique advantages over other thermoplastic
processing methods such as injection molding, pultrusion and tape laying methods. The
nature of injection molding combined with the high viscosity of the thermoplastic precludes
the use of high aspect ratio fibers (> 1000) which provide the necessary mechanical prop-
erties desired in high performance applications. Additionally, it is difficult to make large
parts by injection molding. Sheet forming can potentially make large parts and provide a
much greater control over and ability to predict the final fiber architecture.
Sheet Forming Methods

The major composite sheet forming processing methods can be broadly classified as hot
stamping, diaphragm forming, and incremental processing. Composite sheet stamping or
matched-die press forming imitates the stamping methods employed in the field of sheet
metal forming as a high volume, low cost manufacturing process as shown in Figure 2.15(b).
The composite blank is heated to the forming temperature and then stamped against the
tool surface. A variation on this is rubber tool stamping wherein one or both sides of the
die are made compliant. This helps maintain an even consolidation pressure across the part
in case of any tool misalignment.
Platen
Vacuum Solid or compliant tool

B-6
Clamping ring
Laminate
Upper and lower
diaphragm
Exhaust
(a) Diaphragm Forming (b) Matched Die Forming
Figure 2.15: Composite sheet forming processing methods: (a) diaphragm forming, and (b)
matched die forming [42].
In diaphragm forming as shown in Figure 2.15(a), the blank is held between two dis-
posable, plastically deformable diaphragms of either super-plastic aluminum or polyimide
polymer. During the forming cycle, the diaphragm edges are clamped, heated along with
the blank and deformed through the use of air pressure to the tool surface. The diaphragms
serve to hold the blank in tension and prevent fiber buckling that can occur under com-
pressive stresses. When forming parts containing continuous fiber reinforcement, the di-
aphragms are clamped but the blank cannot be. This is due to the inextensibility of the

fiber reinforcement. Hydroforming is a process similar to diaphragm forming; however,
hydraulic fluid is used to provide the pressure behind a permanent rubber diaphragm.
Incremental processing enables the forming of large structures using smaller, lower cost
fabricating equipment. After the usual heating and forming steps, there is an additional part
transfer step added to the forming cycle. Incremental forming also provides the ability to
construct final shapes that would be very difficult otherwise. Stock shapes can be produced
and later incrementally formed into custom configurations. One promising incremental
forming method is stretch forming. Stretch forming makes exclusive use of aligned, long,
discontinuous fiber reinforcement technology and as the name implies, an extensional mode
of deformation in the fiber direction is enlisted during the forming process. Since the
fibers are discontinuous, the composite sheets may be locally heated and deformed. This
allows certain incremental forming techniques not possible with continuous fiber reinforced
materials. For example, linear beams can be stretch formed into curved sections with
favorable mechanical properties since the fibers follow the curvature of the beam [42] as
Figure 2.16: Linear beams can be stretch-formed into curved sections with favorable me-
chanical properties since the fibers follow the curvature of the beam [42].
The key to successful stretch forming is precise control over the final fiber placement.
This is achieved by clamping both ends of the unformed part, heating up the portion
between the clamps and then carefully forming the stock shape to the desired curvature
[42].
Transport and Other Issues

The major disadvantage of this process is that due to the presence of fibers, the viscosity of
the material is highly anisotropic and hence forming compound curvature shapes leads to
wrinkles and folds during manufacturing as shown in Figure 2.16. Long discontinuous fiber
material alleviates this problem to some extent, but nevertheless this has been a big hurdle
in the lack of interest in using this process for more complex curvature parts. Modeling of
the sheet forming process is quite a challenge. To describe the transformation of a stack of
flat sheets into a complicated three-dimensional shape involves movement of a free surface
and contact with a tool. The deformation can be large, and one must be able to describe
the deformation physics of such highly viscous anisotropic materials. The anisotropy can
be very severe, and the material can have multiple inextensible directions. The layers may
slip over one another during forming.
Qualitatively, one can describe the micro and macro mechanisms the material undergoes
before the part is formed. First, when one places various sheets of thermoplatic tapes

containing continuous or discontinuous fibers and applies heat and pressure, at the micro
level one can expect the resin to melt and percolate to form a more uniform fiber-resin
mixture. Further pressure causes squeeze flow of this material. However, due to the presence
of the fibers, the material has anisotropic viscosity and will only flow in the transverse
direction to the fibers at the macro scale. If the layers of sheets containing uni-directional
fibers were arranged in different directions, one could expect the layers to shear based on
the deformation process it is undergoing.
No comprehensive model for sheet forming exists. There are many geometric mapping
issues as well as transport issues in this process. The modeling should be able to provide
information about the thickness of the composite after deformation, location of the edges of
the blank and the occurrence of defects, such as laminate wrinking and/or fiber buckling.
The important parameters that do influence this process are part geometry, tool geometry,
initial blank shape (fiber composite sheet shape), initial thickness, fiber orientation in the
initial blank, material properties and processing conditions such as forming speeds, applied
pressure and temperature.
2.4.2 Thermoplastic Pultrusion

As it has been around since the late 1940s, pultrusion is one of the oldest composite man-
ufacturing processes. It was originally designed to manufacture fishing rods [43]. This
process can be used for both thermosets and thermoplastics. However, the thermosets have
dominated the composites industry.
Die Assembly Pulling

Mechanism
Preheater Control pi-iji-
Panel .1 -I -I « «,
Composite
(a) Manufacturing Line for Pultrusion of Thermosets
(b) Manufacturing Line for Pultrusion of Thermoplastics
Figure 2.17: Schematic of a pultrusion line [13].
Process
The process involves dragging a combination of fiber and matrix materials from a supply
rack through a temperature controlled tool, which will determine the final part geometry.

The design of these tools depends on whether one is going to use a low viscosity thermoset
resin or high viscosity thermoplastic polymer. For thermosets, one can use bare fiber rovings
to go through a liquid thermoset bath before entering the die for curing and cross-linking.
On the other hand, thermoplastic resins are preimpregnated with continuous fibers in the
form of a tape or the fibers pass through a station of polymer powder bed, where the
thermoplastic powder attaches itself to the charged fiber surface. Therefore, thermoplas-
tic pultrusion requires a preheating area, which can be either an infrared or a convection
oven preceeding the actual tool. After passing the preheating station, the fibers enter the
tapered entry region of the tool where additional heat is introduced to the precursor, assur-
ing complete melting of the thermoplastic matrix and allowing it to spread over the fiber
surfaces. Then the fibers covered with resin go through a tapering die, which consolidates
the composite into the shape of the die. A schematic of a pultrusion station is shown in
Figure 2.17.
The attractive feature of the pultrusion process is that it is a continuous process, and
therefore the material efficiency is extremely high. However, after almost 40 years in produc-
tion, the major application produces only simple profiles as shown in Figure 2.18. Further
understanding of the process physics could extend the application of this process to more
challenging shapes. Thermoplastics, although difficult to process, offer improved impact
strength, and enhanced fracture toughness, and they allow for reshaping and recycling as
compared to thermosets [44].
Figure 2.18: Some typical cross sections made by pultrusion [45].
Transport Issues
The transport phenomenon inside the heated die is of interest as most of the redistribu-
tion of the resin and the consolidation of the fibers and the resin takes place there. The
precursor material used will influence the transport phenomena modeling in this process.
Several different types of thermoplastic preforms can be used with this process. They are
either continuous fibers completely impregnated in the shape of thermoplastic tapes (e.g.
CF/PEEK) or glass fibers embedded in thermoplastic powder and enclosed by a thermo-
plastic tube of the same material or commingled polymer and reinforcing fibers. Figure
2.19 depicts available materials for usage in the thermoplastic pultrusion process.

., «'<Mtinitn«*lfrl fiber*
Limr „ , .... ....
' Pom (brand! t;la« fitter*
'.U'VI | i r -
Figure 2.19: Schematic of different available precursor material for the pultrusion process
[13].
The die assembly for this process has two distinct sections. The first section is the
heated and the tapered entry region (Figure 2.20), which collects the preheated preform,
rearranges the fiber bundles to the desired shape and melts the polymer. The function of
the taper is to consolidate the preform, thus encouraging elimination of voids and complete
impregnation of the fibers with the polymer matrix. The second section of the die assembly
is known as the land region. It is of uniform cross section without a taper and may have
cooling lines attached to it. The role of this region is to solidify the matrix material forming
the final shape of the pultruded part. It is usually cooled to approximately 50-80 degrees C
(around the glass transition point (TG) of the thermoplastic matrix). The process velocity is
determined by the speed of the pulling system located immediately behind the die assembly.
The last step in this production process is to cut the final product into pieces of the desired
length.
Figure 2.20: Schematic of the tapered section of a standard pultrusion die [13].
There are two important parameters the modeling of this process should be able to
predict: (1) the pulling force required to run the operation at a reasonable speed to produce
parts that are free of voids and contain the desired fiber volume fraction, and (2) the desired
level of crystallinity in the matrix with minimal stress concentration in the heating and
cooling profile of the die. Hence the viscous flow physics and the heat transfer during the
process will play an important role in the determination of these key parameters such as

the clamping pressure for the die, preheating temperatures, cooling temperatures, etc. One
of the draw backs of this process has been formation of a fiber nest near the inlet of the die
due to insufficient impregnation of the resin, which leads to halting of the process to clear
the bunching of the fibers and restarting the process. Also it is usually difficult to make
a multi-axial composite part with this process as the fiber direction is the direction of the
pulling force.
2.4.3 Thermoplastic Tape Lay-Up Process
In this process, the tool, called the tow placement head, is designed to conform to the
geometry of the composite structure. Processing of thermoplastic composites is based on
melting and solidification of the matrix. The matrix requires energy input for melting and
energy extraction for solidification from the system. The method of energy transport can be
global where all of the thermoplastic matrix is melted as in compression molding, injection
molding, extrusion, pultrusion, etc., or can be localized as in filament winding and tape
lay-up where only a portion of the matrix is melted.
Process
In this process, 3-mm to 12-mm wide thermoplastic tape preimpregnated with continuous
fibers is placed on the tool surface (if it is the first layer) or on the substrate (previously
deposited material on the tool). The incoming tape or tow and the previously deposited
material on the head (the substrate) are preheated by laser, gas, or any other methods of
concentrated localized energy. Rollers are used to initiate intimate contact and consolidate
the incoming tape to the substrate below. The localized nature of heating demands the
consolidation process also be localized, and it is commonly referred to as in-situ consoli-
dation. Additional, local energy may be provided to heat all the layers underneath in the
thickness direction to further improve the overall degree of bonding, healing and intimate
contact. Void content within the tow and the substrate decreases under the pressure of the
consolidation rollers.
In most industrial applications the thermoplastic tape lay-up process is automated and
also known as automated tow placement (ATP) process. In this process, a relatively thin
tape is consolidated on a substrate under the application of heat and pressure (Figure 2.21).
In most cases, the feed tape, the heater (gas, induction, laser etc.) and the consolidation
rollers/shoes traverse the substrate at a predefined path and velocity.
The material used mostly in aerospace industry is carbon fiber preimpregnated with
PEEK or PEKK thermoplastic matrix. Typical applications are the fuselage and wing
structures of the aircraft. One of the important objectives and advantages of the ATP
process is to eliminate the use of a huge autoclave in order to make the process more cost
effective. Also, the ability to make the part out of the mold is attractive, in addition to
having the capability to create multi-axial laminates and moderately complex structures.
The downside is the investment required in automation and the cost of the tool head.
The demand to be cost effective forces the process to be conducted at the maximum
allowable speed. This requires optimization of the process parameters at desired processing
speed while maintaining the quality of the product. To achieve such goals, a fundamental
understanding of the process is necessary.

4-
Figure 2.21: In-situ thermoplastic tape lay-up process [46].
Transport Issues
Different aspects of the process that can be modeled are intimate contact, polymer heal-
ing and consolidation [47, 48, 49, 50]. To model these processes, one must quantify the
squeeze flow during application of the rollers and the transient heat transfer that governs
the temperature of the resin and affects its viscosity. The heat transfer during cooling in-
fluences the microstructure, entrapment of voids and the quality of the part. The quality
of the part also depends on melting, consolidation, solidification and through the thickness
temperature gradient.
Issues related to consolidation are intimate contact, void reduction and migration, gap
reduction between adjacent layers, adhesion and diffusion of matrix chains. The key issues
for modeling include tow-placement head configuration, consolidation, bonding and the heat
transfer between the incoming tape and the substrate interface. A good bond between the
substrate and the incoming tape requires the interface temperature to be greater than the
melting temperature of the thermoplastic. The temperature gradient through the thickness
is responsible for residual stress development in the composite. The critical issues in the
thermoplastic tape lay-up (or ATP) process are the heating of the tape above the melt
temperature for good bonding with the previous "substrate" layer, without overheating to
prevent degradation. So, the rate of heat input is a critical process parameter and will play
a role of selection on the type of heater used. The heater width is also a parameter to
provide an optimum heating zone for good consolidation.
The consolidation pressure is also a very important parameter. Consolidation pressure
is applied for void reduction and adhesion to the previous layer. Low pressure may create
pools of resin and poor bonding. Excessive force can squeeze the resin out creating a resin-
starved region, and at the same time can deform the fibers, which will reduce the local
strength. Residual stress development in the part is an outcome of the localized heating
and cooling process described earlier and is an important issue. Intimate contact, diffusion

and healing (the movement of polymer chains across the interface of the new tape layer and
the previous substrate layer) are other important issues.
As it is common with other composite processes, the critical issues are addressed by trial
and error methods on the shop floor. Lack of understanding and lack of process models
makes it very difficult to quantify the quality of the part. Detailed knowledge of process
models, in-situ sensing, controls and feedback can greatly improve the part quality.
2.5 Advanced Thermoset Composite Manufacturing

Methods
The major difference between thermoplastic and thermoset advanced composite manufac-
turing methods from the modeling viewpoint is that one can describe thermoset manufac-
turing methods using the physics of flow through porous media as the resin viscosity is low
enough to move relative to the network of fiber preforms. The three methods we will intro-
duce as examples of this class of transport process are autoclave processing, liquid composite
molding and filament winding. In all of the thermoset manufacturing methods, the impor-
tant phenomenon one should also include during the modeling process is the cure kinetics
of the thermoset polymers as it influences the transport mechanisms during processing.
2.5.1 Autoclave Processing
An autoclave is a large pressure vessel with a heating facility, or one can think of an autoclave
as a large oven with an integral pressurizing facility. A schematic of an autoclave is shown
in Figure 2.22.
composite under
vacuum
vacuum line
blower to
circulate air
table or
mold
\
heat source
Figure 2.22: Schematic of an autoclave.

autoclave
cure
Adhesive
layer )
Tool
(a) Bag- -J Tool I

(c)
Fiber preforms
Finished part
Tool
(b) (d)
Figure 2.23: Schematic of four main stages of an autoclave: (a) placement of adhesive, (b)
placement of fiber preform, (c) autoclave cure, and (d) finished part.
Process
Autoclave process is the earliest method used to make advanced composites for aerospace
applications. The four stages involved are shown in Figure 2.23. The material and tool
preparation stage is initiated by first covering the tool surface with a release film that
allows one to detach the composite from the tool surface readily. The next stage involves
cutting the prepreg (continuous unidirectional fibers partially impregnated with the uncured
thermoset resin) layers and stacking them in a desired sequence on the tool surface to form
the composite lay-up. This is accomplished usually by hand lay up, although great advances
have been made in the use of automated tow placement and automated tape lay up for the
stacking sequence step. For example, the Boeing 777 aircraft tail assembly used a variety
of automated processes [51]. Despite these advances, many parts in the aerospace industry
still rely on hand lay-up for this step. The composite lay-up is covered by peel plies, release
fabric and bleeder material in that sequence. Peel plies provide surface texture and release
fabric allows resin to flow into the bleeders. On top of the bleeder material is the breather
material. The breather material distributes the vacuum over the surface area. A vacuum
bag envelopes the tool, the part and ancillary materials for vacuuming.
The third stage, as shown in Figure 2.23, involves transferring the part into the au-
toclave and initiating the curing step by exposing the assembly to elevated temperatures
and pressures for a predetermined length of time. The goal is to consolidate and solidify.
The elevated temperatures provide the heat to initiate the cure reaction, and the applied
pressure provides the force needed to drain the excess resin out of the composite, consoli-
date individual plies or prepreg layers and compress the voids. For thermoset composites
this step is irreversible. Hence, it is necessary to subject the composite part to the correct
processing window of temperatures and pressures to ensure a quality part.
The temperatures and pressures are of the order of 100-200 degrees C and 500-600 kPa
respectively. Also, if one wants to manufacture a large part, a large autoclave is necessary.
As the autoclave is a pressure vessel, it is usually made as a cylindrical or axisymmetric
tube with a door at one end. As the autoclave must be strong at high temperatures as
well, the autoclave is an expensive piece of equipment usually made out of welded steel. An

example is shown in Figure 2.24. Once the part is cured, it is removed from the autoclave
and inspected visually and by ultrasound or x-ray for defects, trimmed usually by a router
or waterjet.
Figure 2.24: A typical autoclave.

Curing is the most important autoclave processing step. Hence it has been the main
focus of modeling. The magnitude and duration of the temperatures and pressures to
which the composite is subjected to during the curing step affect the final quality in terms
of thickness variation in the composite, warpage and void content in the composite.
Transport Issues
To address these critical issues, one needs to understand the mass, momentum and heat
transfer that the composite undergoes during the curing cycle. The temperature and the
pressure of the autoclave influences the temperature of the composite, the degree of cure
of the resin, the resin viscosity, the resin flow, fiber volume fraction of the composite,
the change in the void sizes, residual stresses and strains in the composite, and the cure
time. We will discuss in a later chapter how to develop a model for autoclave processing.
However, due to the extensive requirements of material data and batch-to-batch variation
in properties, one can apply these models effectively only to simple geometries. For complex
geometries one must combine models with sensing and control to produce successful parts.
The advantages of autoclave processing are that it can produce composite structures
with very high fiber volume fraction. Also, a lot of empirical data is available on this
process which makes it attractive when reliability outweighs the cost. Also once the most

time consuming part of the process, the production of the master or the prototype, is
completed, duplication can be carried out at relatively low cost. The major disadvantage of
autoclave processing is the high cost associated with the initial investment of an autoclave
and the limitation on the size of the part due to the size of the autoclave. Also, hand lay
up is an expensive proposition and can introduce many human errors in the manufacturing
of the composite and can lead to a variety of defects. Also, it is difficult to calculate the
time and cost to design a new master prototype as most of the knowledge base is empirical.
Hence, different industries are reluctant to replace other materials with composites and use
autoclave processing to make the part.
2.5.2 Liquid Composite Molding

All liquid molding processes involve impregnation of the resin into a fibrous network bed.
The goal in these processes is to saturate all the empty space (pores) between the fibers with
the resin before the resin gels. This would be difficult to accomplish with highly viscous
thermoplastic resins as their viscosity is very high and impregnation would require very
high pressures. Thermoplastic resins are not generally used with this process as one of the
attractive features of liquid molding processes is to limit the equipment to low pressures
Though there is recent interest in using cyclic thermoplastics which have low viscosities.
Liquid composite molding processes encompass resin transfer molding (RTM), vacuum
assisted resin transfer molding (VARTM), structural reaction injection molding (S-RIM),
co-injection resin transfer molding (CIRTM) and other subsets where the basic approach
is to separately inject the liquid resin into a bed of stationary preforms. There are minor
differences in the above processes that lead to slight or sometimes formidible modifications
in the modeling of the process.
Process
Resin transfer molding consists of a mold cavity that is in the shape of the part to be
manufactured. The fiber preform is placed in the cavity. The mold is closed and clamped or
held under pressure in a press. The resin is injected into the compressed preform through
one or more gates from a pressurized container. Once the mold is full, the injection is
discontinued and the resin is allowed to cure. This cure may be initiated by either heating
the mold which heats the resin as it flows into it, or by addition of inhibitors that initiate
the cure after a time interval allowing the resin to first complete the impregnation of the
preform. The mold is opened once the cure is complete or the part is sufficiently hardened
to be demolded. These steps are depicted in Figure 2.25.
RTM offers the promise of producing low-cost composite parts with complex structures
and large near net shapes. Relatively fast cycle times with good surface definition and
appearance are achievable. The ability to consolidate parts allows considerable time saving
over conventional lay-up processes. Since RTM is not limited by the size of the autoclave or
by pressure, new tooling approaches can be utilized to fabricate large, complicated struc-
tures. However, the development of the RTM process has not fulfilled its full potential.
For example, the RTM process has yet to be automated in operations such as preforming,
reinforcement loading, demolding, and trimming. Therefore, RTM can be considered an
intermediate volume molding process [52, 53].
VARTM and SCRIMP are slight modification of the process where the top half of the
mold is replaced by a vacuum bag (as in an autoclave) and a permeable layer is introduced
at the top or the bottom to facilitate the distribution of the resin throughout the part

quickly. The process relies more on pulling the resin by creating a vacuum from a container
of resin at atmospheric pressure. Figure 2.26 shows the steps in the VARTM process.
1) Preform
Manufacture
5) De-molding
\ /
3) Resin V
Injection A
2) Preform
Compression 4) Resin Cure
Figure 2.25: Schematic of RTM process steps [54].
Vacuum bag Fiber preform

under vacuum
Mold
Vacuum pump
Stepl Step 2
Resin impregnates
Resin injection fibers and cures
StepS Step 4
Figure 2.26: Schematic of VARTM process steps [55].
This process has replaced RTM for some applications due to its simplicity, low initial
capital investment and the ability to manufacture large structures such as bridge sections
and rail carriages as shown in Figure 2.27.
Also, the cost is kept low due to low pressures used in the manufacturing process and
the reactions being carried out at room temperature. It only needs one tool surface, and
the top surface is bagged as in autoclave processing which also cuts down on the tooling
costs. The disadvantages of VARTM are poor surface finish on the bagging side, limitation
to nearly flat structures, time involved in material preparation, poor dimensional tolerances
and lack of automation. The co-injection process, as shown in Figure 2.28, can use RTM
or VARTM process where two different immiscible resins are injected and co-cured to form
a composite containing different resins.

Figure 2.27: Bridge section [56] and railway carriage [57].
/ Separation layer
Vinyl ester
Figure 2.28: Co-injection process which can be RTM or VARTM where two different im-
miscible resins are injected into a fiber preform and co-cured to form a composite [58].

Transport Issues
Several unresolved issues in LCM encountered by composite engineers are mainly in the
areas of process automation, preforming, tooling, mold flow analysis, and resin chemistry.
During the last decade, there have been rapid advances in LCM technology that demonstrate
the potential of the LCM processes for producing advanced composite parts.
In the last decade, one of the major issues faced by manufacturing engineers using
these processes was how and from what locations they should inject the resin into the fiber
network. The goal is to produce a void-free part with uniform distribution of the resin in
between the spaces of the fibrous network. Of course, this would be a function of the fibrous
network, of the part geometry and the fiber volume fraction needed to be achieved, and
also of the maximum pressure available to accomplish the task.
To manufacture parts, practice had converged on trial and error methods in which
the modus operand! was that as certain areas were seen to be resin starved, the injection
location was moved closer to it. One of the difficulties was that the resin movement and
impregnation could not be seen inside a closed mold, so the only way to check if the filling
was successful was to wait until the part had cured. Hence, the part had to be rejected if
there were big unfilled areas, and a new location for the gate was chosen based on conjecture
about the impregnation process. This trial and error procedure was repeated for every
new prototype to be attempted by liquid molding. Many net shape composite parts that
were good candidates for this process were too challenging to attempt by trial and error
methods as the possibilities to fill the empty spaces between the fibers were numerous.
The manufacturing engineer realized the potential of mathematical models and numerical
simulations.
Hence the transport issues to be addressed in this process include impregnation of the
resin inside the fiber preform. The fiber preform may be highly anisotropic and heteroge-
neous and may have more than one scale of pore sizes. Heating of the resin by the mold
to invoke resin cure makes the process nonisothermal, and one must account for heat con-
duction between the mold, fibers and the resin. The flowing resin changes the heat transfer
picture as the heat is also convected due to the movement of the resin. The viscosity of
the resin will change due to the heating of the resin and initiation of the cure, which will
influence the flow dynamics. Hence the flow equation may be coupled with the heat trans-
fer equation and the cure kinetics. Flow and heat transfer through porous media forms
the basis of modeling such processes, where one has to consider empirical relations such as
Darcy's law and heat dispersion coefficients to explain the distribution of resin and heat in
such processes, discussed in detail in Chapter 8.
2.5.3 Filament Winding

Process
The filament winding process is usually used for the manufacture of cylindrical and ax-
isymmetric hollow composite parts. In this process, either wet filaments or preimpregnated
tapes are laid on a rotating mandrel. Schematics of a filament winding machine and the
process line are shown in Figures 2.29 and 2.30, respectively. The fibers and parts made
from filament winding are shown in Figure 2.31.
The winding may be accomplished either by depositing preimpregnated prepregs on the
mandrel (dry winding) or with the fibers being impregnated by passing them through a
resin bath (wet winding). The fiber tows or prepregs are placed on the mandrel under a
fiber tension with a prescribed speed guided by a crosshead. If the resin is a thermoplastic
resin, heat is applied to the tape simultaneously with the winding (usually automated tape

Crossfeed Housing
Figure 2.29: Schematic of a filament winding machine [59].
Compaction
Nip-Point Heater
Mandrel
W V
J V
V Tensioner
V
Figure 2.30: Schematic of the filament winding process [59].
Figure 2.31: Fiber forms and filament wound parts [60].

placement is used for thermoplastics). In the case of thermosets, the mandrel is wound and
may be cured in an autoclave or on-line. During this process, the physical phenomena that
occur are the curing of the resin and dissemination of the heat generated to the ambient.
There is also fiber slippage due to the presence of the uncured resin between the fibers and
as the fibers are under tension. Moreover, voids may form due to air trapped between the
bands of fibers. The mandrel and the composite expand due to changes in temperature,
which leads to the development of thermal stresses and strains, adding to the stresses
developed due to the fiber tension.
Issues
The process variables that can be selected and controlled independently are the winding
speed, fiber tension, and external temperature or heating rates. Hence, the process model
should provide information regarding the mandrel temperature and the temperatures inside
the composite, degree of cure, viscosity, fiber positions, stresses and strains, porosity, and
winding and curing times. The transport of the resin here through a moving fiber bed and
also the cure kinetics reaction that changes the viscosity of the resin requires one to address
the flow, energy and reaction kinetics.
2.6 Exercises
2.6.1 Questions
1. What is the main difference between metal and composite parts in terms of the prop-
erties of finished parts and the raw materials that are used to manufacture them?
2. Why were composite materials used mainly in some selected industries, such as the
aerospace industry, during the early stages of composite material development?
3. What are the two major classes of composite manufacturing processes in terms of
types of molds being used? Give examples.
4. Describe the injection molding process by using all of these words and terms: high-
volume production, thermoplastic resin, solid pellets, short fibers, fillers, feeding, hop-
per, barrel, screw, melting, mixing, functions as a piston, sprues, runners, solidifica-
tion, and ejection.
5. What is a pellet? What are the ingredients? What is the size of a typical pellet?
6. Why is the length of fibers that solidify in the final part limited in the traditional
injection molding process? What is an alternative approach to overcome this? What
is the advantage of using longer fibers in this new approach?
7. While modeling the transport phenomena in the injection molding process, what phys-
ical conservation laws are used? What are the independent and dependent variables
in them?
8. What is "fountain flow" in injection molding? What process and material parameters
determine its significance? What is the result of this flow?
9. What are "skin" and "core" layers in injection molding?

10. Does the length of the fibers change during the flow of suspension in injection molding?
Explain why.
11. What makes injection molding so popular that nearly 20% of the goods are manufac-
tured by this process? What are the advantages and disadvantages of this process?
12. Give some examples of common products that are injection molded.
13. Describe the extrusion process by using all of these words and terms: hopper, polymer
pellets, barrel, screw, die, plasticize, compound, cross sections, puller, sizer, and cutter
or coiler.
14. How does the screw of an extrusion machine work?
15. What are the similarities and differences between the extrusion and injection molding
processes?
16. Give some examples of common products that are manufactured with the extrusion
process.
17. In the last few years, the extrusion process has been modified to allow extrusion of
polymers containing reinforcement. What is the reason for this modification?
18. What are the two phenomena that help to soften and then melt the solid polymer
pellets in an extrusion machine before it is pushed by the screw? Which one creates
more heat?
19. When is a cooling system needed in an extrusion machine? If we turn off the heaters,
do we still need a cooling system? Why?
20. What is "plasticating?"
21. What is "die swelling?" What causes it?
22. If you are asked to design an extrusion machine, how would you calculate the power
needed to run the screw and the pumping rate? What types of suspension flow would
you solve in your model?
23. Describe the compression molding process by using these words and terms: composite
material, mold cavity, pressure, and deform.
24. Compare the injection molding and extrusion processes in terms of (i) ease in material
handling, (ii) automation, (iii) amount of material deformation, (iv) regions of very
high stress in material, (v) need for gates in the mold, (vi) damage of fibers, (vii)
using longer fibers, (viii) achieving higher fiber volume fractions, (ix) cycle time, (x)
repeatability, (xi) dimensional tolerances, (xii) amount of initial investment, (xiii)
storage time and conditions for material, (xiv) difficulty of mold design, (xv) residual
stresses in the parts, (xvi) delamination, and (xvii) warpage.
25. What are the most commonly used materials for the compression molding process?
What are the different versions of them?
26. Describe the procedure of forming the sheets of SMC material.

27. What is "initial charge" in the compression molding process? Why is it crucial to
properly place it inside the mold?
28. In compression molding, what are the typical values for temperature and pressure
within the SMC material during heating and compression? What is a typical cycle
time?
29. Although it is small, why is the flow in compression molding critical for determining
the physical and mechanical properties of the composite?
30. Describe "post-cure" in compression molding. Where does it take place? Why is it
needed?
31. Why is the mold design very important, and why is the overall cost of the molds
usually high in compression molding?
32. What are the most commonly used resin systems in SMC materials for the automotive
and aerospace industries?
33. What is "in-mold coating?" Which industry usually uses it?
34. Why are the temperature distribution and rate of cooling important in the compression
molding process?
35. The tensile strength and elastic modulus of compression molded parts might exhibit
siginificant variations from one molding to another. What are the two main reasons?
36. What are the three advanced thermoplastic manufacturing methods? What is the
common assumption used to model them?
37. What are the main issues in advanced thermoplastic manufacturing methods?
38. Describe the sheet forming process by using all of these words and terms: thermoplas-
tic matrix, short and long fibers, unidirectional or multi-axial sheet preform, stacked
or preconsolidated, forming temperature, mechanical or hydraulic press, form, curvi-
linear tool surface, and cooling.
39. What is "forming temperature" in the sheet forming process?
40. How is incremental reforming of a composite part performed in the sheet forming
process until the final desired geometry of the part is attained?
41. What are the unique advantages of sheet forming over other thermoplastic processing
methods?
42. What are the three major composite sheet forming processing methods?
43. In the stretch forming process, the major issues are wrinkles and folds in the final parts.
What causes them? What type of mathematical model would help the manufacturer
to overcome this hurdle?
44. Describe the pultrusion process by using these words and terms: drag, fibers, ther-
moset or thermoplastic matrix, supply rack, temperature control, and tool.
45. What are the main differences between thermoset and thermoplastic pultrusion?

46. The die assembly for the pultrusion process has two distinct sections: (i) the heated
and tapered entry region, and (ii) the "land" region. What are the functions of these
sections?
47. Where and how does a fiber nest occur in the pultrusion process?
48. Describe the thermoplastic tape lay up process by using these words and terms: ther-
moplastic tape, continuous fibers, tow placement head, subtrate, preheating, rollers,
consolidation, conform, and local or global melting.
49. What are the major issues in the thermoplastic tape lay up process?
50. Can one single mathematical model be applicable for both thermoplastic and ther-
moset advanced composite manufacturing methods? From the modeling viewpoint,
what are the major differences between these two methods?
51. Describe the autoclave process at four stages: (a) placement of adhesive, (b) placement
of cure, (c) autoclave cure, and (d) finished part.
52. What are the typical temperatures and pressures in the autoclave process to consol-
idate and solidify the material? Why is it important to have a proper processing
window of temperatures and pressures for thermoset materials?
53. In the autoclave process, what are the functions of peel plies, release fabric, bleeder
material, breather material, and vacuum bag?
54. During the curing step in the autoclave process, how is the final quality of the com-
posite part affected by the magnitude and duration of the temperatures and pressures
to which the composite is subjected? Explain in terms of the process parameters and
variables used in the mathematical models.
55. What are the advantages and disadvantages of autoclave processing compared to other
methods?
56. Describe the liquid composite molding process by using these words and terms: bed
of fibrous network (preform), resin, impregnation, cure, and demolding.
57. What do RTM, VARTM, S-RIM, and CIRTM stand for? What are the differences
among them?
58. What are the advantages and disadvantages of VARTM over RTM?
59. What are the critical issues in the liquid composite molding process?
60. Describe the filament winding process.
61. What are the two types of filament winding processes? What is the difference between
them?
62. What are the key processing issues when dealing with advanced thermoplastic com-
posites? How do sheet forming, advanced tow placement and thermoplastic pultrusion
processes try to address some of these issues? How can modeling help?

63. List important transport issues in thermoset filament winding, autoclave processing
and liquid composite molding. Name at least two issues that are common to all
the thermoset processes listed above, and name two issues that are specific to each
individual process.
64. You have been chosen to select a composite manufacturing process due to your fa-
miliarity with the processes as a result of the course you took at the University of
Delaware. Your company is looking at making the following five components and
would like you to recommend which process should be considered with a single sen-
tence explanation as to why you selected that process. 1.) Short fiber reinforced
dashboards for the new Acura car. 2.) Telephone poles for the city of Newark 3.)
I-beams for Ford Passenger Vans 4.) Axi-symmetric casing for the rocket motor 5.)
Recycleable door panels for the Mercedes Benz 6.) A composite spring for a helicopter.
65. Which of the cross sections in Figure 2.32 cannot be filament wound?
Figure 2.32: Cross sections for filament winding [60].

1. In order for composites to be widely used, especially by consumer goods industries
such as automotive and sporting goods, two major goals had to be achieved: (i) the
of raw materials had to be reduced, (ii) manufacturing methods had to
be developed to achieve high production by reducing the manufacturing
time.
2. As composites are heterogeneous materials, there is simultaneous transfer of ,
and at , and scales, often along
with reaction, in a multiphase system with time dependent material prop-
erties and boundary conditions.
3. Composites manufacturing processes can be broadly grouped into three categories.
(i) short fiber manufacturing methods: involve the transport of
or fibers and as a into a or through a
(ii) flow or advanced thermoplastic composites manufacturing
methods: involve deformation of or long aligned fibers preim-
pregnated with resin under applied stress, (iii) media or ad-
vanced thermoset composite manufaturing methods: involve impregnating
and nearly stationary fiber networks with resin.
4. As the making of metal molds can be very expensive, one can justify the use only for
high-volume production parts. Recently, researchers are exploring the use of
molds reinforced with powder for small-volume production or for prototype
development.
5. The molding time in injection molding is usually of the order of a few

6. In the injection molding process, the important process parameters that can be con-
trolled on the injection units are the temperature, and
speeds, pressure, and in some instances the temperature.
7. In the injection molding process, the material and geometric parameters that will influ-
ence the manufacturing process and the final properties of the part are the
rheology, the type and content, mold cavity and , the
locations of and on the mold.
8. In the injection molding process, the filled thermoplastic pellets usually contain a
second, discontinuous, usually more rigid phase blended into the polymer. When the
aspect ratio (ratio of largest to smallest dimension) of the second component is around
one, it is referred to as a If the aspect ratio is one to two orders of
magnitude larger, then it is called as
9. In the injection molding process, the most commonly used reinforcements are .
and short usually less than in length.
10. In the injection molding process, the parts usually have a fiber volume fraction be-
tween and %. Filled or reinforced materials provide much dif-
ferent properties than the base resin. For example, reinforced polypropylene provides
higher and lower characteristics than neat polypropylene. In
practice, fibrous reinforcements used with glass fibers dominate the market although
the and fibers provide higher stiffness and strength but are sel-
dom used due to the high of raw materials.
11. The traditional injection molding process limits the length of fibers that solidify in the
final part since the high rates in the barrel and the passage of fibers through
narrow gates and openings in the mold cause significant fiber Usually, the
fiber diameter is of the order of few , and the final length distribution,
irrespective of the starting fiber length, is of the order of to [aa..
The starting length of these fibers in the log-like pellets is usually of the order of
to mm. As a result, new methods to produce pellets containing
longer fibers were developed in which the fibers were pultruded and stayed bundled
together and were not dispersed in the pellet by the action of compounding. These
pellets produced final parts that retained a higher percentage of longer fibers and
consequently showed a significant increase in and toughness.
12. In the injection molding process, the : material selected also plays
a role in the final physical and optical properties.
13. The issues that relate to transport phenomena in the injection molding process are the
of fiber suspensions as they occupy the closed mold, the of the
fibers during the flow, fiber distribution, fiber , and the
transfer that changes the microstructure of the resin.
14. One can account for the mass balance of the suspension in the injection molding
process which can be treated as a material, at least for the short fiber
materials.
15. The conservation of the fiber orientation field in the injection molding process sim-
ply states that if the orientation of the fibers disappears in one direction, it should
in some direction.

16. One can account for the momentum balance of the suspension in the injection molding
process to describe the and the fields during the flow process.
This requires one to describe the constitutive equation between the applied
and the rate experienced by the material. As the thermoplastic melts are
thinning, the viscosity is known to with rate. Addition
of fibers can change the stress strain rate behavior and even make it
17. The energy conservation model in the injection molding process allows one to describe
the history of the melt in the channel between the screw and the barrel,
where it gets its input from the on the barrel and due to viscous
caused by the of the suspension. It also allows one to keep track
of the history in the closed mold as the suspension enters into it, which
plays a crucial role in the resulting
18. In the injection molding process, there are some microscale phenomena occurring si-
multaneously: molecular , , spherulitic growth of polymers during
solidification, and fiber , breakage due to , shearing action in the
screw that results in a , length distribution. For long fiber suspensions, the
constitutive equation may change and also issues such as fiber , clustering
may need to be addressed.
19. The coupling between the transports of and creates a
flow mechanism in injection molding. As the walls are than the core, the
suspension viscosity is near the walls as compared to the core. Hence, under
the same pressure, the suspension in the core moves of the suspension near
the walls, spreading from the like a
20. In the injection molding process, flow (which is the boundary of the
and the that it is displacing, and also known as flow ), causes the
fibers to align in the direction of the near the mold walls and is called the
21. Lack of control of fiber and causes variation in part properties

from one injection to another in injection molding.
22. The screw of an extrusion machine is usually machined from a solid steel rod and fits
within the barrel with less than a clearance. To pump a suspension through
a die, the screw is designed to generate over to atmospheres of
pressure in the suspension.
23. For a simple and crude explanation of an extrusion machine, one may think of a bolt
as the , the nut as the , and the wrench as the If one
turns the bolt and holds the wrench in place, the nut will move forward.
24. (SMC), the most commonly used material for
process, may involve either (i) compounding a resin, combining it with and
, or (ii) prepregs (impregnating a fiber with a resin).
25. SMC material is prepared as follows: is placed on a nonporous nylon sheet.
are added to it. A cover sheet is applied onto the fibers. This sheet,
enclosed between the nylon sheet and the cover sheet, is then passed through several
compaction These mix the resin and fibers together, and also
the sheets. The resin cures slowly, and it takes approximately for the SMC
sheet to be ready to be used in the compression molding process.

26. Several types of SMC are currently used in industry: SMC-R (reinforced with fibers
oriented ), SMC-C (reinforced with unidirectional fibers), SMC-
C/R (reinforced with both oriented and unidirectional fibers),
SMC-D (reinforced with , but discontinuous fibers).
27. It is possible to use both thermoplastics and thermosets in SMC, but the majority of
SMC is done using
28. The final properties of composite parts are influenced by the and
of the initial charge in the mold.
29. In the compression molding process, after SMC material is placed and the mold is
closed, the heated top and bottom platen containing the two halves of the mold
cavity are brought together. This generates and to initiate the
of material.
30. In , after the part is partially cured inside the mold, the mold is
opened slightly and a is injected in the mold. Subsequently, the mold is
again, causing the resin to coat the outside of the part filling any
on it. This greatly improves the on the part and can save several
stages in the painting process.
31. Due to their high viscosity, it is extremely difficult to process thermoplastic resins if
they have to be forced to occupy the empty spaces between fibers to form an advanced
thermoplastic composite. To circumvent this problem, the resin is into the
fiber bundles, or is sprayed as commingled or with the reinforcing
fibers so that the resin does not have to travel far when and are
applied to occupy the empty spaces between the fibers.
32. In sheet forming of nonreinforced thermoplastic sheets, the sheets are usually held in
place along the edges over a tool surface and brought up to their material softening
temperature. The most common forming methods are where the
sheet is between matching dies, and in which a vacuum is pulled
through small holes in the tool face, pulling and spreading the sheet down over the
surface.
33. In composite sheet stamping or matched-die press forming, the composite blank is
heated to the temperature and then stamped against tool surfaces. A
variation on this is tool stamping wherein one or both sides of the die are
made compliant. This helps maintain an even consolidation across the part
in case of any tool
34. In diaphragm forming, the blank is held between two disposable, plastically de-
formable diaphragms of either or During the forming cycle, the
diaphragm edges are clamped, heated along with the blank and deformed through the
use of pressure to the tool surface. The diaphragms serve to hold the blank
in tension and prevent fiber that can occur under compressive stresses.
When forming parts containing continuous fiber reinforcement, the diaphragms are
clamped but the blank cannot be. This is due to the of the fiber reinforce-
ment.
35. Hydroforming is a process similar to diaphragm forming. However,
is used instead of to provide the pressure behind a permanent rubber di-
aphragm.

36. Pultrusion is one of the oldest composite manufacturing processes as it has been
around since the late 1940s. It was originally designed to manufacture
37. For thermoset pultrusion, one can use bare fiber rovings to go through a liquid ther-
moset before entering the for curing and cross-linking. On the
other hand, thermoplastic resins are preimpregnated with fibers in the form
of a tape or the fibers pass through a station of polymer bed, where the
thermoplastic powder attaches itself to the charged fiber surface. Therefore, thermo-
plastic pultrusion requires a area.
38. There are two important aspects to modeling the pultrusion process. The first is
to determine the required to run the operation at a reasonable
speed to produce parts that are free of and contain the desired fiber vol-
ume fraction. The second is to achieve the desired level of in the matrix
with minimal concentration. Hence, the viscous flow physics and the heat
transfer during the process will play an important role in the determination of these
key parameters such as the pressure for the die, temperatures,
temperatures, etc.
39. The key issues for modeling the thermoplastic tape lay up process are: (i) tow-
placement head , (ii) , (iii) , (iv) during melt-
ing of the resin in the incoming tape and the substrate interface without
the matrix. A good bonding between the substrate and the incoming tape requires
the interface temperature to be than the temperature of the
thermoplastic. The temperature gradient through the thickness is responsible for
development in the composite.
40. The winding process variables that can be selected and controlled independently are
the (i) winding , (ii) fiber , and (iii) either external
or rates. Hence, the process model should provide information regarding
the temperatures of and , degree of , , fiber
, and , , and winding and curing
The transport of the resin here through a moving fiber bed and also the cure kinetics
reaction that changes the viscosity of the resin requires one to couple the equations
of , and

Chapter 3
Transport Equations for

Composite Processing
3.1 Introduction to Process Models

A model is an idealized mathematical representation of a physical system or process. To
describe a model, one needs physical laws, constitutive equations and boundary conditions
once the system to be modeled is defined and outlined. In this chapter, we will derive the
physical laws of fluid flow and heat transfer that are encountered in composite manufacturing
processes. Models are useful in expressing the understanding and codifying the knowledge
about the manufacturing operation. Models provide detailed information about a process
such as flow front location, resin pressure, temperature and flow rate. A model is like a
scientific hypothesis which should 'be validated with experiments. If experiments conflict
with the hypothesis, we continue to revise the model until it agrees with the experiments.
Models help us to either eliminate or reduce the trial and error approach used during
composite processing. A scientist is more interested in understanding the physical world by
using models, whereas a process engineer is usually interested in manipulating the model.
A model is formulated using the following six elements:
1. Model or system boundary: Region in which one should consider physical and consti-
tutive laws.
2. Physical laws: In this chapter, we will derive, and then use the conservation equations
for mass, momentum and energy as the physical laws.
3. Constitutive laws: Deformation of materials, transfer of heat, resin cure chemistry,
etc., are expressed through phenomenological laws that are formed based on certain
assumptions and experimental observations in simple geometries.
4. Boundary conditions: The external influences that affect the system or process are
expressed by formulating boundary conditions for the governing variables.
5. Assumptions: In order to simplify the models, assumptions need to be made. This
will allow one to neglect some of the terms in the physical laws. The assumptions
may be about constitutive equations or the geometry of the system and boundary
conditions to simplify them.
6. Experimental validation: For a model that is expected to describe physics, it is impor-
tant to conduct controlled experiments and measure relevant variables and compare

them with the model predictions.
The philosophy behind a good model should be "prepare for the worst and hope for
the best." The assumptions made must still maintain the behavior and features of the
system we are trying to model intact. Otherwise, the model may not properly represent the
physical system.
The general approach to buildind a model is illustrated in Figure 3.1.
Physical Process
Objective
Assumptions and
Simplifications
Mathematical Model
Solution Method
Analytic or Numerical
Results
Adequate Solution NO
,rYES
NO Agree with
Process Physics?
,,YES
Useful Predictions/Designs
Figure 3.1: Flow-chart to build a model.
3.2 Conservation of Mass (Continuity Equation)

In this subsection, we will derive the differential equation for the physical law of conservation
of mass which is also known as the continuity equation for any fluid flow. Then, we will
modify this equation to address resin flow in composite processing applications to include
the presence of fibers.

3.2.1 Conservation of Mass
We will derive the mass conservation equation in two different ways: (i) using Gauss'
Divergence Theorem on any arbitrary shaped control volume, and (ii) a Pseudo derivation
with a prism control volume.
Derivation 1: Divergence Theorem on Any Arbitrary Shaped Control Volume

Let's consider flow of a fluid within a region with velocity U and density p. Although the
derivation is independent of the coordinate system used, let's use the Cartesian coordinate
system here, and let U and p be functions of x, y, z and time t hence we can represent them
as \J(x,y, z, t) and p ( x , y, z, t), respectively. The mass of the fluid within any arbitrary fixed
control volume V at any time t is calculated as M — fv pdV . The rate of increase of M is
calculated as
dM d f f dp
Here, the total time derivative term on the left hand side of Equation (3.1) is carried inside
the integral, by using the Leibniz rule,1 as a partial time derivative. The additional terms
from the Leibniz rule dropped out since the control volume is fixed in space.
The rate at which fluid mass enters the control volume V through its boundary S is the
flux integral and is given by
q = - f pn-UdA, (3.2)
Js
where n is the unit outward normal to S as shown in Figure 3.2.
Figure 3.2: Control volume for the derivation of conservation of mass equation.
1
The Leibniz rule states that
-
at, A^ A(t)
for any continuous function / and its time derivative d f / d t .

In Chapter 8, we will study the micro mold filling issues which may lead to micro voids.
We will model the delayed saturation of the inter-fiber bundles after the flow front passes,
as having imaginary sinks within the reinforcing preform. If there is a sink within V that
absorbs fluid mass at a rate of s(x,y, z,t) mass per unit volume per unit time, then
s(x,y,z,t)dV (3.3)
.'
mass per unit time.
The rate of increase of mass within V is equal to the rate at which mass enters V through
<S, minus the rate at which mass is lost:
dV = - f pn-UdA- I sdV. (3.4)

t Js Jv
In order to combine these integrals, we need to convert the surface integral to a volume
integral so that all the integrals will be volume integrals. For this purpose, Gauss' divergence
theorem will be used. This theorem states that
/ n • (oB) dA= / V • (aB) dV (3.5)
Js Jv
for any scalar a and vector B within a volume V bounded by surface S. n is the unit
outward normal vector on S. By using Gauss' divergence theorem, the first term on the
right hand side of Equation (3.4) could be rewritten as
pn-UdA = f n - ( p U } d A = [v-(pU)dV (3.6)

s Js Jv
where the differential vector operator V in Cartesian coordinates is given by
+ +k
dx dy d
Equation (3.4) takes the following form after Equation (3.6) is substituted into it:
F = 0. (3.7)
Since the considered control volume V is assumed to be of any arbitrary shape, and at
any arbitrary location of the flow region, not only the integral, but actually the integrand,
dp/dt + V • (pU) + s must be zero, too, then
^ + V - ( p U ) = -S. (3.8)
This is the conservation of mass (or, also known as continuity equation) of fluid mechanics.
In a Cartesian coordinate system, it takes the following form by expanding V • (/oU)
l + ^(^)+ |;(^) + l(^)= -s- (3 9)

-
This equation is valid at every location for any fluid flow domain. Here ux, uy and uz are
scalar components of the velocity vector U in the x, y and z directions, respectively. For
most resins, the density is constant and if there is no mass loss, Equation (3.9) reduces to
dux duv du,
-7^- + ~ + ~ = 0. (3.10)
ox ay oz

Derivation 2: Pseudo derivation with a Control Volume
This alternative derivation requires additional steps but is simpler to understand and fol-
low than the first one since it doesn't require knowledge of the Leibniz Rule and Gauss'
Divergence Theorem. This derivation also makes it easier for the reader to understand the
physical meaning of the individual terms in the conservation of mass equation.
Consider a fluid flow within a region with velocity U and density p. Let us again use
the Cartesian coordinate system here, and let U and p be functions of x, y, z and time
t represented as \J(x,y,z,t) and p(x,y,z,t), respectively. However, this time, the control
volume, V has sides of Ax, Ay and Az as shown in Figure 3.3. The mass of the fluid within
this control volume at any time t is equal to M = fv pdV — pAxAyAz. You might object
to this calculation since we treated the density as a constant. Although we let density be
p(x,y,z,t), consider that p appearing in M = pAxAyAz is the volume averaged density
which is within the lower and upper bounds of p within V. The balance of rate of mass
increase (accumulation) inside AxAyAz is given as
Rate of | _ ( Rate of \ ( Rate of \ / Rate of mass lost

mass increase J \ mass inflow I \ mass outflow I I due to a sink
(3.11)
The rate of increase of M is calculated as
— — (pAxAyAz) = AxAyAz -~ (3.12)
since the control volume and hence its sides Ax, Ay and Az are fixed, i.e., not changing
with time. The rate of fluid mass inflow into the control volume V through its face at x is
(pux)\xAy&z. The rate of fluid mass outflow from the control volume V through its face
at x + Ax is (pux)\x+A.x&yAz. Similar expressions can be written through the faces at y
and z for inflows, and at y + Ay and z + Az for outflows as shown in Figure 3.3. Hence,
the net rate of flow is
Rate of \ / Rate of \ . . , ,
. _ — n = AyAz r\(pux)N x — (pux)N
mass inflow / \ mass outflow I
[(pu,
\ A /Y> A -v \( ™,
~ (Puy)
+AxAy [(puz - (puz) IZ+AZ] • (3.13)
If there is a sink within V which absorbs fluid mass at a rate of s(x,y, z,t) mass per
unit volume per unit time, then the net rate of lost mass within V is equal to
/ s(x,y,z,t)dV = sAxAyAz (3.14)

Jv
mass per unit time. On the right hand side of Equation (3.14), s is volume averaged.
Substituting Equations (3.12)-(3.14) into (3.11) results in
-£ AxAyAz = AyAz [(pux) x - (pux^ '

y
+AxAy [(puz) \z - (puz) |^+Az]

(3.15)

P«v
Inflow flux through ^x x (jt + Ax, y + Ay, z + Az).*^ Outflow flux through
the face at x the face at x+Ax
\ «»
#*
/
_^P M ** + A*
"V^ ^ Z"("AZ''" / v ... \

x
..-•-""" ' A
^^
Figure 3.3: Control volume for the pseudo derivation of conservation of mass equation in
Cartesian coordinate reference frame.
Dividing both sides of Equation (3.15) by the control volume AxAyAz leads to
y - ((My) (f)U Z) \Z ~ (f)U z
-s. (3.16)
dt Ax Ay Az
As Ax, Ay and Az —> 0, Equation (3.16) converges to
dp d , , d . , d (3.17)
This is identical to Equation (3.10) in Derivation 1. Or, using the differential vector oper-
ator, V, we can rewrite it as
which is the same as Equation (3.8). Here, dp/dt is the partial time derivative of p at a
fixed spatial location. Alternatively, the continuity equation can be written in terms of the
substantial time derivative Dp/Dt following a fluid particle. Since
5Qdz SQdy SQdz
Dt dt dx dt dy dt dz dt
3() d() d() d()
dt dx dy y dz
(3.19)
UL
then, dp/dt — Dp/Dt - U • V/9. Substituting this into Equation (3.18), and rewriting
V • (pU) as Vp • U + pV • U, we obtain the following
(3.20)

Most fluid flows in composite manufacturing processes will be treated as quasi steady
state (dp/dt = 0), and incompressible (p — constant). Hence, the continuity equation will
simplify to p V - U = — s. In many applications, there won't be any significant sink effects,
so the continuity equation could be further simplified to
V-U = 0 (3.21)
which can be written in open form as
9^+duy_ + duL =
ox oy oz
1 d(rur) I due
r Orn 1
r 80 dz
1 d(r2ur) I due sing 1 du<t> _
~~
rÔ or
o • rt
rsm # o/i
av rsmt//i a<p
o i — \ )
in xyz Cartesian, r9z cylindrical, and rO(f> spherical coordinate systems, respectively.
3.2.2 Mass Conservation for Resin with Presence of Fiber

Here we will derive the equation of mass conservation for resin flow with the presence of
fiber phase. We will assume the following:
• Fibers are incompressible.
• The velocity and stress-strain changes are small in the control volume.
• The process is quasi-static.
• Body forces such as self weight are negligible.
Consider a fluid (resin) flow within a region consisting of fibers as shown in Figure 3.4.
The derivation is very similar to the one in the previous subsection, except that we will
use pb = (mass of resin) /(control volume containing both resin and fibers) as the resin den-
sity, and U = uxi + uyj + uzk as the interstitial velocity of the resin within the com-
posite. Inside a partially filled fibrous region, pb = eSp, where e is the porosity of the
control volume or that fraction of the control volume available for resin to occupy (e —
porous volume/control volume), S is the saturation fraction of the porous space filled by
resin, and p is the actual resin density (resin mass divided by resin volume). In many other
textbooks and in some chapters of this book, the porosity will be written as e = 1 — Vf,
where Vf is the fiber volume fraction. The porous volume within the control volume is
completely empty when 5 = 0, and completely filled when 5 = 1.
The mass balance for a control volume can be expressed as
o
- AxAyAz = AyAz [(pbux) \x - (pbux)

ly+Aj/j
*)
-sAxAyAz. (3.25)
Dividing both sides of Equation (3.25) by AxAyAz and then taking the limit as Ax, Ay
and Az —> 0, Equation (3.25) converges to
dpb d . . d . . d
= pbUx pbUy
7K ~fa( >~dy( >~~dz(pbU^~S' ( 3 ' 26 )

Figure 3.4: Control volume for the pseudo derivation of conservation of mass equation for
resin flow through a fibrous region.
Since p\, =
d(eSp] _ _ 9(eSp) d(eSp) d(eSp) dux duy duz
which can be written in vectorial form as

9(eSp)
= s. (3.28)
Ot
Note that even if the resin density p is constant, the porosity and/or the saturation of
fibrous media may not be constant within the entire region. Hence, V(eSp} may not be
zero everywhere. The reader must keep this fact in mind. Further simplification can be
obtained depending upon the manufacturing process being considered [61].
3.3 Conservation of Momentum (Equation of Motion)

As we have done in Derivation 2 of the previous section, we will consider a control volume
as shown in Figure 3.5. In the figure, only the forces in x direction induced by stresses
are shown. Now, let's take a diversion to understand what a stress on a fluid is. Stress
is a measure of force per unit area transmitted by physical contact either within a body
(of a continuum system, which is a fluid here) or by contact with the body at its external
surface, a is the stress tensor whose components are aij. Each componentCTJJhas two
directions associated with it. The second index j gives the direction of the force per unit
area, and the first index i gives the normal direction of the surface. The surface might be
an external one, or a hypothetical interior one within the fluid domain. The diagonal stress
components, when i — j are called normal stresses, and the off-diagonal components when
i ^ j are called shear stresses.
Usually, the stress tensor is expressed as the sum of two components
[stress tensor] = — pressure [unit tensor] + viscous stress tensor

-P6tj
'yx 1 0 0 'yx
cr,yy a
zy 0 1 0 'xy
T
yy (3.29)
0 0 1 TXZ
The motion of an incompressible substance only determines its stress state to within an
arbitrary isotropic constant (a scalar multiple of 6ij), and that is the negative pressure,
— P. A positive pressure generates a negative normal stress. The viscous stress arises from
the fluid motion, and is related to the deformation of the fluid by constitutive equations
as we will study in the next section. If there is no fluid motion (hydrostatic case), then
all viscous stresses TIJ are zero since there is no fluid deformation. In this case, all shear
stresses cr^ are zero, and normal stresses an are equal to —P.
AyAz
Figure 3.5: Control volume for derivation of conservation of momentum equation for fluid
flow.
Let's consider the forces, in the x direction only, acting on the control volume shown
in Figure 3.5. Once we have the force balance in the x direction, the procedure can be
repeated in the y and z directions as well. The force balance on the control volume yields
x component of x component of
Dux
FT = m total stress forces I body forces, FB due to
on all six surfaces gravity, magnetism, etc.
Du^
— <7T AyAz
:+Aa
ArrAz — a,yx AxAz

y
AxAy
2+Az
(3.30)

Here, Dux/Dt is the substantial derivative of the velocity component ux and given by
Dux/Dt — dux/dt + U • Vu x , and FB is the body force which could be the total of grav-
itational, magnetic, etc. forces per unit area acting on the fluid. For example, if there is
only gravitational force acting on, then FB = pge where, p is the fluid density, g is the
gravitational acceleration, and e is the unit vector along the direction of gravitational force
which is dependent on the coordinate system (e.g., if z axis is the radial axis drawn from
the center of the earth, then e — — k, Fgx = FBV — 0, and FBZ = —pg)-
By dividing both sides of Equation (3.30) by AxAj/Az, we obtain the following:
Du x dP drxx dryx drz

—f^T — —~^ -- 1- 1- H FBx (6.6L)
Dt dx dx dy dz
as Ax, Ay and Az —> 0 in the limit. Similarly, one can repeat the force balance in the y
and z directions as well, yielding
DUy QP (JT C^T* QT

(3.32)
dy dx dy ' dz
^
Duz dP drxz , &ryz . drzz
(3.33)
J
~Dt dz ' dx dy ' dz
One can rewrite the momentum equation with substantial derivative terms in expanded
form as follows
dux dux dux dux dP drx dryx : drz
u
x ^. 1 V i ' z y (3.35)
dt ' dx dy dz dy dx dy dz
duz duz duz duz dP drxz dryz drzz
Uy Uz ^~ - (3.36)
dt ' dx dy dz d^ dx dy ^dz
We can combine Equations (3.31)-(3.33) in vectorial form. The physical meaning of each
term is explained below the equation
T Hydrodynamic force Force due to stresses Body force

Inertia lorce
This is called the conservation of momentum equation, or also known as the equation of
motion. These equations along with the continuity equation describe the physical laws for
the selected system. Considering gravitational force as the only body force (i.e., F = pg),
the equation of motion can be written in Cartesian, cylindrical and spherical coordinates
as listed in Tables 3.1, 3.2 and 3.3, respectively. However, one does need a relationship
between stresses and the deformation of the fluid before one can solve for either pressure or
velocities experienced by the fluid. The equations that describe these are discussed in the
next section.

Table 3.1: The equation of motion in terms of r in. rectangular coordinates in x, y and z
directions.
(z-dir.:) p = _^
dx
+[ f^
dx
+dy^ + dz
P9x
dvt
(y-dir.:) p
(z-dir.:) p
Table 3.2: The equation of motion in terms of T in cylindrical coordinates in x, 9 and z

directions.
dvr dvr Vfj dvr v2 dvr

(r-dir.:) p
"d^ ~r~~dJ r
8P_ ldT6r drzr

--(
dr r dr r 09 oz
H,
dt dr r 89 r dz
= _i^ + fl^2( r 2 T r ( ? ) + ±:
r 89 r dr r 89
(z-dir.:} SF
r aw
^
dz [r dr r 89 dz

Table 3.3: The equation of motion in terms of r in spherical coordinates in r, 9 and
directions.
(r-dir.:)
v
vr , Vr. <l> dvr
I dt T ur dr ~r r rsinl? 9c/>
c9P 1 1
r r rsm rsm9 r J
9-dir.:)
e
at dr "T" r <96> rsinS
IdP I 5 1 d r^ cot
r ~^"
dd ^^~
r3dr rsmOd9 rsm 36 — P9e
Mir.:)
I dP I d I d i cot 0
rsmt rsm

3.4 Stress-Strain Rate Relationship
In the previous sections, the conservation equations of mass and momentum were derived.
The unknown variables appearing in these equations are the velocity vector U, the fluid
pressure P, and the viscous stress tensor T. Pressure P is a scalar, U has three scalar
components, and viscous stress tensor T has nine scalar components; however, only six of
them are independent scalar components if it is a symmetric tensor, as it will be assumed
in this book. A symmetric stress tensor is assumed in order to satisfy zero net angular mo-
mentum of control volumes. Thus, we have ten unknown scalar variables. In the Cartesian
coordinate system, they are ux,uy,uz,P,Txx,Tyy,Tzz,TXy,Txz,Tyz. These variables can be
functions of spatial independent variables x,y,z and time t. However, we have only four
scalar equations, one continuity and three equations of motion. We need six more equa-
tions. In this section, we will study the relation between the stress tensor and deformation
of fluid. They will provide six additional scalar independent equations to complete the set
of equations.
3.4.1 Kinematics of Fluid

The motion of a continuum can include translation, deformation and rotation. The velocity
vector U itself describes the translation of the continuum. Let's write the velocity vector
in Cartesian coordinates, xyz as U = uxi + uyj + uzk, or as U = w;i in short tensorial
notation where i can take values of x,y,z, and i will correspond to unit vectors i, j, or k,
respectively.
Unlike the motion, the deformation and rotation of a continuum are dependent on the
spatial derivatives of velocity as we will see in this subsection. We described the differential
vector operator, V, at the beginning of this chapter. The velocity gradient is given as
VU =
.dux
11 -.
dx dx dx
du. du7
dux duz
i (3.38)
~d7 ~fc
or, using tensorial notation,
dux 9uy Quz dui du2 du3 ~
dx dx dx dxi dxi 9xi
dux QUy Quz dui 9u2 9u3
VU = 9y 9y dy dx2 9X2 9X2
(3.39)
dux 9uy du,
. dx3 dx3 dx3 .
or, as (VU)jj = duj/dxi = Ujti in short. By adding and subtracting |(VU) T , velocity
gradient can be written as
VU =
\ JVU-(VU) T |
rate of strain tensor 7 vorticity tensor 10

u3_ , u2_
dx2 ^ dx3j
dua dui
dxi dx3
(3.40)
The manipulation above was done to decompose the velocity gradient VU into a symmetric
part 5(VU+ (VU) T ), and an anti-symmetric part i(VU- (VU) Thus, one can express
the strain rate tensor as
in = ( u j i + uu).
> 1J \ J-)L ''•:}/
(3.41)
\ I
The rate of strain tensor, 7 describes the rate at which the material (fluid in our case)
is changing its shape irrespective of the translational or rotational motion. If one considers
two close points P and Q within the fluid domain, then the distance between them is
ds = \/<ix • <ix, where <ix is the position vector from one point to the other. One can show
that
2
d(ds}
_
, . , , . ,
— / T x • 'V • /7"V — fiT •'"V- • HT •
,„ ^
I i 4-/ 1
t-tA. I ti-iV \JjJui I'l'] UvJ-i 1 ' V *-* . T r i j J
at
Hence, the rate of change of the squared distance can be written in terms of 7 and ofoc only.
For that reason, 7 is also called the rate of deformation tensor. It is a symmetric tensor
since 7 — VU + (VU) , and A + AT is symmetric for any tensor A. The scalar magnitude
of 7 tensor, which is independent of the coordinate system is given by
(3.43)
and is called the "strain rate."
Components of the rate of strain tensor are listed in Tables 3.4, 3.5 and 3.6 in Cartesian,
cylindrical and spherical coordinates, respectively.
In addition to deformation, the motion of a continuum may include solid body rotation.
Vorticity tensor, uj
Uij = Ujti - mj (3.44)
describes this solid body rotation. The fluid flow is called irrotational if the vorticity tensor
is a zero tensor, i.e., all the components are zero.
Example 3.1: Simple Shear Flow

Consider flow of resin within a region in which the velocity field is given by ux = cy, uy — 0,
and uz — 0 where c is a constant (see Figure 3.6). Find the strain rate and vorticity tensor
for this flow. Also calculate the magnitude of the strain rate.

Table 3.4: Rate of strain tensor in Cartesian coordinates
dx
7yy —
dy
dvy dvx
= 7ya
dx dy
dvz dvy
dy dz
dvx dvz
7xZ ~r\ "T~ ~^
dz dx
Table 3.5: Rate of strain tensor in cylindrical coordinates
=2—
dr
dvr
lee = <* -
r 09 dr
Jzz =
dz
d 1 dvr
r~dJ
1 dvz dvg
7«0 — -r -57T
dO + ~x~~
dz
dvr dvz
~0 1 ^
dz dr

Table 3.6: Rate of strain tensor in spherical coordinates
7rr =
dr
dvr
rd6 dr
1 dv^ vr vg cot i
rsin# dd> r r
d ve\ 1 dvr
= 70r = r — —
Or r r 89
sin 9 d f v^ \ 1 dvg
rsin^ dd>
1 dvr d fvd,
h r— ——
r sin 9 dd> dr V r
Figure 3.6: Velocity profile in steady simple shear flow.

Solution
The rate of strain tensor 7 and the vorticity tensor LJ can be found using Equations 3.41
and 3.44, respectively and are calculated to be
0 c 0 0 -c 0
c 0 0 c 0 0 (3.45)
0 0 0 0 0 0
For this flow, the scalar magnitude of the strain rate tensor is equal to 7 = \/^(c 2 + c2) = c-
Example 3.2: Two-Dimensional Simple Elongational Flow

Consider stretching of a viscous material thin sheet in the x direction as shown in Figure
3.7. This flow is also called simple extensional flow. The velocity field in the sheet is given
by ux — ex, uy — —cy, and uz = 0 where c is a constant. Find the strain rate and vorticity
tensor. Calculate the strain rate. Is the flow irrotational?
ux(x) = cx
y
Figure 3.7: Two-dimensional elongational flow.
Solution
The rate of strain tensor 7 and the vorticity tensor u are calculated to be
2c 0 0 0 0 0
7= 0 -2c 0 0 0 0 (3.46)
0 0 0 0 0 0
Since cj is zero, the flow is irrotational; hence there is no vorticity and because of this, the
simple elongational flow is sometimes called pure shear flow. The strain rate is equal to
7 = /i(4c 2 + 4c2) = 2c. •

Example 3.3: Three-Dimensional Simple Elongational Flow
Consider a cubic rod of viscous material being stretched in the x-direction by velocity
component in the x direction being ux = ex as shown in Figure 3.8. The flow within
this material can be described by the velocity field given by ux = ex, uy = —q//2, and
uz — —cz/2 where c is a constant. Find the strain rate and vorticity tensor. Calculate the
magnitude of the strain rate tensor. Is this flow irrotational?
ux(x) = cx
Figure 3.8: Three-dimensional elongational flow.
Solution
The rate of strain tensor 7 and the vorticity tensor LJ are calculated to be
2c 0 0 0 0 0
7= 0 -c 0 0 0 0 (3.47)
0 0 -c 0 0 0
The strain rate for this case is equal to 7 = -\A(4c2 + c2 + c 2 ) = \/3c. Again this is an
elongational flow and irrotational as u\ = 0. •
3.4.2 Newtonian Fluids

Earlier in this chapter, the momentum equation was derived in terms of the viscous stress
tensor r. In this section, r will be related to the rate of strain tensor 7 in order to complete
the set of equations for the fluid flow. (Recall that, so far the number of equations is less
than the number of unknowns in the equations.) There is no unique relation between r and
7 that is valid for all fluids. However, the simplest relation between them which is valid for
many fluids is a linear relation. This linear relation idea was first proposed by Newton; hence
the fluids which obey this relation are called Newtonian fluids. Later, Navier and Stokes
derived the equations for the flow of Newtonian fluids independently. These equations are
called the Navier Stokes equations. The linear relation is given by
+ M7 (3.48)

where fj, is the viscosity of the fluid. The assumption of mechanical and thermodynamic
pressures being equal (known as Stokes' assumption) yields
(3.49)
Hence, a normal viscous stress TH and a shear viscous stress r^ are given by
(3.50)
(3.51)
Although many fluids are characterized very well as Newtonian fluids, there are many
other fluids which behave differently. The relation between the viscous stress and the rate
of strain tensors is not a linear one as in the Newtonian fluids. Some typical non-Newtonian
fluids are "shear-thinning," "shear-thickening," and "Bingham plastic" fluids. These fluids
will be discussed in detail in the next chapter.
Let's return to Newtonian fluids. If the fluid density is assumed to be constant (incom-
pressible fluid), then according to the conservation of mass equation, dp/dt + V • (pU) =
0 + /oV • U = 0, which requires that V • U = 0. Then, the V • U term in the normal stresses
drops out. So, for constant density fluids, we have
Til = (3.52)
(3.53)
(3.54)
For constant viscosity, incompressible fluids, momentum equations (3.34)-(3.36) reduce to

the following after substituting viscous stress equations (3.50) and (3.51):
dux dux dux dP _i_ Z7V, C\ K K N

• Ux — 1- Uy — h Uz T f Ex ^-J-OOJ
dt dx dy ~dz~ dx dx2 dy2 dz2
dUy dUy dP 'd2u y i d2u y i d2u y _|_ p_ /"Q CC^l
ux ~r -^By ^-"JUj
dt n
dx +
~dy 1h dy dx2 dy2 dz2
fduz duz duz dP i a d2uz d2uz d2uz
+ •U* a ' A* + Bz-
\~dt Ox dy ~dz~ dz dx2 dy2 dz2
or, in vectorial form as

DU
= -VP (3.58)
where V 2 ( ) — d2()/dx2 + d 2 ( ) / d y 2 + d 2 ( } / d z 2 . This is the conservation of momentum

equation for Newtonian fluids with constant density and constant viscosity. Tables 3.7,
3.8 and 3.9 list the N-S equations for incompressible resins in Cartesian, cylindrical and
spherical coordinate systems.

Table 3.7: The Navier-Stokes equations for incompressible resins in Cartesian coordinates
in x, y and z directions.
[ dux ^
r., 1
dt
u
x ^
dux
ox
|
1 u
y ^
dux
dy
1 Uz
dux
~d7
dP \82ux , d2ux , d2ux} , r
1
a 9 1 Q 9 ' a 9
i
OX
' r
arc c*y az J ' -^Sa:
(y-dir.:)
aw y l
x y
L dt dx dy
dP
n
dy ' A1 [ -~i o
ox^ ' ov
*"!y 9 ' oz*
0 9 '
J
By
[ duz duz duz

r* . ~r MX -7; ~~r Uy -— +
dt dx dy
duzl
J
dP
dz +^ [ 9x2
z
I
%2
z
1 z
dz2 J
I T^DBz
Table 3.8: The Navier-Stokes equations for incompressible resins in cylindrical coordinates
in £, 6 and z directions.
, .. . dur dur durr dur r

r-dir.: P\-^r+ur-jrL + — 1^ ~ ~
r +U
-^T
dP d_f\d_ I d2ur d2ur 2 due

dr \r dr
9wg ug due dug

~x
dr -- ' --- ~5^
r 89
IdP d il d 2 <9ur
--5S-
r d0 "5"
dr \r-^-
dr T
r2 "aF
39
I du
--2z , 3w MO 9uz 9w
(z-dir.:) ^, - — + U r _ _z + —+u
dt dr r 69 dz
_^ [ i — f ~^1 1 52«z 5V FBz

Sz r dr \ dr I r2 d92 dz2

Table 3.9: The Navier-Stokes equations for incompressible resins in spherical coordinates
in r, 9 and <f> directions.
+ Ur +
(r-dir.:) P \ gt dr ~*~ r 56 rsm6 dd> r
dP \ dd ( 1 d . 2 ,\ 1 d ( sm. g. dur\ 1 9V
r
9r r 2 ^r(
o" V~? 9r "*-) / r29smOdd
• /i "57;
V ~o7T
96 / r 2o sin
• 2/i
9
2 d 2
T -^7( (u» sm 0) -
r 2 sin 6
,. , I » e e g
dir.:) p 1 -5T+ u '-~a~ H
r aa"
ad rsmv d<p r r J
19P [ 1 9 / 2 9u<A 1 9 / 1 9 . u sm6i

= ---57T
r oti +A« ir^
-^-5-
dr (»•
\ ^—or J + ^^z -^-5^7j(
r* dd \srn6 da e )
1 92ua 2 9ur
r sin2
2
J
9urf, we duj, UA, QUA u&Ur uguj,

-~n
ay ' r ouH7T ~! r sin
^~5~^T
p c/(/> "^ r ' r cot 6
sin (
. ,, dtp
rsind a.i' ir~?"n~
2
dr V "5~
9r / ^J
r 2 ^S
96 V ~^~S
sin 6* ^7i ("*
1 92u^, 2 9ur 2cot6>

r sin 6 9^2
2 2
r 2 sin6 9</> 2 B<t>
Example 3.4: Derivation of Viscous Term in Equation (3.58)

Explain the simplification of the viscous term in Equation (3.58) to /LiV2U from 2^V 2 U.
Solution
As seen in Equation (3.34), the x-component of force due to viscous stresses is drxx/dx +
dTyX/dy + drzx/dz, and for constant density fluids, TXX = 2/j,dux/dx as derived from Equa-
tion (3.50). The x derivative on TXX results in drxx/dx = -^(2fj,dux/dx) = 2/j,d'2ux/dx^.
2
However, we have the resultant force as ^[d ux/dx^ + (etc.)] as seen in Equation (3.55). To
eliminate the coefficient 2 in the momentum equation, one needs to look at the entire terms
as
drxx ^ dryx . drzx _ ( d \ dux~l d \duy «9ux] d \duz
^~ ~^ r ~^ + TT"
dx dy dz ^ \ dx [ dx \ dy [ dx dy \ dz ["dx dz
jp
dy2 dxdy dxdz dz2

, .
(3-59)
The three terms drop out since their summation is zero because Qjfg- + -^ + ^jf = 0 for
incompressible (constant density) fluids. Similar derivations can be repeated in the y and
z directions to show that V • r = /nV 2 U for incompressible Newtonian fluids. •
3.5 Examples on Use of Conservation Equations to Solve

Viscous Flow Problems
The conservation of mass equation (a partial differential equation on scalar variables) and
the conservation of momentum equations (three partial differential equations on scalar vari-
ables) were derived earlier in this chapter. Then constitutive equations were studied to
relate the viscous stress tensor to the rate of strain tensor. We substituted these constitu-
tive relations into the momentum equations for Newtonian fluids with constant density and
viscosity and formulated four equations containing the four unknown dependent variables:
P,ux,uy,uz and four independent variables x,y,z and t. For non-Newtonian fluids, or, for
Newtonian fluids with non-constant density and/or viscosity, the corresponding constitutive
relations must be used together with the general momentum equations, Equations (3.34)-
(3.36), instead of using Equations (3.55)-(3.57). The constitutive relations for some of the
non-Newtonian fluids will be studied in the next chapter. However, before we can solve a
fluid flow problem, we need the same number of variables and equations and a sufficient
number of boundary conditions to pose a problem to obtain a unique solution.

In general, there are two types of boundary conditions: kinematic and dynamic. Kinematic
and dynamic boundary conditions deal with the velocity and stress fields, respectively.
Considering the physical contact of the fluid at the boundary, boundary conditions can
be further divided into five groups [3]:
1. Liquid-solid interface (contact at solid surface),
2. Liquid-liquid interface,
3. Liquid-vapor interface,
4. Free surface, and
5. Specified inlet and exit boundary conditions.

At the liquid-solid interfaces, the relative velocity of a viscous fluid with respect to the
solid boundary is assumed to be zero. That is, U = Usoii<j. This is known as the no-
slip condition. Although this assumption is not always correct, i.e., fluid may slip on the
solid surface, the idea of a no-slip approximation is supported by many experiments in the
literature [3].
Some examples of fluid flow problems with "Liquid-solid interface" type boundary con-
ditions are shown in Figure 3.9. In all four problems, it was assumed that the fluid domain
in the z direction is so long that there is no variation in the z direction. In (a) and (b), a
fluid is bounded by two infinitely long parallel plates. The lower plate is stationary, but the
upper one moves horizontally in the x direction. Due to the disturbance from the moving
upper plate, there will be fluid flow. The upper plate is pulled with a constant speed V in
(a). In (b), the pulling force is specified instead of the speed.
(a) (b) Pulling force (per unit
Pulling speed plate surface area)
Moving plate % Moving plate ; 7
////////////// Mr*>F
\
Kinematic b.c.: ux = V, Dynamic b.c.: lxy=r
uy=0 Kinematic b.c.: «,. =0
Fluid Fluid
Kinematic b.c.: ux = 0, / Kinematic b.c.: ux=0,

uy=Q Uy=0
y. Fixed plate
Torque applied on outer

cylinder (per unit cylinder
6 Angular speed surface area)
of outer cylinder
Dynamic b.c.:
Kinematic b.c.:
«, =0, Kinematic b.c.:
ua=QRn K, =0
Kinematic b.c.: Kinematic b.c.:

«r=0, « r =0,
"e=0 U = 0
Figure 3.9: Four example situations for different boundary conditions, (a) Kinematic bound-
ary conditions at the upper and lower boundaries for fluid flow within a rectangular channel,
(b) The same as in (a), except that the pulling force F on the plate is specified instead
of the speed. So, this boundary condition on the upper boundary of (b) is dynamic, (c)
Kinematic boundary conditions on the outer and inner cylinder boundaries of fluid flow
within a concentric domain, (d) The same as in (c), except that the torque T applied to
the outer cylinder is specified instead of the angular speed. So, this boundary condition on
the outer boundary of (d) is dynamic.
The no-slip condition can be directly applied in (a). If the plates are impermeable (non-
porous), then there is no fluid flow in the normal directions on the plates, which can be
written as U • n = uy = 0 at y = 0 and y = h, where U is the fluid velocity vector, and n

is the normal vector on the plate. The tangential velocity component, ux — V at y = h,
and ux = 0 at y — 0, considering the no-slip condition. These are kinematic boundary
conditions since they only involve the velocity field.
The boundary condition on the upper plate in (b) is a dynamic condition. The pulling
force applied on the plate is specified. This force can be related to the shear stress, which
is usually needed in the dynamic boundary condition. In fact, this problem is a one-
dimensional problem, i.e., velocity vector and stress tensor are functions of only y, not x.
Hence, rxy is constant at y = h. The dynamic boundary condition is then rxy = F/A, where
A is the area of the plate.
In (c) and (d), the fluid domain is a concentric gap between a fixed inner cylinder and
a rotating outer cylinder. Since the inner cylinder is fixed, (i.e., has a zero velocity vector),
the fluid will also have the same velocity vector due to the no-slip condition. In (c), the
angular velocity of the outer cylinder is specified as 9. Hence, the fluid will also have the
same velocity, ug = 0Ro.
In (d), the external torque applied to the outer cylinder is specified as T. To relate the
T to the shear stress rre, one can show that as rre is constant over the surface area li^R^L
as this problem is also one-dimensional; the velocity and stress fields are functions of r only,
and hence TTB is constant at r = RQ. The corresponding dynamic boundary condition is
then Trg = T/2irRQL. Here, L is the length of the cylinders in the z direction.
Consider the two immiscible fluids A and B within a rectangular channel as shown in
Figure 3.10. The kinematic boundary conditions on the upper and lower plates are UXQ = V
at y = JiA + hs, and uxj\ — 0 at y — 0, respectively. We need two more boundary conditions
at the liquid-liquid interface in order to uniquely solve this problem. For viscous fluids, the
velocities are assumed to be continuous at their interface. So, U^ = UB in vectorial form,
or UXA — UXB and uyA — %B in scalar form at y = HA- Considering the dynamical
interactions of adjacent control volumes of fluids A and B, the viscous shear stress rxy
must be continous across the interface. Hence, Txy^ = rxys which can also be written as
Pulling speed
; Moving plate
Kinematic b.c.: M,n = V,
Fluid B
Kinematic b.c.; Ux^—Uxgt Dynamic b.c.: txyA =

u u
yA ~ yB
Fluid A
Kinematic b.c,: u^ — 0,
/////////^^^^//////
«,*=o
//, Fixed plate
Figure 3.10: Boundary condition at a liquid-liquid interface.

3.5.2 Solution Procedure
In this chapter, so far we have studied the necessary tools to solve isothermal flow problems.
These tools are conservation equations for mass and momentum which are mathematical
models of physical laws, and constitutive equations to relate the stress tensor to the fluid
deformation in terms of rate of strain tensor. These equations are valid everywhere in the
fluid domain. Different boundary conditions and assumptions made in different fluid flow
problems are the reasons why different solutions are obtained in different situations. We
can generalize the solution procedure as follows:
1. Choose coordinate system and verify parameters,

2. State any physical conditions (such as symmetry about a boundary, one-dimensionality,
two-dimensionality, steady state) in mathematical terms,
3. Write governing equations (conservation of mass, momentum and constitutive equa-
tions) and neglect terms that are zero or negligible compared to other terms,
4. Write the boundary conditions,
5. Solve for pressures, velocities and stresses, and
6. Calculate other quantities of interest such as flow rate, forces, etc., by integrating
velocities, pressure or stresses.
Below we will solve several fluid flow problems by following this solution procedure assuming
Newtonian constitutive law, and then in the following chapters, the procedure will be applied
to the solution of different composite manufacturing processes.
Example 3.5: Plane Couette Flow

Couette flow, named after M. F. A. Couette, is flow in a rectangular channel induced by
a moving upper boundary at a constant speed V. The geometry and the corresponding
boundary conditions (Figure 3.9(a)) were stated in the previous section. In reality, the
length of the channel in the x direction is never infinite, despite the assumption made.
However, we will assume that the channel is long enough that the end effects are negligible
so a fully developed steady-state velocity profile is created. Now, let's demonstrate the
solution procedure for this problem.
Solution
Step 1: Cartesian coordinate system is chosen and attached at a convenient location as
shown in Figure 3.9(a). The parameters are the speed of plate V, height of the channel h,
and viscosity of the fluid n.
Step 2: As we stated in the previous section, we assume that the problem is two-dimensional
in the xy plane, i.e., the z component of velocity uz is zero, and the variables do not vary
in the z direction (d(}/dz = 0). We also assume that the fluid is Newtonian.
Step 3: The governing differential equations are the conservation of mass and the conser-
vation of momentum equations, Equations (3.10) and (3.55). We will consider steady-state
flow (d(}/dt = 0 for any variable). Note that steady state doesn't mean D()/Dt — 0 for a

variable since it is the substantial derivative following a fluid particle. Also, a fully devel-
oped velocity field in the x direction will be considered in the channel, hence <9( )/dx = 0.
Step 4: The boundary conditions have already been shown in Figure 3.9(a) as ux = V,
uy = 0 at y = h, and ux = 0, uy — 0 at y = 0.
Step 5: For a steady state with no-sink effects, the conservation equation can be simplified
to
dx dy dz
where uz — 0 due to 2-D assumption, and dux/dx = 0 due to the fully developed velocity
assumption. Then, Equation (3.60) reduces to duy/dy = 0. Integration of duy/dy = 0
yields that uy = uy(x), i.e., uy is not a function of y, but can be a function of x. The
boundary conditions show that uy — 0 for all x values, and hence uy must be zero within
the entire domain as well since it is not a function of y either. The only non-zero velocity
component is then ux which is a function of y only. How do we find ux(y)l We use the
momentum equation in the x direction:
(dux dux dux dux\ dP \drxx dryx drzx\
P -^r + ux — h uyy — I- uz —— = - — + — h -r h -^— + rBx (3.61)
\ dt dx dy dz J dx [ dx dy dz J
If the fluid is a Newtonian fluid, needed components of the stress tensor are equal to
dUx
T
xx = o^W = n0 /-) co \
(3.6za)
dx
T
idu x duy\ dux
yx = M -«- + ^ = ^— (3.62b)
V dy dx J dy
rzx = ^(^ + ~} = 0 . (3.62c)
\ dz dx J
Hence,
d ,„, d (dun
^ ' dy \ dy
(3.63)
uy-
After eliminating the terms which are zero and considering that F# — — pgk, hence FBX = 0,
Equation (3.61) reduces to
The momentum equations in the y and z direction reveal that ^ and ^ are equal to zero
if one ignores gravitational effects.
As the fluid pressure is the same at the inlet and exit and there is no pressure build-up
inside the geometry, dP/dx = 0 as well, which reduces Equation (3.64) to

Integrating Equation (3.65) with respect to y twice yields ux(y] = c\ + c^y where c\ and c<i
are constants to be determined by using the boundary conditions. u x (0) — 0 requires that
ci — 0, and ux(h) = V requires that c-2 — V/h, so
V
(3.66)
which is a linear velocity profile as shown in Figure 3.11.

Pulling speed
Figure 3.11: Velocity profile in a rectangular channel induced by a moving plate at constant
velocity V.
Step 6: The viscous shear stress Txy on fluid at any location is rxy = /j,[(dux/dy) +
(duy/dx)} = fJ,(V/h + 0) = [j,V/h which is a constant. The flow rate across a vertical
cross section of the channel is Q — /0 aux(y)dy — J0 a(Vy/h)dy — aVh/2 where a is the
dimension of the channel in the z direction. The flow rate is linearly proportional to V and
h. The shear stress rxy, which is equal to the required pulling force per unit plate area, is
linearly proportional to V, but inversely proportional to h. •
Example 3.6: Combined Couette-Poiseuille Flow

Couette flow was studied in the previous example. Another flow problem that was studied
by and named after Poiseuille, has the same geometry as in the Couette problem, except
that both plates are fixed, but there is a pressure drop applied across the two ends of
the channel. We will introduce "Combined Couette-Poiseuille Flow" in this example. The
problem geometry and the boundary conditions are shown in Figure 3.12. The fluid pressure
is P = Pi at x = 0 and P = PP at x = L.
Solution
Step 1: Cartesian coordinate system is chosen as shown in Figure 3.12. The parameters
are V, h, L, /j,, Pi, Pe.
Step 2: Two-dimensional steady-state flow in xy plane is considered with a Newtonian

fluid. The end effects are neglected.
Step 3: The governing differential equations are Equations (3.10), (3.55), and (3.56) with

/ Pullina soeed
/// Movinq plate '/""""////"'"""""""""/"'"//""/"
\Kinematic b.c.: ux = V ,
Fluid
Dynamic b.c.:/ Dynamic b.c.:
Kinematic b.c.: ux — 0,
Figure 3.12: Combined Couette-Poiseuille flow.
the assumptions of a fully developed velocity field in the channel.
Step 4: The boundary conditions are shown in Figure 3.12 as ux = V, uy = 0 at y = h,

ux = 0, uy = 0 at y = 0, P = Pi along x — 0, and P = Pe at x — L.
Step 5: The solution is exactly the same as in Step 5 of Example 3.1 up to the momentum
equation in the x direction:
dP_
(3.67)
dx
In this case, dP/dx ^ 0 here as specified by the boundary conditions. The momentum
equation in the y direction, Equation (3.56) yields
0 = - (3.68)
dy
neglecting the body force. Thus P is a function of x only. ux was found to be a function
of y only from the continuity equation (see Example 3.1). The left hand side of Equation
(3.67) is a function of x only, and the right hand side is a function of y only. In order to hold
this equality for all x and y within the fluid domain, both sides must be constants. Hence,
dP/dx = c, which means that the pressure changes linearly in the x direction. Using the
dynamic boundary conditions at both ends of the channel, dP/dx = (Pe — Pi)/L. Equation
(3.67) reduces to
pe _ pi
2 (3.69)
dy p,L
Integrating Equation (3.69) twice with respect to y yields ux(y) = [(Pe —
ciy + c?. Boundary condition n x (0) = 0 yields c% — 0. c\ is found by using the last boundary
condition, ux(h) = V. Hence,
/ \
= G, i, / 9
" \ '
(3.70)
pressure driven flow drag flow

It is very interesting that the velocity profile given by Equation (3.70) is the superposition of
the two u x (y)'s: the first one is induced by a pressure gradient without a moving boundary
plate (Poiseuille flow), and the second one is induced by drag flow induced by a moving
plate (Couette flow) as we studied in Example 3.1. The individual and superposed velocity
profiles for two typical cases, where Pe < P0, and Pe > P0, are shown in Figure 3.13.
uCouette(y}+ Poiseuille (
ifPe<P0
Figure 3.13: Velocity profiles for combined Couette-Poiseuille flow.
Step 6: What is the flow rate in this flow? Flow rate can be calculated as Q = /0 ux(y) a dy,
where a is the width of the channel in z direction. For this flow, it will be
rh n V 1 , (Pi-Pe)ah3 ahV
(3.71)
Q = Jo I\- 2fj,L y
l^ \ ady
- 12ML +
^T'
Example 3.7: Flow in Concentric Cylinders due to Longitudinally Moving Inner

Cylinder
Consider an incompressible fluid between inner and outer cylinders with radii Ri and R0,
respectively, as shown in Figure 3.14. The inner cylinder is pulled along the z direction with

a constant velocity V. The fluid is assumed to be Newtonian with viscosity ^. Assume that
the cylinders are very long in the z direction, and consider steady-state, fully developed
flow. Find the velocity field, viscous stress tensor, flow rate and required pulling force per
unit length.
Side view End view
Fluid
Pulling speed
Moving cylinder
Kinematic b.c.:'
u = 0, UQ = 0, M = 0 Kinematic b.c.:
ur = 0, UQ = 0, u z = V
Figure 3.14: Incompressible fluid flow between two concentric cylinders induced by the
motion of inner cylinder in the z direction [62].
Solution
Step 1: Cylindrical coordinate system is chosen as shown in Figure 3.14. The relevant
parameters are Ri, R0, V, and \JL.
Step 2: Steady state (d()/dt = 0), fully developed (no end effects, d\J/dz = 0), and
incompressible flow (Dp/Dt — 0, hence V • U = 0) is considered in this problem. Due
to symmetry, UQ = 0 and d()/d9 = 0. Also, no body force (including gravity) will be
considered here.
Step 3: Conservation of mass equation in the cylindrical coordinates is

dp 1 <9 . . \ d . U . 9, u =
1 (prur) H (P 0) ~l \P z) 0- (3.72)
£?t T1 C^T1 7" 90 (?2
The conservation of momentum equations in the r direction:
dur dur
I
Ug dur
1. 1_
Ua
V, I
~^ I ^v/i
~~dt or r ac/ r r dz
I d . d
- -^7.(rr8r) + ^-(
7T
dr r dff dz
and the conservation of momentum equations in the z direction:
duz duz UQ duz duz
~^r
ot
P\u HZ"
r 06 ~7S~
az

Step 4: No-slip boundary conditions are
ur = 0, uz = V &t r = Ri (3.75)
ur = 0, uz = Q at r = fl0. (3.76)
Step 5: After eliminating the terms that are equal to zero, Equation (3.72) reduces to
A ( r « r ) = 0. .(3-77)
Integrating Equation (3.77) with respect to r yields
rUr = f(z) (3.78)
as rur is not a function of r, but could be a function of z. But, as flow is fully developed
flow (so dur/dz — 0), f ( z ) has to be equal to a constant; hence,
rur = ci. (3.79)
Applying boundary condition either (3.75) or (3.76), c\ = 0, hence ur = 0. The only non-
zero velocity component is then uz. For an incompressible Newtonian fluid, one can now
find the components of the stress tensor as follows:
f/1 1
Trr = 2n-—^ = 0 (3.80a)
or
O
<3-80b>
= 0 (3.80c)
d (u \ I du ]
r — —e + - —r-r =0 (3.80d)
or \ r J r oU \
dus 1 du
or a
The only non-zero stress component is rrz, and its derivative with respect to z is also zero.
Hence, one can simplify the momentum Equations 3.73 and 3.74 to
(3.82)

Equation (3.81) implies that P ^ P(r). There is no external pressure drop applied in the
z direction either; hence P =£ P ( z ) . Equation (3.82) reduces to
duz
— =0. (3.83)
or
Integrating Equation (3.83) with respect to r yields
duz
^~ (3.84)
or
and further integration results in
(3.85)
Boundary conditions (3.75) and (3.76) can be applied which allows us to find c\ and c^'.
uz(Ri) = GI InRi + C2 = V, (3.86)

u
z(Ro) = c C
l hl-Ro + 2 = 0. (3.87)
Subtraction of Equation (3.87) from Equation (3.86) yields c\ — V/\n(Ri/R0), and c% —

— GI ln.R0. Substitution of c\ and c% in Equation 3.85 gives the velocity profile
ln(r/R0)
(3.1
This velocity profile is sketched in Figure 3.15.
Pulling speed
Moving cylinder
Fluid
y///////////////////
• Stationary cylinder^
Figure 3.15: Velocity profile due to inner cylinder moving with speed V in the z direction.
Step 6: The flow rate is
Q = I °uz(r)2Trrdr
JRi
27TV n (3.89)
l
°

The only non-zero stress component rZT is calculated as follows:
' dur duz
— A "a
dz
dr [ In
(3.90)
The external force per unit z length, Fi, required to pull the cylinder to maintain its speed
at velocity V is calculated as
= AT,.
r=Ri
In (Ri/Ro) r=Ri
(3.91)
In
Note that F0 = (2vrRO)TZT\T=R O = 2Tr/j,VR%/ln (Ri/R0) acts on the stationary outer cylinder,
which is greater than Fj. •
3.6 Conservation of Energy

In the previous sections, the mathematical modeling was based on the assumption of isother-
mal flow. For isothermal flows, all we need are conservation equations of mass and momen-
tum, constitutive equations to relate the stress tensor to fluid deformation, and a set of
boundary conditions. In manufacturing, as one has to heat and cool the resin, the process
is hardly isothermal although some of the manufacturing operations may be. The temper-
ature will play a very significant role due to the sensitivity of the resin viscosity to the
temperature and exothermic reactions in case of thermoset resins.
Hence, for nonisothermal cases, there is a need for an additional equation in order to
solve for the flow parameters. Considering the physical law of the conservation of energy
within any control volume, this equation will be derived here. Although a relatively detailed
derivation will be presented here, readers are referred to [63] since the derivation requires
some thermodynamics knowledge.
The momentum equation was given in Equation (3.37) for any type of fluid flow. Al-
though the next step may not be obvious to some readers at the moment, the dot product
of Equation (3.37) with velocity U results in:
U P (3.92)
Dt
Since (D/Dt)(A B) =B (DA/Dt) + A • (DB/Dt) for any two vectors A and B, one can
write (D/Dt)(U-U) = 2U-(DV/Dt). Hence, the first term in Equation (3.92) can be
rewritten as U • \p(DV/Dt)] = pD(±U -U)/Dt = pD(±\U\2)/Dt where i U - U = ^ U 2 is
the kinetic energy of fluid particles per unit mass. Hence, Equation (3.92) can be recast as
D /I
P U - -U-(VP) (V-r) (3.93)
Dt \2

which is called the conservation of mechanical energy equation. Recall that — VP + V • r =
V • a is the surface force per unit volume due to the total stresses, and FB is the body force
per unit volume. Also recall from the introduction to physics and dynamics courses that
U • F is the rate of work done by any force F on the material (fluid particles here) moving
with the velocity U. Hence, one can physically describe the conservation of mechanical
energy equation (Equation (3.93)) as follows: the rate of increase (accumulation) of kinetic
energy per unit volume at any point in the fluid domain is equal to the summation of the
rate of work done per unit volume by the forces due to the fluid stresses and body forces.
Consider the control volume shown in Figure 3.2 which is fixed in space. One can write
the energy balance for this control volume as follows:
Rate of increase \ / Inflow flux \ / T n n \ i Rate of energy
ott internal
• 4. i andj — I off -internal
4. i andj +, / Inflow
P,
flux
, \ +. I increase
. , to
due .
, . ,. , . ,. \ of heat I
kinetic energy / \ kinetic energy / \ ' y total stress a
( Rate of energy
. &y
increase due to
body forces FB J
\
+
\
/ „
^
,,
..
generation
'
\
I Rate of energy \
/
,_ ...
(3.94)
The individual terms can be expressed mathematically as follows:

Rate of increase \ j r / i \ r ft f 1 \
of internal and = — / ( pE + p-|Uj 2 ) dV.= / — ( pE + - J U | 2 ) dV (3.95)
i • ,• I at Jv \ 2 J JV ut \ 1 )
kinetic energy /
where E is the internal energy of fluid particles per unit mass. The total time derivative
was moved inside the integral as a partial time derivative, and the additional terms were
eliminated using the Leibniz rule since V is fixed. The first term on the right-hand side of
Equation 3.94 can be mathematically represented as
Inflow flux \ , - .
of internal and = / — f pE + p— |U| J n - U c L 4 (3.96)
kinetic energy I
The minus sign is due to the fact that n is the outward normal vector, and — n-UcL4 is
the infinitesimal inflow velocity flux of fluid particles through the infinitesimal surface area
dA. The second term on the right-hand side of Equation 3.94 can be expressed as
Inflow flux \i •f .. .,_ _ _
= /I -n-qdA
-n-qdA (3.97)N
of heat '
) Js ' -
where q is the heat flux vector. The third term on the RHS of Equation 3.94 will be
^gy \
Rate of energy ,
increase due . to ] = / n • (a • U)
U) dA (3.98)
JS
total stress a J
where a is the total stress tensor. The energy contribution due to the body force term will
be
Rate of energy
increase due to | = / U • FB dF (3.99)
body forces F^

and finally, the last contribution will be
Rate of energy
= / RdV (3.100)
generation Jv
where R is the rate of energy generation per unit volume due to internal energy sources,
(such as chemical and nuclear reactions). Equation (3.94) can be assembled in mathematical
form as follows:
= -f - fn-
Js Js
n-(a-\J)dA+ / U-FBdV + / RdV. (3.101)
s Jv Jv
Applying Gauss' divergence theorem (Equation (3.5)), the first three surface integrals on
the right hand side of Equation (3.101) are converted to volume integrals, and Equation
(3.101) becomes
+V • q + V • (<r • U) + U • FB + R\dV
(3.102)
Since the control volume V is arbitrary, not only the integral but actually the integrand
must be zero:
1
I (~) I / \ 0
). (3.103)
The first two terms in Equation (3.103) can be rewritten as

(3.104)
In the third equality line of Equation (3.104), ^ _)_ ^y . u was replaced by — U • Vp — s by
using the conservation equation (Equation (3.8)). After substituting Equation (3.104) into
Equation (3.103), it reduces to
r V-(vU)~l3-FB-R = 0. (3.105)
Dt V 2' ') \ 2
Equation (3.105) is expanded by writing the total stress tensor as a = —PI + r
(3.106)
V • (r • U) that appears in Equation (3.106) can be expanded as T : (VU) + U • (V • T). The
double dot product between two tensors, say A and B, is denned as A : B = AijBji =
AnBu + AI^BII + Ais-Bai + 421-612 + ^22-622 + ^23-B32 + A3iB13 + A32B23 + ^33-633, which
is a scalar. Equation (3.106) then reduces to
-r : (VU) - U - (V • r) - U • FB - R = 0. (3.107)
The second term on the left-hand side of Equation (3.107) is rewritten by substituting the
expansion from Equation (3.93). Thus, Equation (3.107) expands to the form
DE_ U F 1
Dt
+ V • q + V • (PU) - T : (VU) - U • (V • r)
-U-F j B --R = 0. (3.108)
Using the fact that U • (VP) - V • (PU) = -PV • U, and simplifying Equation (3.108)
results in
DE
= - y - q - P V - U + r : (VU) + s (E +-\U\2} + R. (3.109)
L)t \ 2
This is the conservation of energy equation, but it is not very useful, since we cannot
evaluate the first term, DE/Dt directly.
The internal energy E will be written by using thermodynamic relations, and then
DE/Dt will be substituted into Equation (3.109) to obtain the final form of the conservation
of energy equation.
One can use the thermodynamics relation H = E + P/p in order to write the internal
energy E in terms of enthalpy H. Then DE/Dt is equal to
— - —
Dt ~ Tn

DH 1 DP
Dt p Dt
DH 1 DP
(3.110)
~Dt ~p~Dt
The conservation of mass equation was used on the second line of Equation (3.110) to
replace Dp/Dt by —pV • U in the absence of sink term s. Hence, Equation (3.109) reduces
to
DH
, _ = -V-q-PV-U- (VU) + (3.111)
p Dt p '
Canceling the two —PV • U terms, the equation simplifies to
(3.112)
' Dt Dt
Considering that H is a function of P and T,
dH
dH = dT (3.113)
dP T
and
DH dH DP OH DT
Dt dP TDt dT pDt
8H DP DT
(3.114)
~dP m~Di~I-VD~t
where cp (= dH/d'T\p) is the specific heat evaluated at constant pressure. After substituting
Equation (3.114), Equation (3.112) takes the following form:
dH DP DT DP
P pcp = - V - q + r : (VU) + (3.115)
dP Dt Dt
Also, expanding the substantial derivative DT/Dt as dT/dt + U • VT, Equation (3.115) can
be rewritten as
dT_ DP
} (3.116)
~dt ~Dt'
This is called the conservation of energy equation. In many processes, the last term
(l ~ P^p T) ^j is very small, so it is neglected, which then further simplifies the con-
servation of energy equation to
= -V-q + r:(VU) + ^ (3.117)

convection conduction viscous dissipation energy generation
transient
The physical meaning of individual terms in Equation (3.117) is written underneath them.
Note that the summation of the two terms on the left-hand side of Equation (3.117) is
simply pcpDT/Dt. R is usually due to chemical reactions of the resin and/or microwave
induction heating of the polymer.

Example 3.8: An Alternative Derivation of Energy Equation
In this section, the derivation of the conservation of energy equation was carried out by
expressing the internal energy E in terms of enthalpy H as E — H — P/p. Alternatively,
one could express the internal energy E by using another thermodynamic relation and derive
the energy equation in terms of different variables. In this example, we ask to you to use
the infinitesimal internal energy given by
= -Pdv + TdS (3.118)
in the derivation of energy equation. Here v = l/p is the volume of fluid per unit mass,
and S is the entropy of fluid per unit mass.
Solution
As E is a function of v and T, dE can also be written as
dE dE
dE = dv dT. (3.119)
dv T
dT
Hence, the total time derivative of internal energy is equal to
DE dE Dv dE DT
+
~Dt dv T
~Dt ~dT V 7)t
( dS \ Dv dE DT
— 1 p _j_ jP
dv J 1 Dt _j_ (3.120)
V T ^ dT ~Dt'
Now Dv/Dt can be written explicitly as
Dv
Dt Dt
I Dp
(3.121)
where Dp/Dt was replaced by — pV • U — s using the conservation of mass equation. For
brevity, no sink case (s = 0) will be considered from now on, and the substitution of
Equation (3.121) into Equation (3.120) yields
v U-
OE DT
Dt T
^~dT V ~Dt
DT
V UH v (3.122)
P 9T n
~° Dt

where cv •(= dE/dT\v) is the specific heat evaluated at constant volume, and |^\T = §y v —
|^ p relation (Maxwell equation) was used to replace |^ T. After substituting Equation
(3.122), Equation (3.109) reduces to
DT
- V-\J + cv—-| = - V - q - P V - U + r : (VU) + P. (3.123)
LJ t
—PV • U on the left-hand side cancels —PV • U on the right-hand side, and expanding the
substantial derivative as DT/Dt = dT/dt + U • VT, Equation (3.123) reduces to
dT OP
— + pcv\J.VT = - V - q + r : ( V U ) - T — V-U+R. (3.124)
This is the conservation of energy equation, but it is seldom used due to the need for cal-
culation of the underlined term. For incompressible fluids, we do recover Equation (3.117).
3.6.1 Heat Flux-Temperature Gradient Relationship

Previously, a constitutive equation was studied to relate the stress tensor to the strain
rate tensor, since the stress tensor appears within the momentum equations. In the energy
equation, the heat flux q appears. In this section, we will study another constitutive
equation to relate the heat flux to the temperature field, q is the conductive flux through
the polymeric liquid and the reinforcing fibers. In general, heat can be transmitted in terms
of conduction, convection and radiation. However, here q doesn't include the convection
part, and in many composite manufacturing processes, the radiation term is negligible. For
most materials (including many fluids and solids), the heat flux is linearly proportional to
the temperature gradient and was first proposed by Fourier [64]
q=-k-VT (3.125)
where k is the thermal conductivity tensor of the composite material. The minus sign is
because heat is transmitted from hotter to colder locations. Hence, the energy equation can
be rewritten as
dT
pcp— + pcpU-VT = V-(k-VT)+T:(VU) + fl. (3.126)
For an isotropic thermal conductivity which is constant within the entire domain, k • VT
reduces to fcVT where k is the scalar thermal conductivity. Hence, the energy equation
further simplifies to
dT
pcp— + pcpU-VT = fcV2T + T : (VU) + R (3.127)
for materials with constant (uniform) isotropic thermal conductivity. However, composites
may have nonisotropic thermal conductivity especially when carbon fabric is used, in which

case the conduction term is expanded into
dT
V - ( k - V T ) = — (fc n —
d dT . dT , <9T
hK + k23 -Z-
9X2 8x2
d dT dT dT
-— (3.128)
0x3
Example 3.9: Heat Transfer in a Material with Nonisotropic Thermal Conduc-

tivity
Consider a composite of thickness h having thermal conductivities of k(, k'2 and k'3 along the
principal directions of the fibers and perpendicular to the fiber direction. This composite has
fibers at an angle 9 with respect to the large faces of the composite as shown in Figure 3.16.
The composite is held between two highly conductive materials maintained at temperatures
TU and TL as shown in Figure 3.16.
Figure 3.16: A composite section being heated by two isothermal surfaces at uniform tem-
peratures TU and TL. The fiber direction in the composite is at angle 0 with the vertical
direction x\ as shown.
How will you calculate the heat flux flowing normal to the large faces of the plate? Will
the heat flux vector be parallel to the temperature gradient VT as is the case for isotropic
materials?

Solution
Note that as h <C L, W, one can assume isothermal surfaces parallel to the large faces of
the composite. This is usually true everywhere except near the edges. If the plate thickness
h is small compared to L and W, edge effects are negligible. This VT will be perpendicular
to the lateral faces. Hence ^- = 0 and jj-j- = 0.
For an anisotropic composite, one could write the relationship between the heat flux
and temperature gradients as follows:
- k — k — k — (3129)
dxi dx2 dx3
=
dT dT dT
— <?2 ™21 r K22 r K23 lo.loU)
5xi dx2 dx3
9T
— k —
dxi dx2 °~
Now as j^ = 0 and ^ = 0, Equations (3.129)-(3.131) reduce to
(3.132)
dT
= ^- (3.133)
dT
= k31— (3.134)
ox i
where qi, q%, and 53 are the components of the heat flux vector q = qii + q%j + gsk. Thus
q\ will be heat flux in the i direction. Also,
dT TU-TL
-- (3.135)
and /en will be related to k ( , k^ and fc3 as follows:
jfcn = l*k{ + /i4 + Z|fc^. (3.136)

where fc^, fcân(i ^3 are the principal conductivities and li, 1% and /3 are direction cosines
of the 1-axis relative to the principal axes 1', 2' and 3'. For this case, it simplifies to
kn = cos02k{ + sm92k'2. Note that as q has non-zero q^ and g3, it will not be along the
same direction as VT. •
3.6.2 Thermal Boundary Conditions

In general, three types of boundary conditions exist when one is interested in calculating
the temperature from the conservation of energy equation. They are:
1. Boundary temperature T is prescribed.
2. The external heat flux, q — —kdT/dn is prescribed, where n is the outward normal
direction on the boundary.

3. Convection heat transfer coefficient h is prescribed. The related boundary condition
is q = —kdT/dn = /i(Too — T), where T^ is the ambient temperature adjacent to the
boundary, since the convected heat flux is equal to the conducted heat flux.
Some examples of thermal boundary conditions are shown in Figure 3.17.
Convective heat transfer:
h and 7^ are prescribed
T = Tw\ is prescribed
-/- T = TW2 is prescribed

T(x,y,z,t)
External heat flux, q

is prescribed
' T = rw3 is prescribed
,dT
q=
~kTn
Figure 3.17: Examples of three types of thermal boundary conditions.
Example 3.10: Temperature Distribution Within Concentric Cylinders due to

Different Wall Temperatures
Consider an incompressible resin between two concentric cylinders with radii Ri and R0, as
shown in Figure 3.18(a). Assume that the gap between the two cylinders is much smaller
than the radii, (R0 — Ri) <C Ri- The outer cylinder is rotated around the z axis with a
constant angular speed of u>. The fluid is assumed to be Newtonian, and the viscosity /j,
doesn't change significantly with temperature, /n ^ f^(T). Assume that the cylinders are
very long in the z direction, and consider steady-state flow. Find the resin temperature
distribution if the inner and outer cylinder walls are kept at constant temperatures Ti and
TO, respectively. Also find the resultant heat flux through the system.
Solution
Steps 1-5: Although the cylindrical coordinate system seems to be the logical choice here,
the Cartesian coordinate system is preferred because of its simplicity. The justification for
this choice is that since (R0 — Ri) <C Ri, the velocity component in the radial direction ur
is expected to be much smaller than the one in the tangential 0 direction ug. Hence the
flow is assumed to be only in the 0 direction. With a coordinate transformation such as

(b)
Moving plate
u =
Fluid
*y, Fixed plate
uy=Q
Figure 3.18: (a) Geometry for two concentric cylinders and boundary conditions. The outer
cylinder rotates while the inner one is stationary, (b) The geometry can be converted into
one-dimensional planar Couette flow if RQ — Ri <C RI-
x = Ri6 and y = r — Ri, the problem is simplified to one-dimensional in the x direction.

The simplified problem geometry and the corresponding boundary conditions are shown in
Figure 3.18(b). This problem is exactly the same as the one studied in Example 3.3, except
that this one is nonisothermal due to the different thermal boundary conditions applied at
y — 0 and y — R0 — Ri. However, since fj, ^ /u(T), the velocity distribution solutions will
not change, so the result can be taken directly from Example 3.3:
V
(3.137)
since the equivalent V = R0u) and h — R0 — Ri.

Assuming an isotropic thermal conductivity k for the resin, the energy equation (Equa-
tion (3.127)) is written as
dT
= fcV2T + T : (VU) + R. (3.138)
Here -^- — 0 considering steady state, and R — 0 since there is no heat generation within
the resin. The only non-zero velocity component is ux as found above. Considering that
the resin should have the same properties at every 9 (hence x} value, the temperature T is
expected to be a function of y only. Hence, after dropping the zero terms, Equation (3.138)
reduces to
dT dT <9T
pcp — — = k + r : (VU)
dy dz dx2 ' dy* dz2
f dT d2T
pcp \ux(0) + (0) — + r : (VU)

0 = k—2- + r : ( V U ) (3.139)
The only non-zero terms in the viscous stress tensor are rxy and Tyx:
d d
^ = ryx = J^ + ^}=J^^
\ dy dx J + ^l}=^-.
\R0-Ri dxj R0-Ri (3.140)
Hence the viscous dissipation term can be calculated as

/,-,TTs 9ux duv
r:(VU ) = rxy + ryx
M
^k) (0)
R0to
rio — rii J \ ILO — Jn
= MT^V =A. (3.141)
The constant A is the energy generated within the fluid due to the viscous dissipation.
By substituting T : (VU) from Equation (3.141) and replacing d2T/dy2 with d2T/dy2
as T is only a function of y, Equation (3.139) reduces to
f - £ -•
By using the nondimensionalized variables, T = T/(T0 — Ti) = T/AT and y = y/(R0 — Ri) =
y/h, Equation (3.142) takes the following form:
/AT\2
B
- (lF ) - D (3 143)
'
where D = f (:§^)2 = f(M') 2 - Integrating Equation (3.143) with respect to y twice yields
T (y) - Df + erf + c2 (3.144)
where the constants c\ and c% are to be determined by using the thermal boundary condi-
tions. Boundary condition T(0) = T;/AT results in c^ = Tj/AT, and the other boundary
condition T(l) = T0/AT results in c\ = 1 — D. Hence, the resin temperature distribution
is given by
(3.145)
For T0 > TJ case, a typical nondimensional temperature profile is shown in Figure 3.19
underneath the velocity profile. The nonlinearity is due to heat generation induced by
viscous dissipation. Step 6: Conductive heat flux in the x and z directions is zero since
the temperature doesn't change in those directions. The flux q (which is dimensional here)
through the top and bottom plates (where n — y and n — —y, respectively) are
OT _ dT _ fcAr dT
dn dy h dy

„, „, Pulling speed
- Moving plate //////////////////// T = To '//////////
y=\ ^ R m
•> = yl(R0-Ri)
x
y- Fixed plate = To-Tt
- Ti
Iv +
AT
D = ^-
Figure 3.19: Velocity and temperature profiles.
fcAT D)
(3.146)
h
-k—-k—- kAT 9T
y=0 dn dy h dy
kAT fcAT(l - D)
[20(0) + 1-D] = (3.147)
h
Note that, q
y=0 y=l
Although there is no energy source inside the fluid, it was assumed that the velocity and
temperature profiles do not change along the x direction, and the steady state was assumed,
the conductive heat flux at the two walls is not equal. This is because mechanical energy
is converted into heat due to viscous dissipation within the fluid. •
3.7 Exercises
3.7.1 Questions
1. Why does one formulate a process model?
2. What are the main ingredients needed to create a mathematical model?
3. The conservation of momentum equation can be succintly written as
ITU
P (3.148)
~Dt ~

Describe the physical significance of each term.
4. How is the rate of strain tensor calculated from the fluid velocity vector? Explain the
physical meaning of the scalar magnitude of this tensor, called the strain rate.
5. How is the vorticity tensor calculated from the fluid velocity vector? What type of
flow results if all the components of this tensor are zero?
6. When are the conservation equations of mass and momentum not sufficient to solve
flow problems? What additional equation is needed? What physical law is used to
derive that equation?
7. Explain the kinetic energy of fluid particles.
8. What is the substantial derivative of internal energy of a fluid, DE/Dt in terms of
fluid material parameters, temperature T, pressure P and velocity U?
9. What are the three types of thermal boundary conditions?
3.7.2 Problems
1. The conservation of mass equation is
?T + V • (pU) + s = 0 (3.149)
or, alternatively
— + p V - U + s = 0. (3.150)
What is the difference between dp/dt and Dp/Dt? The second term in the first
equation is V • (pU) whereas it is pV • U in the second equation. Are they equivalent?
Explain.
2. For a two-dimensional, constant density and steady state fluid flow, the velocity com-
ponents are given as ux — ax and uy = by. What is the relation between a and 6?
Can a = 26? Explain.
3. Construct numerical examples of U in which 7 and ui (i) are both zero, (ii) are both
non-zero, and (iii) one of them is zero and the other one non-zero.
4. In a plane Couette flow configuration, the fluid is bounded by two parallel plates with
a depth of h. For a Newtonian fluid with viscosity p., what are the velocity, viscous
stress tensor, and vortex tensor if the upper plate is pulled with a constant speed of V
in the positive x direction, and the lower plate is pulled with velocity V in the negative
x direction? If both plates are pulled at the same speed in the same direction, what
is the fluid velocity profile? What is the viscous stress tensor, TJJ in this case?
5. What is the required force per unit plate area in order to pull a plate in plane Couette
flow? How does the force change with the viscosity and the density of the fluid?
6. In a combined Couette-Poiseuille flow (Example 3.6), if the flow rate is Q = 0, at
which y location does ux(y] = 0? Explain the importance of your result. In this case
(Q = 0), does it mean that there is no fluid flow? Explain.

7. Repeat Example 3.10, if viscosity changes with temperature as fj, = /^>exp (—bT).
8. The three types of thermal boundary conditions for an isotropic material are (i) T =
Tw, (ii) q = -kdT/dn, and (iii) q = -kdT/dn = h^ - T). How would one write
these boundary conditions if the material was anisotropic?

Chapter 4
Constitutive Laws and Their

Characterization
4.1 Introduction
In the previous chapter, we familiarized ourselves with the physical laws needed to cre-
ate a mathematical model for any manufacturing process and tailored it for composites
processing. The important pieces needed to construct the model are
• identification of the system along with its boundaries,
• the governing equations for conservation of mass, momentum and energy,
• constitutive equations to describe the materials and their phenomenological behavior,
and
• boundary conditions to tailor the model to a specific composite manufacturing process.
We need constitutive laws because we cannot completely describe, from first principles,
some of the transport phenomena such as the nonlinear material behavior of resin, the resin
and fiber interactions and resin cure kinetics at the macro scale.
Constitutive equations are empirical relations between parameters of interest. They
endeavor to incorporate the physics observed from the experiments or studied and analyzed
at the micron and molecular level into the equations at the macro scale. They have to
be objective such that the relationship and the results do not change with the coordinate
frame. Almost all constitutive equations require the researchers to characterize constants
needed in the equation that are specific to the material and its state. For example, when
a fluid is subjected to a stress, if the stress is always directly proportional to the strain
rate the fluid undergoes, the constant of proportionality (which can be characterized by
experiments) is called viscosity. This constitutive relation is known as Newtonian law and
the fluids that exhibit this behavior are called Newtonian fluids. Constitutive equations
should not exhibit any singularity or instability that is an artifact in the processing regime
to be consistent with the physics.
Constitutive equations are necessary to describe the processing of composite materials
due to their heterogeneous nature, complex chemistry of the resin, its interaction with
fibers and fillers and simultaneous transport of mass, momentum and energy at the micro,
meso and macro levels. Also, issues that are analyzed at the micro scale, such as growth

rate of a micron-size spherulite, can be represented at the macro scale level in terms of
crystallization kinetics, by use of appropriate constitutive equations. Constitutive equations
thus endeavor to describe the global picture of the process and the relationship between
the process parameters instead of the details at the micron level, which is of little interest
to the process engineer. However, constitutive equations invariably require the researchers
to determine constants that may be functions of the material or even process conditions.
Thus, independent characterization and cataloguing of material constants for constitutive
equations can become a daunting task and slow down and undermine the modeling and
simulation of such processes.
In this chapter, our goal will be to introduce to the reader various constitutive equations
that are used to describe the material behavior, or the manufacturing process behavior. We
will also comment as to the characterization, development and availability of the empirical
constants for such constitutive equations.
4.2 Resin Viscosity

Every fluid substance offers resistance if one tries to make it deform or flow. This resistance
arises because one is trying to change the arrangement of molecules of that material in
its fluid state. This property has been termed viscosity. The dimensions of viscosity are
ML~lT~l. For units, one can use Poise (P) or Pascal-second (Pa.s). One Poise is equal to
0.1 Pa.s. The viscosity of water is one centiPoise (cP) which is one hundredth of a Poise.
Water, corn syrup, liquid metals and other short chain molecules are called Newtonian
fluids because the viscosity of such fluids can be characterized by a single value which does
not change with its shear rate. As illustrated in Figure 4.1, in general, the viscosity is a
function of pressure, temperature, degree of cure, and shear rate. If there are particles or
fibers suspended in the resin, then the fiber volume fraction and orientation of the particles
can influence the viscosity if their aspect ratio is greater than one.
Continuity Equation
Momentum Transfer
Figure 4.1: Flowchart illustrating the dependence of viscosity on temperature, cure, shear
rate, particle volume fraction and orientation. Velocity and pressure are dependent on
viscosity through the mass and momentum conservation.
Resin velocity and pressure are calculated by solving the equation of motion which
contains the viscosity. Hence the velocity and pressure are functions of viscosity.
Most thermoset resins can be treated as Newtonian, although this may not be strictly
true under high shear rates. However, their viscosity is affected by temperature and cure
kinetics. Thermoset molecules will cross-link and undergo exothermic reactions when initi-

ated by a catalyst that can be invoked by heat or chemicals. This phenomenon is known
as curing. As the thermosets cure, their viscosity increases, as one would need more force
to move a molecule that is cross-linked. Thus, constitutive equations to describe the cure
kinetics and dependence of viscosity on degree of cure are necessary for thermosets. Before
the initiation of the cure, viscosities of thermosets are usually between 100 cP and 500 cP.
Hence, most of the polymer composite processing and manufacturing methods are mod-
eled using the low Reynolds number flow assumption or creeping flow assumption, in which
one neglects the inertial force in favor of the viscous force. This argument is even stronger
when one has to process thermoplastic resins as their viscosities under quiescent state when
they are in a melt form can be as high as 10,000 P. This is primarily because at the molecu-
lar level thermoplastic resin forms a mosaic of long chained molecules all entangled together
in the quiescent liquid state [62]. As soon as one subjects them to shear, these molecules
start to align in the direction of the shear; thus they can slip over each other much more
easily as they are no longer entangled, as shown below in Figure 4.2.
(a) Quiescent state (b) Under shear
Figure 4.2: Applied shear causing the molecules to align along the flow direction.
Thus, the resistance to flow can dramatically reduce due to the change in the struc-
ture under applied shear load reducing the viscosity by orders of magnitude. Such liquids
are known as shear thinning fluids, where the viscosity decreases with shear rate. Thus
thermoplastics belong to a class of non-Newtonian fluids. Thermoplastics may also display
viscoelastic behavior due to the long chained spring like molecules; however, in composites
processing, due to the presence of the fibers and low flow rates, one can ignore the viscoelas-
tic effects [65, 66]. Usually, one checks the Deborah number (De) to gauge the importance
of viscoelasticity. De is the ratio of elastic effects to viscous effects and if De <C 1, one can
safely ignore the elastic effects of the thermoplastic polymers. This is usually true for almost
all composites manufacturing processes. As there is no cross-linking or reactions that the
thermoplastics undergo in their melt state, cure kinetics characterization for thermoplastics
is not necessary.
The viscosity of the resin also changes with temperature for both thermoplastics and
thermosets. This effect is more significant for thermoplastics. The viscosity will usually
reduce by one to two orders of magnitude as the temperature of the material increases from
the melt temperature to a few degrees higher than the melt temperature. This is primarily
due to reduction in the resistance to flow as the molecules at high temperature can move
much more freely. Molecular dynamic simulations can be performed to monitor the motion
of each and every molecule under applied shear and temperature [67]. These simulations
confirm the macroscopically observed behavior. This information is not very useful from the
processing viewpoint, but can help in development of constitutive equations for temperature
dependence of viscosity.

4.2.1 Shear Rate Dependence
For process modeling, one needs a relationship between the stress the material is subjected
to and its deformation rate. Usually, one would express this relationship as
Z = r?i (4.1)
Where T_ is the stress tensor, 7 is the strain rate tensor, and r/ is the viscosity of the material.
For a Newtonian fluid, the viscosity is a constant and can be expressed as
V = H (4-2)
However, for shear thinning materials, such as thermoplastics, one must be able to express
the change in viscosity with shear rate. There are three phenomenological models that are
commonly used to describe the shear thinning nature of the material. They are known
as the power-law model [68, 69], the Spriggs truncated model [70] and the Carreau model
[71, 72]. Their form for viscosity can be expressed as shown below:
(power-law model) (4.3)
if 7 < 70
(Spriggs model) (4-4)
if? > To
(Carreau model) (4.5)
Spriggs
10 100 1000
Shear Rate (1/s)
Figure 4.3: Graphical depiction of viscosity changes with the shear rate on a log-log scale
as described by various viscosity models.
Figure 4.3 graphically depicts how the viscosity changes with the shear rate (7). The
units of shear rate are 1/s. Here, 7 must be independent of the coordinate system to
maintain objectivity, chosen as the magnitude of the strain rate tensor, and given by
7 -r
9 t-~i (4.6)

Figure 4.4: Schematic of a cone and plate viscometer.
Experiments are conducted in a cone and plate device or a capillary rheometer to mea-
sure the viscosity under a prescribed shear rate. Cone and plate, as shown in Figure 4.4, is
usually a suitable device for viscosity measurement at low shear rates. Capillary rheometer
as shown in Figure 4.5 is suitable to measure viscosity under high shear rates.
For Newtonian fluids, the value of the viscosity should be the same at different shear
rates. However, for thermoplastic resins, this is not true. At different shear rates, one
measures different viscosity values. To measure the change in the viscosity as a function of
the shear rate, one has to subject the material to different shear rates. Almost all of the
thermoplastics display a Newtonian plateau at low shear rates, then a logarithmic decrease
with increase in shear rate and again a plateau at high shear rates as shown in Figure 4.6.
Figure 4.3 shows how the constitutive Equations (4.2)-(4.5) try to capture the observed
behavior. The Carreau model correctly captures the behavior of shear thinning materials.
However, one needs to determine four parameters by fitting the form of Equation (4.5) to
the experimental data. One can assume that when the shear rate is infinity the viscosity
goes to zero, i.e., 77(00) = 0, and thus reduce the Carreau model to three parameters.
The Spriggs model needs only three parameters too, but does not predict the plateau at
high shear rates and does not have a smooth transition from the Newtonian plateau to the
power-law unlike the Carreau model. The power-law model requires only two parameters
and does not predict any Newtonian plateau. Thus, at low and high shear rates, the power-
law model will give physically incorrect results, whereas the truncated Spriggs model will
be inaccurate at very high shear rates. However, the power-law model is popular for its
simplicity and captures the essential behavior of shear thinning in the intermediate shear
rate region, which is usually the case when processing such materials.
Example 4.1: Axial Annular Flow of a Power-Law Polymeric Fluid [62]

A fiber of radius R^ is dragged through a cylinder of radius R0 to transfer resin from
container A to container B as shown in Figure 4.7. The resin viscosity can be described by
a power-law fluid.
1. Find the velocity profile of the resin between the cylinder and the fiber, assuming
entrance and exit effects are negligible.
2. Find the volumetric flow rate Q from A to B.

Constant force
or
constant flow rate
2RP
03
0)1 Thermocouple
Melt
reservoir
"Gl
05
1
LUi
2R
Figure 4.5: Schematic of a capillary rheometer.
600 - -
400 - -
Increasing temperature, T
1
o
en
>
g 200 +
CO
10 10
Shear Rate [1/s]
Figure 4.6: Schematic of viscosity versus shear rate at various temperatures for thermoplas-
tic resins.

2R;
2Rr
Figure 4.7: Axial annular flow of a power-law polymeric fluid.
3. What is the force necessary between regions 1 and 2 to drag the fiber with velocity
Solution
1. Attach the radial coordinate frame such that the z direction is along the center of the
rod as shown in Figure 4.7. Postulate that ty — vg = 0 and vz = vz(r) (satisfying the
continuity equation), which implies that
r = r(r). (4.7)
To find the velocity profile, one can use the z direction of motion
1
(4.8)
r dr
as all other terms are zero, if we ignore inertia and unsteady effects due to low Reynolds
number flow.
Note that now we need to subsitute the power-law constitutive model to relate stresses
to velocity gradients
>rz (4.9)
where
(4.10)
and
(4.11)
Since
dvz
= 7zr = (4.12)
dr '
Equation (4.11) reduces to
dvz dvz
7= (4.13)
dr dr

as ^f- < 0 and 7 should be always positive.
Substitution of Equation (4.13) into Equation (4.10) results in
77 = m (4.14)
dr
Substitution of Equation (4.14) into Equation (4.9) gives
(4.15)
dr
Now if one substitutes Equation (4.15) into Equation (4.8), the following differential equa-
tion for vz is obtained:
d
' ' """ l ' = 0. (4.16)
dr [ \ dr
Integrating twice and using the boundary conditions
v
z — o a-t r = i (4.17)
vz = 0 at r = R0 (4.18)
results in
(4.19)
2. The volumetric flow rate can be found as follows:

rtio "l- 1-
Q= 27tri dr — (4.20)
J pij
where re = Ri/R0.
3. The force is calculated as
(4.21)
(re - Kn)R0
4.2.2 Temperature and Cure Dependence

The viscosity of all resins decreases with temperature. For thermoplastics, the constitutive
equation usually follows an Arrhenius law which has an exponential drop in the viscosity
with temperature. The generic form usually is represented as
7?(T) = 770 exp -i- (4.22)

c2T

Temperature, T
Figure 4.8: Sketch of viscosity dependence on temperature for thermoplastics.
where r/o is the viscosity at temperature TO and c\ and 0% are constants that depend on
the material. Temperature dependence of some of the common thermoplastics is shown in
Figures 4.6 and 4.8.
Thermosets also exhibit similar temperature dependence, but their temperature behav-
ior is coupled with the cure kinetics. Usually, the viscosity for thermosets reduces with
temperature, T and increases with degree of cure, a. Both phenomena can be described
well with exponential curves. Hence, the viscosity for a thermoset can be expressed in a
generic constitutive equation as
c
i (4.23)
??(T, a) = ?)o exp —- + c3a
where ci, c% and 03 depend on the thermoset material under consideration. There are many
other ways to characterize the viscosity dependence of reacting systems.
Two concurrent phenomena govern the rheological behavior of a reacting system: one
associated with the intensification of the mobility because of the increase in temperature,
responsible for decreasing the viscosity, and another one related to the growing size of
the molecules during cure, responsible for increasing the viscosity of the resin [73]. The
empirical Williams-Landel-Ferry (WLF) equation [74], valid near the glass transition and
based on the free-volume theory, is frequently used to represent the first phenomenon:
ry
In = (4.24)
where Ci, C% are adjustable parameters and T0 is the reference temperature.

The underlying concept of free-volume theory is that the movement of the molecules is
intrinsically conditioned to the amount of free volume in a molecular ensemble; the less the
unoccupied space, the more the collisions among the molecules, resulting in a slow response
to a perturbation in an equilibrium state [75].
With the objective of accounting for the second phenomenon mentioned earlier, Enns
and Gillham [76] proposed the following equation:
In 77 — In r/oo + In Mu (4.25)
RT0

with rôo as the extrapolated viscosity as T —» oo, E^ as the activation energy and Mw the
average molecular weight. The reference temperature, T0, is arbitrarily chosen to be the
temperature above which the Enns equation is valid to describe the viscosity-temperature
dependence. There are many relations in the literature that describe the average molecular
weight as a function of degree of cure and the molecular weight of monomers [76, 77, 78, 79].
Many authors [80, 81, 82, 83, 84, 85, 86] have followed an empirical equation, which was
proposed by Stolin et al. [87] and was similar to Equation (4.23), in order to calculate the
resin viscosity:
r/(T, a) =
exp ( —- + Ka (4.26)
\K1
where U is the activation energy of the viscous fluid, R is the gas constant and K is
a constant which accounts for the effect of the chemical reaction on the change in the
reacting mass viscosity and, consequently, on the dissipation intensity. It is assumed that
U is independent of the degree of cure. The values for these parameters for two systems are
listed in Table 4.1.
Table 4.1: Parameters for Equation (4.26)

Author System •Ho U K Range of
(Pa.s) (J/mol) (Pa.s) Validity
Lee et al. [84] Hercules 3501-6 7.93xlCT14 9.08xl04 14.1±1.2 a < 0.5
Dusi et al. [86] Fiberite 976 1.06x10-° 3.76xl04 18.8±1.2 a < 0.2
One commonly used empirical relation is [88, 89, 90]:

a+ba
77 = A^ exp (4.27)
a, -.}
The parameters for a few common systems are listed in Table 4.2.
Another related form, proposed by Lee and Han [91, 92, 93] is:
77 = r, exp (4.28)
\RT
where the fluid activation energy, En, and the frequency factor, A,,, are given by:
E^ — a + ba A^ — a0exp(-b0a), (4.29)
with a, 6, a0 and b0 as specific constants for each resin. For example, consider a system
composed of a partially cured unsaturated polyester resin, OC-E701 [91], 43 wt % of styrene
and t-butyl perbenzoate as an initiator. The constants for this system are: a=7.8 kcal/mole;
6=19.7 kcal/mole; a0=6.41xlO~5 N.s/m 2 ; 60=23.1. However, Lee and Han [91] pointed out
that for these values, at temperatures higher than 156.2°C, the viscosity calculated by
Equation (4.28) decreases with an increase in a, which is not physically correct. Hence,
they proposed two other equations, valid for the system used: one based on the Tajima and
Crozier [94] model:
26.8(41.63+ r-90.19a)
log 77(T, a) = (23.64 + 3.82a) - (4.30)
55.03 + T- 90.19a

Table 4.2: Parameters for Equation (4.27)
Authors System An Er, «9 a b Range of
(Pa.s) (J/mol) Validity
J. M. Castro and RIM2200 10.3xlO~8 41.3 0.65 1.5 1.0

C. W. Macosko [88]
(1980)
J. M. Kenny et al. Commercial 3.416xlO-n 64900 0.088 3.706 -34.62 30-60° C

[89] grade
(1990) thermoset
DSM resin
for RTM
D. S. Kim and DGEBA 3.60xl<T10 58600 0.765 1.0 5.2 70-90° C

S. C. Kim [90] and
(1994) TETA
(lOphr)
and another one based on the Hou [95] model:
-T- (4.31)
Hence, it should be clear to the reader that development of a universal formula for viscosity
as a function of temperature and cure does not exist. However, forms suggested in Equations
(4.26)-(4.28) can accomodate many thermoset resin systems.
4.3 Viscosity of Aligned Fiber Thermoplastic Laminates

The deformation of a bundle of aligned fibers lubricated with viscous resin is primarily
viscous. The deformation response of such materials will be a strong function of the na-
ture of the resin and the fiber arrangement. For transversely isotropic bundles or lami-
nates, there are two dominant shear modes: longitudinal shearing and transverse shearing.
The schematics of the two modes are shown in Figure 4.9 [6]. Both shear modes may
be important as aligned composite laminates are deformed to form complex shapes. For
thermoplastics, these material constants display non-Newtonian behavior and need to be
characterized. For thermosets, one must separately consider the elastic deformation of the
fibers by characterizing the elastic constants. In this section, we will only consider the
transverse deformation of a material, which on a microscale consists of fibers and resin but
is treated as a homogeneous material on the macroscale.
Thermoplastic composite sheet forming involves the deformation of a laminate within
and out of the plane and is characterized by the flow of resin and fibers. It is, therefore, nec-
essary to have effective constitutive relations describing the highly anisotropic flow behavior

(a) Transverse Shear (b) Longitudinal Shear
Figure 4.9: The deformation response of a bundle of aligned fibers lubricated with viscous
resin. For transversely isotropic bundle or laminates, the two dominant shear modes are (i)
transverse shearing, and (ii) longitudinal shearing [6].
of these laminates. Unfortunately, the shear and extensional properties of long discontinu-
ous fiber reinforced composites in their melt state are difficult to obtain using traditional
rheological techniques, such as cone and plate and capillary rheometers, due to the presence
of continuous or long fibers.
One way to describe their shear behavior is to use squeeze flow to characterize the
bulk transverse shear viscosity of these highly filled viscous resin systems. Squeeze flow is
invoked by placing the material between two impermeable platens and applying a normal
force. One may characterize the material under constant applied load or under a constant
closure rate of the platens. Such industrial testing devices are referred to as the parallel
plate plastometer or squeeze plate viscometer [96, 97]. These devices measure radial flow
between two parallel disks and have been used to study the viscosity of polymer melts and
other viscous materials.
The advantages of this type of test include mechanical simplicity, inclusion of fibers
without the danger of attrition, achievement of very high shear rates, usage at high tem-
peratures and the ease with which high-viscosity materials can be tested [98]. Additionally,
this type of flow is of interest since it is encountered within lubrication systems and the
stamping of plastic sheets. Finally, it provides a technique for investigators to evaluate
rheological equations under transient conditions.
In the parallel plate plastometer, the test material, in the form of a cylinder, is placed
between parallel, circular flat plates. With the lower plate fixed, either a constant force
or a constant closure rate is applied to the upper plate. If a constant force is applied,
measurement of the resulting displacement of the upper plate is used to determine the
rheological properties of the specimen. If a constant closure rate is applied, measurement
of the resulting force on the upper plate is used to determine the viscosity dependence
on shear rate. Although these experiments involve unsteady shear flows, the flow rates
are usually modest so that the analyses are based on quasi-steady state solutions. Two
different sample arrangements may be used in the plastometer. Either the specimen sample
cross-sectional area can be equal to the cross-sectional area of the plates, in which case the
area under compression is constant, or the cross-sectional area of plates may be larger than
the specimen sample, in which case the volume of the specimen is constant.
Squeeze flow rheometers have been used to study both unfilled viscous and viscoelastic
liquids and have been modified to study fiber filled thermoplastic materials. Experimental

squeeze flow studies on polymeric liquids indicate that under slow loading rates, their behav-
ior can be approximated through the shear dependent viscosity [99, 100, 101, 102]. However,
under rapid loading, viscoelastic effects may become evident [103, 104, 105, 106, 107, 108].
The magnitude of the material's Deborah number is often used as a determinant of its re-
sponse. The Deborah number, De, is denned as the ratio of the fluid's relaxation time to a
characteristic time of the squeezing process. Low values of the Deborah number correspond
to viscous fluids while high Deborah numbers correspond to fluids with an elastic response.
The flow of sheet molding compounds was investigated in [109, 2]. The squeeze flow
behavior of aligned fiber reinforced thermoplastic materials has been discussed in [110, 111,
112]. They treated these composites as transversely isotropic materials. Experimental ob-
servations of aligned fiber reinforced APC-2 material by these investigators showed that the
resulting squeeze flow deformation is strictly perpendicular to the fiber direction. This is
due to the high ratio of extensional viscosity in the fiber direction, which is infinite in the
case of continuous reinforcement, to the shear viscosity of the composite transverse to the
fiber direction. Therefore, with no resin percolation out of the fiber bed, these compos-
ites have been viewed as incompressible anisotropic fluids with an effective shear viscosity
transverse to the fiber direction. O'Bradaigh [113] has experimentally measured the effects
of transverse squeeze flow on the cross-sectional thickness variation of diaphragm formed
from APC-2 components. Hull, Rogers and Spencer [114] have examined the evolution of
fiber wrinkling during these squeezing flows.
Shuler and Advani [2] used a servohydraulic test frame with specially designed hot
platens. These test platens, as depicted in Figure 4.10, consisted of two square steel platens
fastened to two specially constructed round steel fixtures attached to the test frame's hy-
draulic rams. Cartridge heaters were mounted within these fixtures to provide the platen
heat and were controlled through feedback controllers that can receive temperature infor-
mation from thermocouple probes mounted within the steel platens. Shuler and Advani [2]
mounted a video camera perpendicular to the sample, recording the material flow during
the test. For steady squeeze flow testing, a constant force may be applied and the change
in height measured over time, or a constant closure rate may be applied with the change in
force measured over time through appropriate load cells. If desired, special oscillatory, dy-
namic or exponential loading rates may also be applied through the servohydraulic system.
Air Jets
Hot Platen
Cartridge Heaters (*6)
Clamp
/l\K M Clamp
i Beam
W Thermocouples (*6) ^l//
Hot Platen
Figure 4.10: High temperature squeeze flow set up for thermoplastic composite laminates
in a servohydraulic test frame [42].
With this system, they tested three different combinations of aligned fiber materials:

clay matrix with nylon fibers, clay matrix with glass fibers, and PEEK matrix with aligned
carbon fibers (APC-2). The model matrix of clay was prepared with various volume frac-
tions of nylon fibers and 60% glass fibers. The thermoplastic PEEK material contained 64%
aligned carbon fibers. The sample size was 1 cm in thickness and occupied the complete
cross-sectional area of the platen that would squeeze the sample with the hydraulic cylin-
der. The force and displacement data were recorded. As the clay matrix displayed shear
thinning behavior well described by a power-law model, the same constitutive form
rj(j) = m-jn-1 (4.32)

for the composite was assumed. The analysis showed that one could match the experimental
data by modifying just the bulk viscosity constant m, as shown in Table 4.3.
Table 4.3: Power-law Viscosity Parameters for Unfilled and Fiber Filled Clay
Fiber Volume Percentage Platen Closure Rate [cm/min] m [Pa sn] n
0 0.0254 to 0.762 30,000 0.1
20% Nylon Fibers 0.0254 82,000 0.1
40% Nylon Fibers 0.0254 110,000 0.1
50% Nylon Fibers 0.0254 300,000 0.1
60% Nylon Fibers 0.0254 810,000 0.1
60% Glass Fibers 0.0254 1,650,000 0.1
They found that the unfilled clay and the filled samples behaved as shear thinning power-
law fluids. Table 4.3 summarizes the results that were plotted over a broad range of shear
rates. It reveals the decidedly nonlinear relationship between the composite's transverse
shear viscosity and the percentages of fibers. The clay filled with 60% nylon fibers resulted
in a transverse shear viscosity 27 times greater than the viscosity of the unfilled clay, while
60 volume percentage of the glass fibers resulted in a transverse shear viscosity 55 times
greater. From this information, it seems that adding the same volume percentage of smaller
diameter fibers has the effect of increasing the transverse shear viscosity even more than
the increase found using larger diameter fibers.
The reinforcing PEEK matrix polymer in the APC-2 laminates is known to behave as
a shear thinning Carreau-type fluid. The four parameter Carreau fluid can be reduced to
three parameters by assuming that the fluid viscosity goes to zero at infinite shear rate.
Thus, the three-parameter Carreau fluid model [71, 72] describes the viscosity as Newtonian
behavior at low shear rates followed by shear thinning power-law behavior at higher shear
rates, and is commonly expressed as:
(A7) (4.33)
where 770 is the zero shear rate viscosity — the viscosity of the material when deformed
infinitely slowly, n is the shear thinning exponent that adjusts the slope of the shear thinning
region and A is a time constant that adjusts the position of the "knee" in the r]vsj curve
where there is an onset of shear thinning behavior. The Newtonian model is recovered for
n = 1, and the power-law expression is approached for large values of A.
For the PEEK matrix, these viscous parameters were measured by [115] and are listed
in Table 4.4. Viewing the transverse shear flow of the fiber filled matrix as viscous flow

with a lubricating fluid between the fibers, the Carreau model was investigated as perhaps
an appropriate model to also describe the shear thinning viscous behavior of the APC-2
composites.
Table 4.4: Carreau Viscosity Parameters for PEEK at 370°C

PEEK Carreau Viscosity Parameters at 370° C:
770 = 687Pa.s
A = 0.0932sec
n = 0.787
Shuler and Advani [2] collected the platen force data for the four closure rates and used
least-squares fit to the Carreau model to find the parameters for the bulk transverse shear
viscosity of the APC-2 laminates. The three Carreau parameters of Table 4.5 were found to
produce loading curves that closely matched the experimental platen force data collected.
Table 4.5: Carreau Model Parameters for the Transverse Shear Viscosity of APC-2 Material
at 370°C.
APC-2 Transverse Shear Viscosity Carreau Parameters at 370°C.
•to = 2.5 * 106Pa.s
A = 50.0sec
n = 0.65
The Carreau model curve for the transverse shear viscosity of the APC-2 material at
370°C based on the parameters listed in Table 4.5 are graphed in Figure 4.11. The Carreau
model viscosity of the neat PEEK matrix polymer at 370° C is graphed in Figure 4.11 as well.
It is noteworthy that the transverse shear viscosity of the composite is approximately 3600
times greater than viscosity of the PEEK matrix resin. Also, the onset of shear thinning
behavior occurs at a lower shear rate than for the neat resin. Since the Carreau model
captures both the Newtonian behavior at low shear rates and the shear thinning behavior
at higher shear rates, this three parameter model is able to describe the viscous behavior
of the unidirectional APC-2 laminates over a range of shear rates.
It is instructional to note that during squeeze flow the material experiences a range
of shear rates that vary both over time and throughout the volume of the material. The
transverse shear rates encountered in squeeze flow range from very low at the start of each
test and at the symmetry planes to a maximum which occurs at the largest closure rates
adjacent to the platen contact surfaces near the outer edges of the samples. Because squeeze
flow encompasses such a broad range of shear rates throughout the volume of the material,
a simple Newtonian or power-law fluid model cannot adequately describe the squeeze flow
behavior of the laminate that, depending on the shear rate, follows both Newtonian and
shear thinning behavior. Hence the use of the Carreau model is more appropriate for
composite laminates.
Example 4.2: Squeeze Flow of GMT Material

A thermoplastic material reinforced with fibers (GMT) is expected to behave as a power-law
fluid. To find the power-law constant, m, and the power-law index, n, squeeze flow of GMT

10'
T=370'
10"
w 10 APC-2 Carreau Parameters

ro Ti_=2.5e6 Pa-s
Q.
X=50.0 s
n =0.65
to
8
w
PEEK Carreau Parameters

10
Ti.=687 Pa-s .„_.
^'=0.093 s
n =0.787
10'
10 10" 101
Shear Rate (s )
Figure 4.11: The Carreau model curve using the parameters listed that describes the trans-
verse shear viscosity of the APC-2 material and the resin PEEK at 370°C [42].
between two disks is proposed as shown in Figure 4.12, in which one can measure the force
and the displacement. Conduct the analysis to delineate the approach.
Solution
As h <C R, one can assume that shear forces will dominate. Also for GMT materials, the
viscosity is very high such that the Reynolds number is much less than unity. Hence, one
can ignore the inertia forces and assume a quasi-steady state process. A "quasi-steady
state" as we will see in Chapter 5, implies a "steady state" at a given instant. This allows
us to solve the steady-state problem at any height h, which will then change at the next
instant and the velocity profile will change accordingly and achieve steady state instantly.
Using mass conservation for a disk of any radius r < R, one can show that
f
-'fnrr = 2vrr / vr dz (4.34)
Jo
where VT is the radial velocity and h = dh/dt is the instantaneous disk velocity. See Figure
(4.13) for the derivation of Equation (4.34).
The mass that disappears in the ^-direction must appear in the radial direction as shown
, ^ dz.
pvrr — = p I 2iTrvr(z) , (4.35)
In the equation of motion, as only the shear stress component rrz is important, the r
component of the equation, ignoring inertia and gravity as well, reduces to
drrz dJP
(4.36)
dz dr '

2h(t)
Figure 4.12: Schematic of GMT material between two parallel disks of radius R with cylin-
drical coordinate system placed midway between the disks.
"\ Velocity profile, vr (z)
symmetry
Figure 4.13: Sketch of velocity profile of the material between the midplane and the upper
platen in compression molding of a radial charge.

The changing radial velocity vr(z) is introduced through the boundary condition at z = h(t)
vr(z = h) = Q. (4.37)
Further, because of symmetry
f)n
^=0 at z = 0. (4.38)
\JZ
The other two components of the equation of motion reduce to ^ = 0 and §f = 0;

hence P is a function of r only as shown in Figure 4.13. Thus one can integrate Equation
(4.36)
(4 39)
.dr>" '
For power-law fluids,
/ rli \n
(4.40)
Substitution of Equation (4.39) into Equation (4.40) and integration of vr with respect to
z results in
\ i+s"
(4 41)
1 + s V m dr s) '
where s = 1/n. Note that the velocity profile is identical to fully developed flow between
parallel plates separated by distance 2h. Now, one subsitutes Equation (4.41) into Equation
(4.34), and integrates with respect to z, to obtain the following differential equation for P(r):
One can integrate Equation (4.42) to obtain the pressure profile
„ „ m(2 + s}n(-h}nRl+n " l+n
where Pa is atmospheric pressure at r = R. The maximum pressure as expected is at the

center (r = 0).
The total instantaneous force that must be applied to the disk to maintain the closing
speed of h is obtained by integrating P over the disk surface
Equation (4.44) is called Scott's equation [102].

If h was constant, one could rewrite Equation (4.44) as
(4 45)
-
where

By taking the natural logarithm of Equation (4.45), one can obtain
'I'
(4.47)
One can find A and b from the plot of In F versus In ( ^ ) as shown in Figure 4.14. From b,
ln(F)
In (A)
In (1/h)
Figure 4.14: Approach to find the power law parameters from squeeze flow compression
experiment in which the material is squeezed at the constant rate of h and the required
force, F, is measured.
one can find n. Knowing n, R, s = l/n and A, one can find m. •
Next, we will discuss how the presence of short fibers influences the viscosity and how
one can model this physical effect.
4.4 Suspension Viscosity

In processes such as injection molding and extrusion, a short fiber suspension is created
when the polymer in the pellets, containing the short fibers, melts. In compression molding
of short fiber composites, materials such as sheet molding compound (SMC) that contain
chopped glass fibers are heated to soften the resin to a paste to form a suspension. This
suspension is then pumped into a mold in the case of injection molding, through a die in
the case of extrusion, or squeezed into a mold by mold platen in compression molding.
The fibers are convected with the polymer and solidify to create the short fiber composite
part. The important issues here are the microstructure created in the part by the fibers
due to their orientation and concentration distribution and the process parameters such
as injection pressure and flow rate needed to inject the suspension into the mold or die.
Suspension viscosity plays a crucial role in modeling of these issues.
4.4.1 Regimes of Fiber Suspension

A suspension of uniform, cylindrical rods (approximation for fibers) is characterized by the
particle volume fraction c and the fiber aspect ratio r — L/D, where L is the fiber length
and D the fiber diameter. A suspension is dilute only if
1
c< -z. (4.48)
r2

Often this requirement is phrased in terms of 'the number density n (particles per unit
volume), and the requirement for a dilute suspension is
- . (4.49)
When the fibers are long and slender (r <C 1) this requires a very small volume fraction. For
example, a suspension with fibers of aspect ratio equal to 100 must have a volume fraction
less than 0.01% to be dilute. If the fiber volume fraction is increased such that
1 1
or (4.50)
then the suspension is said to be semi-dilute. In this regime the fibers seldom touch,
but fibers experience frequent fluid-mechanical interactions from the perturbation of fluid
velocity caused by the nearby fibers. Some workers call this the semi-concentrated regime.
Increasing the volume fraction still more, to
1
<c or n> (4.51)
reaches the concentrated regime. Here the average interfiber spacing is of the order of a
fiber diameter, so that each fiber is always touching, or nearly touching, many other fibers.
Figure 4.15 maps out these regimes in terms of volume fraction and aspect ratio. As
shown in the figure, all commercial composites fall into the concentrated regime. No com-
mercial materials are truly dilute. Hence we will discuss here the phenomenological equation
to describe the viscosity of concentrated suspensions.
1000
£ 100
CO
o
0)
Q. 10
.001 .01 .1
Volume Fraction, c
Figure 4.15: Different regimes of concentrations for fiber suspensions [116].
The most important action of a fiber in a suspension is to resist stretching of the fluid
along the fiber axis. All fiber suspensions have high viscosities in the fiber direction. This

effect is greatest in steady uniaxial elongation in which the flow field lines are along the
fiber length direction, where the fibers exert maximum resistance to the stretching motion.
In contrast, fibers add very little resistance to a shearing motion either parallel or
perpendicular to the fiber axis. If one models the fiber using slender-body theory, the fiber
adds no resistance to these motions at all. Shearing flow tends to make the fibers align
parallel to the planes of shear, where they exert minimum resistance to the deformation.
As a result, fiber suspensions have much lower viscosities in steady simple shear than in
steady uniaxial elongation. That is, their Trouton ratio rje/rjs is much greater than three.
The low shear viscosity relies on fibers being aligned in the flow direction. This is usually
not true in a start-up flow. If the fibers are initially random, then the shear viscosity is
high. After a small amount of strain the fibers start to align, and at some point many
fibers orient around 45° to the flow direction. This is the direction of greatest stretching
in a simple shear flow, so at this point the viscosity reaches a maximum. With continued
shearing the fibers rotate towards the flow direction, and viscosity drops steadily until it
reaches the low steady-state value. There will also be normal stresses during the start-up
of steady shear, as each fiber contributes to the stress in the direction of its axis. If the
final fiber orientation is not symmetric about the plane of shear, the normal stresses will be
present at steady state.
Suspension viscosity, in addition to the volume fraction, c and the aspect ratio, L/D of
the fibers, will also depend on the orientation state of the fibers. Hence it is important to
characterize the orientation state. It is relatively simple and straightforward to characterize
c as it is the ratio of the volume of fibers to that of the total suspension volume. Aspect
ratio is also easily characterized using the geometry of the fiber. However, to characterize
the orientation state, one needs to develop a description.
Description of the Orientation of a Single Fiber

The orientation of a single fiber relative to a reference coordinate system can be specified
by the angles (<j>, 9} as shown in Figure 4.16.
Figure 4.16: Definition of the orientation of a single fiber in a Cartesian coordinate frame
[117].

Alternatively, one can describe the orientation of the. fiber using a unit vector p directed
along the fiber axis. The two descriptions are related
pi = sin 9 cos (f> (4.52a)

p2 = sin 0 sin <j> (4.52b)
p3 = cos9 (4.52c)
where p; (i=l,3) are Cartesian components of p. Orientation space is the set of all possible
directions of p and corresponds to the surface of a unit sphere. Sometimes, the fibers
are long and the parts are thin which constrains the fibers to lie in the plane. Thus the
orientation is called two-dimensional or planar orientation. In Figure 4.16, if one selects the
1-2 plane as the planar orientation plane, then 9 will be equal to vr/2 or p% equal to zero
for every fiber. The planar orientation can be described by either (f> or a two-dimensional
vector p. The orientation space for two dimensional orientation will be a unit circle.
Probability Distribution Function

In a real composite there are fibers oriented in many different directions. Figure 4.17 is
a redrawn image of some of the fibers in a composite and denotes the complexity of the
situation. It should be clear that, in practice, it will be a formidable task to keep track
of the orientation of each individual fiber. It will be useful to use a description that can
embody many different directions.
Figure 4.17: Sample of fibers digitized from a radiograph of a plaque of sheet molding
compound [118].
The most basic description is the probability distribution function. If we consider a small
region from a composite or a suspension, we would expect to see many fibers with different
orientations of fibers. The probability distribution will give us a measure of the state of
fiber orientation at that location. Thus one can define if>(0, (f>) such that the probability of

the fiber lying between the angles 6 and (6> + dO) and angles </> and (^ + d(j>) is given by
1^(6, 4>] sin Od0d(/>. Here sin 9d9d<j) is the increment in area on the surface of the unit sphere.
This distribution function can also be represented in vector form as V'(p)- F°r planar cases,
as sind is unity, the distribution function can be represented as ?/>^(</>).
This distribution function must satisfy two obvious conditions. First, one end of the
fiber is the same as the other end; hence, ip must have the property of periodocity,
>)=i/>(v -&,</> + IT). (4.53)
For the planar case,

V ^ ) = ^ + T). (4.54)
Secondly, every fiber must have some direction, hence the integral of the distribution func-
tion over the surface of the orientation space must be unity
f2lT /"7
/ / = 1. (4.55)
Jo
JO Jo
JO
For planar situations

c9ir
(4.56)
This is known as the orientation normalization condition.

The distribution function •0 is a complete description of the orientation of the fibers at
any location. Thus if the orientation state changes with position in a flowing suspension, ijj
will be a function of position in addition to a function of the angles 9 and </>.
To estimate the distribution function at a given location, one should first capture an
image of the fibers at that location, for example, the image shown in Figure 4.17. Let us
suppose that the image is a planar one; thus to estimate ^, one would create a histogram
as shown in Figure 4.18. This is done by dividing the histogram in n bins, each of width
(vr/n). Hence to find the orientation average of any function, one can use ijj as the weighting
function.
Therefore, the orientation average of any function g(9,4>] is given as
< g > = f * T ^ (j)}g(0, (j>) sin Qd0d(f>. (4.57)

Jo Jo
That is, < g > is the average of g over all directions, weighted by the probability distribution
function.
Orientation Parameters
The probability distribution function is a complete description of orientation state, but
it is also cumbersome. A number of orientation parameters have been defined to provide
concise and more easily interpreted measures of orientation. The best known is the Hermans
orientation parameter. It concerns the special case of axisymmetric orientation, when the
fibers are uniformly distributed in <f> so that i/j is a function of 9 only. The extent of alignment
around the 9 = 0 axis is then measured by the parameter /, defined as
/=3<cos 0>-l_ (45g)

1.5
67% Initial Mold Coverage
o
'• 1.0
m
5
0.5
-n/2 o
1 71/2
Orientation Angle,
Figure 4.18: Histogram and probability distribution function for the fiber orientation in
Figure 4.17 [118].
When the orientation is random / — 0, while completely aligned fibers give / — 1.

Many other orientation parameters have been defined. It can be shown that, if the
probability distribution function has certain symmetries about the coordinate axes, then a
particular set of orientation parameters provides all the information needed to predict the
influence of orientation on the elastic properties of a composite. However, as there is no way
to model the influence of processing conditions on the orientation parameters, they cannot
be used to predict flow-induced orientation.
Orientation Tensors
A description which combines the generality of the probability distribution function and
the concise nature of the orientation parameters is a tensor description of orientation. A
second-rank orientation tensor can be defined as
dij = < p^ > (4.59)
and a fourth-rank tensor as
a>ijkl = < PiPjPkPl > (4.60)
That is, the components of the orientation tensors are formed by taking the orientation
average of the products of components of the vector p. These tensors are a generalization
of the orientation parameters. It is evident from their definition that a^ and aî will
transform according to the rules of tensor transformation, so they are tensors. They are
also symmetric, i.e.
Oij = a-ji (4.61)
The normalization condition, Equation (4.54), implies that the trace of d^ is unity,
Oij = I (4.62)

(In this and all subsequent indicial equations a repeated index implies summation over all
possible values.) Equations (4.61) and (4.62) show that only five of the nine components
of Oij are independent. For planar orientation the tensor a^ has four components, but
only two are independent. The tensor description of orientation replaces the distribution
function with a small number of discrete values.
Figure 4.19 shows some example planar orientation states and the corresponding ori-
entation tensors. When an equals unity then all the fibers are aligned along the 1-axis.
When an and ayi both equal one half, the fibers are randomly oriented. If the direction of
principal orientation is other than the 1-axis or the 2-axis then a\i will be nonzero.
Random Aligned
is: •x-/ -i
0.5 Ol F0.7 Ol _ F 1 0
a
<t~[0 0.5] "V ~ [ 0 0.3J "*' [ 0 0
Figure 4.19: Planar fiber orientation states and the corresponding tensor representations.
There are a number of physical interpretations of the orientation tensors. They can
be thought of as a generalization of the orientation parameters, as the moments of the
probability distribution function or as the coefficients of a series expansion of the distribution
function. For a complete review see [119]. For the present we note that the orientation
tensors are free from assumptions about the shape or symmetry of the distribution function,
and can be readily expressed in any convenient coordinate system.
Example 4.3: Orientation Tensor for Uniformly Distributed Fibers in 3-D

If the fibers are uniformly distributed in three-dimensional space, what will the components
of a be?
Solution
As the fibers are uniformly distributed, an = a^ = 033 and 012 = a23 = asi = 0. From
normalization, we know that an + 022 + 033 — 1. Thus,
i 0 0
0 i 0 (4.63)
0 0 I
It can also be proved that the nth-rank orientation tensor provides sufficient information
to predict the effect of orientation on any nth-rank property of the suspension or composite.

Viscosity and elastic stiffness are fourth-rank properties, and one would normally have to
know ciijki to predict them. However, we will later see ways to approximate a^ki in terms
of dij, so that the second-rank tensor dij can be used as a description of orientation state.
The orientation tensors can easily be determined from experimental data. If the ori-
entation of N fibers is measured, and if the vector pk describes the orientation of the /cth
fiber, then the second-rank tensor is approximated by
an =
where wk is the weighting factor for the fcth fiber. If the fibers are almost circular in cross
section, then wk can be taken as 1, which reduces Equation (4.64) to
This equation presumes that the sample is unbiased [120].
4.4.2 Constitutive Equations

For process modeling purposes one is interested in a general constitutive equation — one
that represents the behavior of the material in any type of flow: shear, elongation or mixed;
steady or unsteady. It is also important to account for the effect of fiber orientation. A
suspension in a given flow field will exhibit different stresses if its fiber orientation state is
different.
Typically the compressibilities of the suspending fluid and the fibers are negligible, so
the total stress a^ is separated into an isotropic pressure P and an extra stress r^:
aij = -P6ij + nj (4.66)

Subsequent attention is focused on relating the extra stress to the fiber orientation state,
the rate of deformation, and suspension parameters such as the fiber volume fraction, the
fiber aspect ratio and the viscosity of the suspending fluid.
A variety of theories exist to predict the viscosity of suspensions of fibers in a Newtonian
fluid. All of them can be written in the general form for TJJ [121]:
B [îkakj + a^j] + C%- + 2FdijDr (4.67)

Here 7^ is the rate of deformation tensor, rjs is the solvent viscosity, c is the particle volume
fraction, A, B, C and F are material constants, and Dr is the rotary diffusivity due to
Brownian motion. Note that the extra stress r^ is a linear function of the instantaneous
rate of deformation, except for the rotary diffusion term. This term is usually neglected for
suspensions of fibers with large aspect ratios. The dij and dijki are orientation tensors that
describe the state of fiber orientation at that location.
Exact expressions for the coefficients A, B, C and F are given in [122, 123] for dilute
suspensions. For a semi-dilute suspension, slender-body theory was used following the work
of [124]. Batchelor [125] used this type of theory to model the stress in a fiber suspension
undergoing uniaxial elongational flow, assuming that the fibers were all aligned in the
direction of stretching. Batchelor modeled the fluid-mechanical interaction between the
particles, treating each fiber as lying within a cell created by the surrounding fibers, and

thus extended his theory beyond the dilute range. A key physical concept in Batchelor's
theory is the idea of hydrodynamic screening, which assumes that the velocity disturbance
caused by each particle is felt only a distance L away. The particle's nearby neighbors limit
the long-range disturbance, and the major effect of the particle is to alter the fluid velocity
only in the immediate vicinity. [126, 127] derived the constants by substituting the result in
[125] into a general constitutive equation. Shaqfeh and Fredrickson [128] have developed a
theory that gives this as the correct result for isotropic (3-D random) orientation in a dilute
suspension. They argue that Batchelor's result for A is correct for any orientation state,
provided the suspension is dilute. Dinh and Armstrong [127] used an approach similar to
[125] and adopted ideas from liquid crystal theory about the distance between a fiber and
its nearest neighbors to determine the cell size to predict the constants.
The slender-body approach is quite useful because it allows a way to incorporate hy-
drodynamic interactions and model nondilute suspensions, but it has some limitations.
Slender-body theories are strictly applicable only for very high aspect-ratio fibers, so they
might not be very accurate when the fiber aspect ratio is low (say, r = 10). Also, slender-
body theory cannot represent the interaction between two fibers that pass within a distance
on the order of D of each other, so truly concentrated suspensions cannot be modeled.
Still, these theories do extend into the semi-dilute range, and give a good idea of the type
of constitutive equation one might use, even for a concentrated suspension.
Equation (4.67) can easily be recast into the form
T
ij = f]i [Jij + Npjkidijki + Ns {jikdkj + aijjkj}} (4.68)
where the coefficients 777 , Np and Ns depend on rjs, c, A, B and C, and a^ and aî are the
second and fourth ranked orientation tensors. Now 777 contains all the isotropic contributions
to viscosity (from both the solvent and the particles), while anisotropic contributions by
the particles are represented by two dimensionless parameters, Ns and Np. Np is called the
particle number and N3 the shear number [121]. These parameters depend on the particle
aspect ratio and volume fraction, but (at least for dilute suspensions) not on the orientation
state of the fibers. When both of these parameters equal zero, Equation (4.68) reduces to
an isotropic Newtonian fluid.
The particle number Np is the key rheological parameter to describe the behavior of a
fiber suspension. Physically it represents the factor by which the suspension resists elonga-
tion parallel to the fiber direction, as compared to other deformations. Evans [126] was the
first to identify this parameter and its key role in suspension rheology. For a suspension
of slender particles Np can be quite large. Figure 4.15 shows how Np varies with volume
fraction and aspect ratio according to the theory of Dinh and Armstrong, using the aligned
assumption for inter-particle spacing. The other theories give similar predictions.
4.5 Reaction Kinetics

An important processing step in reactive polymer composites, which usually involve ther-
moset resins, is the reaction that starts from monomers or oligomers and through an addition
or condensation mechanism forms a three dimensional cross-linked network. The reaction
can be activated either thermally by heating up the monomer or chemically by the addition
of initiators. The phenomenon is generally referred to as curing of the resin. The degree
of cure is usually proportional to the fraction of the network formed. The reaction is an
exothermic one, so heat evolved during the formation of the network needs to be convected
out of the composite.

Some of the important resins that react as they are processed are phenolics, unsatu-
rated polyesters, epoxies and thermoset urethanes. Often, these materials are processed by
compression, autoclave or liquid composite molding. The advantages of reactive processing
are that the material is shaped into its final form before it reaches high molecular weight
(hence viscosities are low and consequently the pressures required for processing are low).
One of the disadvantages is that one has to deal with removal of the heat generated during
the reaction. In order to understand reactive processing, one must have an appreciation of
the reaction kinetics (how the reaction proceeds with time and temperature). Once this is
understood and characterized, the familiar concepts of momentum and energy balance as
detailed in Chapter 3 can be applied to predict the interaction of cure with flow and heat
transfer.
The reaction may be easy to characterize, as in the case of epoxy and polyester resins, or
may be very difficult to describe, as in the case of polyamides and polyurethanes that evolve
volatile by-products. However, it is important to characterize the cure kinetics of the resin
because it influences the viscosity of the resin and may govern the flow of the resin. Secondly,
as significant heat is evolved during the curing of the resin, it cannot be ignored when
modeling the heat transfer process during manufacturing. Modeling of the heat transfer
phenomenon during processing allows the engineer to predict the temperature history of
the composite during manufacturing and to design appropriate heating and cooling cycles
for the material. If an appropriate cooling system is not designed, the polymer can degrade
due to the excess heat generated by the reaction. Thirdly, reaction kinetics can forecast
the time of resin gelation. The gel point is defined by the degree of cure at which the resin
has networked sufficiently that it no longer needs the mold or the die to maintain its final
shape and can be demolded. This can help save processing time for the component. The
resin is allowed to reach complete cure outside the mold in an oven or on the factory floor.
Hence, there is the need for a constitutive equation that can describe the reaction on
a macro scale and can be coupled with the momentum and energy equations to determine
the pressure, temperature and degree of cure simultaneously. On the micro scale, if there
is evolution of volatiles or water vapor during the curing process, it can lead to micro void
formation. To model void formation and growth, one may need many constitutive parame-
ters to describe the mass diffusion process such as mass transfer coefficient, expressions for
vapor pressure, partial pressure and solubility which are usually not readily available.
The general approach to the constitutive equation development for resin kinetics is
traditionally derived from the type of the reaction and the chemistry of the reaction. Ther-
mosets usually cure by either addition polymerization (for example, unsaturated polyesters)
or condensation polymerization (for example, urethanes). Consider, as a typical example,
the reaction between two chemical groups denoted by A and B which link together two
segments of polymer chain PI and P2:
PiA + P 2 B-PiABP 2 (4.69)
For example, if it was the polyurethane reaction, A would represent an OH group and B an
NCO group, resulting in
PiOH + P 2 NCO = Pi-N-C-O-P 2 (4.70)
H O
The reaction can be tracked by monitoring the instantaneous concentrations of A and B,
denoted by CA and CB- They can be measured in moles per gram and will decrease with
time as more A's and B's react with one another to polymerize.

The rate at which the constituents A and B react will in general depend on the temper-
ature and on the concentration of the reactants (sometimes catalysts are added to speed
up the reaction). The higher the number of A and B molecules in a given space, the more
likely it is that some will react. An equation describing the reaction rate as a function
of concentrations of the reactants and temperature is called a kinetic equation because it
describes the motion of the reaction. Many reactions of this type follow a kinetic equation
such as
Ra (moles per gram per second) = ——^ = k0 exp (-E/RT) CAC% (4.71)
(2iC
While in some cases there is a good physical reason for choosing one kinetic type of equation
over another, mostly one can think of a kinetic equation as an empirical model which mimics
the behavior of the resin. Equation (4.71) is referred to as a second order kinetic equation,
because two concentrations are multiplied together on the right-hand side. A first order
kinetic equation will depend on the concentration of only one of the groups. For example,
if it was dependent on group A only, then
7x~y
Ra (moles per gram per second) = -- -— = fcoexp (-E/RT) CA (4.72)

at
This obviously is not appropriate for this reaction since B groups as well as A groups must
be present for a reaction to occur. In Equation (4.71), ko is the rate constant and is the
empirical parameter to be determined from experiments, E is the activation energy for the
reaction, R is the universal gas constant and T is the absolute temperature in K.
Once the kinetics are defined, one can analyze how the reaction proceeds with time.
First, note that Ra is the rate at which the A groups disappear. Also as one B group reacts
with one A group, so
d_C^ = dCB
dt dt ^ '
The initial conditions for Equation (4.71) are the known initial concentrations of A and B,
denoted by CAO and CBO- Instead of tracking C\ versus time, it is more useful to find the
extent of reaction C* , which can be defined as
C* = (4.74)
C* is zero when there has been no reaction and equals unity when all of the A's have
been consumed and the reaction is complete. C* can also be called the degree of cure or
conversion (also sometimes the symbol a is used to denote degree of cure). Substitution of
this in Equation (4.71) with some algebraic manipulation gives
dC1*
— = k0 exp (-E/Rr)CAo(l - C*)(A - C*) (4.75)
with an initial condition of C* — 0. Here A is equal to CBO/CAO, and A equals one if A and
B are present in equal number of moles.
Example 4.4: Degree of Cure with Time

If the temperature of the polymer is held constant at T — 400°K and A — 1, then using
Equation (4.75) plot degree of cure with time for initial concentration of CAO = 0-5. Assume
reasonable values for other parameters. How do the results change, if the temperature is
lowered to 350°K?

Solution
One can integrate the ordinary differential Equation (4.75) to find cure as a function of
time:
C* = (
k0exp(-E/RT)CA0t ' '
t (sec)
Figure 4.20: The degree of cure as a function of time for the parameters chosen in Example
4.4.
One can easily plot this equation for C* with respect to time. Selection of ko = 3 and
E/R = 300 results in the plots shown in Figure 4.20. •
For a reaction in which temperature varies with time, which is the case for all composite
processing methods, one needs to solve Equation (4.75) once the temperature history T(i)
is known.
If the polymerization mechanisms and the order of the reaction are known then it may be
straightforward to determine the molecular weight and the gel point explicitly as a function
of the extent of reaction at a single temperature. However, the chemistry is usually complex
and the reactions are taking place at different temperatures as the curing process by nature
is nonisothermal. Hence the order of the reaction is not known and one cannot usually
have a single type of constitutive equation to accommodate the chemical complexity of the
reaction.
Hence, kinetics equations due to complex reactions are strictly empirical. For example,
cure of unsaturated polyesters is fairly well represented by a kinetic equation such as
dC*
= k0exp(-E/RT)(C*)m(l-C*y (4.77)
dt
Since dC*/dt = 0 for C* = 0, one assumes that the resin starts with a small degree of cure,
say C* = 0.0001. One now needs to measure ko and m and n from experiments, where
(m + n) represents the reaction order. There are many other deviations from this type of

reaction. As outlined in [129], one can in general decouple temperature and reaction effects
and express
dC*
— = K(T)/(C*). (4.78)
Here f ( C * ) is the function that describes the rate of reaction in terms of primary con-
stituents and empirical parameters, K is the rate constant denned by the Arrhenius type
of relationship and expressed as
K(T) - A exp(-E/RT) (4.79)
where A is the frequency factor. Different forms are proposed for f ( C * } in the literature.
We will list two of the most common ones used. The first one corresponds to an nth degree
reaction which takes the form
f(C*) = (1 - C*)n. (4.80)
And the second one is related to the autocatalytic reaction as follows:
f ( C * ) = (1 - k2C*}m(l - C*)n (4.81)

in which m + n represents the order of the reaction and k% is described by the Arrhenius
equation.
4.5.1 Techniques to Monitor Cure: Macroscopic Characterization

The widely used method to characterize and validate kinetic models is to experimentally
measure degree of cure as a function of time and temperature. One can monitor this at the
macroscopic and microscopic levels by recording chemical, physical (refractive index [130],
density [131] and viscosity [132]), electrical (electrical resistivity [133, 78]), mechanical and
thermal property changes with time [134, 135]).
Usually a differential scanning calorimeter (DSC) or differential thermal analyzer (DTA)
is employed in both isothermal and dynamic modes. The isothermal scans provide the heat
of reaction, and the dynamic scans yield degree of cure or the extent of reaction as a function
of time at a specific heating rate [136]. A DSC is capable of controlling the temperature
of a small sample of material and of simultaneously measuring the rate of heat flow into or
out of the sample. Curing reactions can be tracked this way because they are exothermic.
Whenever a linkage is formed, a certain amount of chemical energy is converted into heat.
If HR is the total heat of reaction (i.e. calories per gram), then the rate of heat liberated is
dC*
Q = HRM— (4.82)
at
where M is the mass of the sample. Kinetics are best characterized by reacting the sample at
a constant temperature and measuring Q with time. Several runs at different temperatures
are needed to find the temperature dependence.
This is by far the most widely utilized technique to obtain the degree and reaction rate of
cure as well as the specific heat of thermosetting resins. It is based on the measurement of the
differential voltage (converted into heat flow) necessary to obtain the thermal equilibrium
between a sample (resin) and an inert reference, both placed into a calorimeter [137, 138].
As a result, a thermogram, as shown in Figure 4.21 is obtained [139]. In this curve, the
area under the whole curve represents the total heat of reaction, HR, and the shadowed
area represents the enthalpy at a specific time.

(U
D)
C
03
6
>,
a.
ro
W
"o
0
I
Temperature
Figure 4.21: Example of a Thermogram — rate of enthalpy change with temperature [129].
The DSC can operate under isothermal or nonisothermal conditions [140]. In the former
mode, two different methods can be used [141]:
i) A sample is placed into a previously heated calorimeter (faster equilibrium [142]) or
into an unheated calorimeter, whose temperature is raised as quickly as possible up to the
curing temperature.
ii) A sample is cured for various times until no additional curing can be detected; then,
the samples are scanned (heating rate ranging from 2 to 20 °C/min) in order to measure
the residual enthalpy, Hres. The degree of cure is calculated directly,
(4.83)
HR
but not the reaction rate, which is obtained by tangents to the curve of a versus time. For
reactions with very small exothermal heat, this method should be utilized instead of the
first method.
In the nonisothermal or dynamic mode, a sample is set into a calorimeter and the
temperature is raised at a certain constant heating rate up to the operational temperature.
The total heat of reaction is independent of the heating rate (recommended range is 2-
20°C/min [141, 134]). Three methods are possible:
i) All kinetic information (A and E in equation (4.79) can be obtained from only one
experiment. Although this method has been successfully applied for some first order re-
actions, it is not accurate for others; the heat of reaction is higher (around 10-30%) when
compared with the isothermal mode [141].
ii) A and E in equation (4.79) can be accurately measured from the values of the
peak exotherm temperature for various heating rates for all reactions [141]. This is the
recommended method.
iii) More general than the second method, it measures A and E from the values of
the temperature necessary to reach a constant conversion for various heating rates. This
technique needs considerable effort to be moderately successful.
Although many researchers use DSC for measuring enthalpies over the entire curing
process, it is not accurate after the gel point [143, 144, 145].
Several authors have pointed out that the parameters of the reaction rate expression for
isothermal and dynamic conditions may be different [143, 146, 147, 148, 149, 150, 151].
One possible explanation for different results between isothermal and dynamic analysis
was first given by [152], and it is related to the fact that the degree of conversion is a

function of the curing time and temperature. Therefore, we have:
da (da\ i da\ dT ,A OA.
+ (484)
-* = U)T Ud^'
where da/dt represents the dynamic reaction rate, (da/dt)? the isothermal reaction rate
and dT/dt, the heating rate.
According to some authors [134, 147, 149, 152, 153, 154, 155], the isothermal rate in
reality is expressed by equation (4.78). The physical meaning of the term (da/dT)t was
questioned by [156] and [157] as well as [158]. They affirmed that (da/dT)t has to be
zero since if one fixes the time, the positions of all the particles in the system will be
fixed, making a constant. On the other hand, by using thermodynamics, [154] showed that
(da/dT)t exists and is non-zero.
Equation (4.84) can also be recast in a different form:
da (485)
. , 0
where a = dT/dt. For isothermal experiments a=0, and there is no difference between
equations (4.78) and (4.85). But as the dynamic measurements are simpler and faster
than isothermal ones (for the first case, only one experiment is needed to obtain all kinetic
parameters), it is important to calculate the term (da/dT)t in order to acquire a relationship
between dynamic measurements and isothermal parameters.
Other thermal techniques to characterize cure are thermogravimetric analysis (TGA)
[76, 159], high pressure calorimeter (HPC) [141], thermomechanical analysis (TMA) [141,
160] and differential (or dynamic) thermal analysis (DTA) [161]. These are rarely used and
will not be discussed here.
However, we can briefly mention another technique used which is called torsional braid
analysis (TEA). This technique is a variation of torsion pendulum (TP) and was developed
by [162] in 1958. It consists of measuring the frequency and decay constants which charac-
terize each wave resultant of free torsional oscillations (at approximately 1 Hz) subjected
to a sample (a glass braid impregnated with a resin). These measurements are converted
into elastic (stored energy) and loss (loss energy) moduli, which are related to transition
(gelation and vitrification) times and temperatures.
TEA is a sensitive technique for determination of physical changes in the resin [163, 164,
165, 166, 167, 168], occurring at and after the gel point; it has a lower limit of detectability
[141]. TEA is not capable of measuring the degree of cure.
Other mechanical techniques are dynamic mechanical analysis (DMA) [169, 170] and
rheological dynamic spectrometer (RDS) [76, 171, 172, 173].
Due to the fact that there is no accurate technique valid for the entire curing reaction,
two techniques should be used to follow cure: one applied before gelation (DSC) and another
one applied after gelation (TEA, DMA, TMA, d.c. conductivity [174, 175, 176, 177]) .
4.5.2 Technique to Monitor Cure: Microscopic Characterization

During curing there are many reactions occuring simultaneously. DSC tries to capture the
overall reaction rate. However, if one is interested in understanding details of individual
reactions, one must resort to microscopic characterization.
Sophisticated techniques are required to measure the concentration of all components
in order to trace individual reactions occurring during cure. Some examples are Fourier
transform infrared spectrocospy (FT i.r.) [76, 178, 179, 180], solid state nuclear magnetic

resonance (n.m.r.) [181, 182, 183, 184, 185, 186], near infrared spectroscopy (n.i.r.) [187,
188, 189, 190] and chromatography [183, 191].
The spectroscopy methods consist of dispersing radiation from a source and passing it
over a slit system which isolates a narrow frequency range falling on the detector [184].
By using a scanning mechanism, the energy transmitted through a sample as a function of
frequency, known as the spectrum, is obtained and compared with the spectrum character-
istic for each functional group of thermosetting resins. The mid-(m.i.r.) and near-infrared
(n.i.r.) regions of the spectrum can be utilized. Although all functional groups involved in
cure reactions of epoxy resins have strong characteristic absorptions in the m.i.r. region,
the m.i.r. spectra of epoxy resins and hardeners are very complex [190]. The absorption
bands of the main functional groups in cure reactions of epoxies are well-isolated in the
near infrared region of the spectrum (10,000 and 4000 cm"1). A graph of absorbance versus
wavenumber, as shown in Figure 4.22, is generated, presenting peaks correspondent to func-
tional groups, such as epoxide, primary and secondary amines, and hydroxyl. The values
of the absorption bands for these groups can be found in [187, 188, 189, 190].
•eo
10000 7000 4000
Wavenumber (cm 1 )
Figure 4.22: Absorbance as a function of wavenumber. Every peak is characteristic of a

particular group [129].
The basic principle of all these methods is the comparison between the spectrum of refer-
ence substances and spectra of the reactants and products of a curing reaction subjected to
radiation. A qualitative and quantitative identification of the components is then possible.
However, microscopic characterization has not yet being linked to the phenomenological
parameters used in cure-kinetic equations but helps in understanding how the components
react.
4.5.3 Effect of Reinforcements on Cure Kinetics

Usually the resin flows through the fiber reinforcements, and these fibers may be sized and
treated with chemical compounds, such as silane, in order to enhance coupling between the

fiber and matrix phases [192, 193], which may change the kinetics. It is essential to know
to what extent this coupling alters the cure kinetics and thus if it is possible to use the
kinetic parameters from neat resins to describe the kinetics for resin-reinforced materials.
However, there is no consensus with respect to the influence of fillers or reinforced materials
on the cure kinetics. Inorganic fillers are used in thermosetting resins in order to reduce the
cost and the shrinkage and as a heat sink to achieve a better temperature control across
a molded part during cure [194]. Dutta and Ryan [195] analyzed the influence of carbon
black and silica on the cure kinetics of DGEBA/m-phenylenediamine, concluding that the
heat of reaction is independent of the filler content but dependent on the type of filler,
the overall reaction order of the system is not significantly affected, and the reaction rate
changes because of the variations in the rate constants of the autocatalytic model. This
effect is more sensitive at higher temperatures and for carbon black, probably because of
chemical complexities on the carbon black surface [195].
Whereas [196] did not verify any effect of particulate fillers (glass, calcium carbonate
and aluminum) on the reaction kinetics, [194], working with calcium carbonate and clay in
an unsaturaed polyester resin, concluded that the reaction rate increases by increasing the
filler content.
When working with vinyl ester (specifically DERAKANE 411-C50), [92] observed a
drastic influence of the fibers (E-glass) on the induction time (time required for the reaction
to become observable at a specific temperature). An induction time of 90 minutes and 5.5
hours was necessary for RTM runs at 53°C and DSC runs at 50°C, respectively. [197]
affirmed that the age of the resin can also alter the induction time; at 70°C, a reduction
time of 50% was found after 10 months of storage. All these effects are more evident at low
temperatures.
Han et al. [198] found that the rate of cure of a resin is greatly influenced by the pres-
ence of fibers and the type of fibers employed; the rate of reaction for resin/fiber system
can be 60% different from that of neat resin, after a ten-minute cure. A similar conclu-
sion was presented by [199] for graphite/epoxy composites based on TGDDM/DDS; they
verified large differences — see Table 4.6 — in the kinetic parameters when considering an
autocatalytic model.
Table 4.6: Kinetic Parameter Percentage Errors Between Composite and Neat Resin
Graphite Epoxy Composite Ai A2 Eai Eci2 m n

(min"1) (min^1) (J/mol) (J/mol)
1 Composite-Neat Resin . 83.2% 50.3% 5.70% 0.344% 36.0%

' Composite ' 11.1%
It is clear that the surface of reinforcement can affect the kinetics. The disagreement
affects the extent. The type of resin and the temperature range are important considera-
tions. Generally at low temperatures, one must be cautious about applying the neat resin
phenomenological parameters to a system in which the resin will impregnate a network of
fibers.

4.6 Crystallization Kinetics
While one needs to model cure kinetics when processing thermosets, one has to account for
crystallization for thermoplastics as they solidify. Composites that contain thermoplastic
polymers as the binding matrices can be formed or reformed by application of heat to melt
or soften the polymer and stress to shape it. It is then subjected to cooling conditions that
will solidify the polymer. The solidification of thermoplastics, in general, semicrystalline
polymers, and its effect on the resulting microstructure does play an important role in
composites processing and hence, it is useful to model and study their behavior.
4.6.1 Introduction
The term crystallization has its roots in the word crystal, which refers to an ordered arrange-
ment of molecules/units, which can be categorized in a specific way. Thus crystallization
refers to the phenomenon of turning into a crystal. First, it is important to distinguish
between the phenomenon of solidification and crystallization although one uses them as
synonyms. Solidification refers to the transition of a substance from the liquid state to the
solid state; it doesn't require it to solidify into an ordered structure. On the other hand,
crystallization specifically refers to the transition of a body from the liquid state to an or-
dered solid state or a crystalline state. While solidification refers to all substances in general,
crystallization usually refers to long chain structures, such as thermoplastics and proteins
for example. "Crystal" refers to solidified metal structures too, due to their regularity. An
important point to note is that although the term crystalline polymers can be theoretically
defined, it is not physically realizable, since there is always a separate noncrystalline phase.
Hence thermoplastics can be in either an amorphous state (no crystals) or a semicrystalline
state (partial crystallinity). Crystallization evolves either from a solution or from the melt.
These types of crystallization entail different concepts. We restrict ourselves here to only
crystallization from the melt as thermoplastic composites involve processing of melts.
When we consider the crystallization of thermoplastics, the complex nature of their
structure is influenced by the processing conditions. Depending on how the thermoplastic
is cooled, it will either crystallize (slow cooling) or solidify into a glassy state (fast cooling);
unlike a pure metal melt, which will always crystallize. This occurs due to the structure
of polymers, i.e., their chain-like molecules. The ordering of these chains does not occur as
easily as does the ordering of the atoms of a pure metal melt, where they organize them-
selves into a regular lattice (ordered structure/unit) when the thermodynamic conditions
are conducive. Instead, various effects come into play at the micro and the macro level of
the crystallizing molecules, which makes crystallization in the case of polymers not a truly
thermodynamic transition.
4.6.2 Solidification and Crystallization

One may quantify the differences between solidification and crystallization using the concept
of phase transition as well. Phase transition refers to a change occurring between the solid,
liquid and gaseous states, the three fundamental states of matter. When the change from one
state to another occurs at a specific temperature (at a certain pressure), then the transition
is termed a first order transition. More precisely, the transition occurs at the point when
the first derivative of the state functions (volume and enthalpy) exhibits a sudden jump,
i.e., when the first partial derivative of the Gibbs free energy (G) shows a discontinuity. In
explicit terms: dG = Sdt + VdP, hence the entropy, S, and the volume, V, also exhibit a
discontinuity [200].

With polymers there is no transition from the liquid to the gaseous state, as the tem-
perature of decomposition of the polymer is much lower than the temperature required to
separate the molecules; hence, the polymer disintegrates before it can turn into a gas. Also,
for semicrystalline polymers, the solid/liquid transition does not take place abruptly; in-
stead, it occurs over a range of temperatures, i.e., the primary state functions (V, H) change
gradually between the values corresponding to solid and the liquid states [201].
When amorphous (irregular or having no order) solid materials or glasses solidify, the
transition temperature is identified by a change in the second derivative of the primary
state variables such as the Gibbs free energy. Hence the "glass transition" is known as a
second order transition. The phase transition concept is illustrated in Figure 4.23.
>,
Q.
LLJ
Temperature Temperature
o O
4-J~
0!
CD
I
O
tf=
O
CD
Temperature Temperature
fa) (b)
Figure 4.23: Variation of thermodynamic variables with temperature, (a) refers to a semi-
crystalline polymer and (b) refers to an amorphous polymer [200].
4.6.3 Background
The knowledge that a thermoplastic could crystallize was not realized until 1912, when
Von Laue showed that, because of the repetitive character of their lattices, crystals would
scatter a beam of x-rays into regular patterns which were analogous to optical diffraction
patterns [202]. Thus, subsequent work on polymeric materials demonstrated that they
exhibit crystallinity at the level of molecular packing. Thus the next step was to deter-
mine the development and nature of this crystallinity, which to this date is not completely
understood.
The chemical properties of a thermoplastic composite product are dictated by its matrix

material microstructure, hence the need to model and accurately predict the microstruc-
ture evolution of the thermoplastic during its solidification. In semicrystalline polymers,
the solidification conditions have a strong influence on the evolution and the resulting mi-
crostructure [203]. It has been shown that the kinetics of crystallization is the limiting
factor during the growth of crystals from quiescent melts, instead of the growth following a
truly thermodynamic progression. Thus, methods that involve the kinetics are often used
to model and describe the microstructure instead of classical phase change methods (used
to describe the solidification of water, as an example). Several models have been developed
to describe the crystallinity variation with temperature in semicrystalline polymers [204].
But these models require the temperature profile in order to calculate the crystallinity and
various schemes have been developed to couple these models with conservation of energy
equation for the composite.
4.6.4 Crystalline Structure

It has been shown that crystallization of thermoplastics occurs by the stacking up of indi-
vidual polymer chains side by side to form a crystal lattice or by the physical phenomenon
of the folding of polymer chains. This is shown schematically in Figure 4.24. Polymer chains
fold back upon themselves to form a crystal called a lamella. Stacks of lamellae connected
by regions of amorphous material or interlamellar links make up a semicrystalline polymer.
Figure 4.24: Polymeric chains forming a crystal [202].
The crystallization from the melt is also referred to as bulk crystallization, as the move-
ment of chains is hindered by other chains in their path and also by crystallized areas in the
bulk. Crystallization in the melt or bulk occurs by the formation of crystals in the radial
direction from a central nucleus, also known as spherulites. A schematic of a spherulite is
The formation of spherulites is described by the phenomenological theory first proposed
by [205]. They theorized that in order for growth of a spherulite to take place, two conditions
must be met: the medium must have a high viscosity, and noncrystallizable material (or

Figure 4.25: Schematic of a spherulite showing lamellae [201].
solute) must be present. Similar to solidification of metals, the solute is rejected from the
crystallizing solid and pushed ahead of the solidifying interface, and is assumed to promote
the instability of the solid/liquid interface. They suggested that branches of the spherulite
penetrate into the melt and grow preferentially in regions rich in crystallizable material.
Initially, the nucleation process must occur in order for the polymer chains to attach
themselves to the nuclei and facilitate growth of the crystal. Then nucleation and growth
occur together for a certain amount of time, which is followed by a free growth phase of
the spherulites. Free growth continues until the spherulites impinge on each other, and
the process of secondary crystallization takes place. Secondary crystallization refers to
the attachment of chains on a smooth surface of the crystal, where previously no growth
occurred. It is much slower compared to primary crystallization because the polymer chains
are not able to find nuclei to attach themselves to, and they are also hindered from diffusing
to other favorable growth sites. Finally, after crystallization is complete, the body cools
down to the ambient temperature by convection [206].
One can address the crystallization kinetics on two scales that are coupled. At the
microscopic scale, one needs to model the nucleation and growth of a spherulite and on a
macroscopic scale one needs to determine the overall crystallinity behavior of the polymer.
It is obvious that changes at the microscopic level will influence the macroscopic constitutive
equation.
4.6.5 Spherulitic Growth
Spherulitic growth is still not fully understood, but it has been shown that their radii often
grow linearly with time under isothermal conditions, which supports a kinetics controlled
growth theory [206, 207, 208].
The growth of the tips of the branches of a spherulite follows the kinetics of attachment
of polymer chains given by the Lauritzen and Hoffman theory [209, 210]. Thus, the growth

rate of the crystal can be represented by [206]:
dR,'9 _ -U*
= GO exp exp (4.86)
dt R(T - TAT/
Here, the first exponential term represents the temperature dependence of the segmental
jump rate in the polymer; the second term is the contribution from the net rate of secondary
nuclei formation on the surface of a lamella. Rg is the grain radius, U* is the activation
energy, R is the universal gas constant, and T^ is the temperature at which all motion
associated with viscous flow cease. Kg is a constant related to the growth regime and is
specific to a particular regime, / is a correction factor that accounts for the change in
value of the heat of fusion at low temperatures (close to T g ), and AT is the undercool-
ing. Undercooling is defined here as the difference between the melting temperature and
the crystallization temperature. GO is a pre-exponential constant that gathers terms not
strongly dependent on the temperature and has different values corresponding to the dif-
ferent regimes of crystallization. Table 4.7 lists the kinetic, thermodynamic and material
properties for polyethylene.
Table 4.7: Properties for Polyethylene [206].

Kinetic Data
Kg (K) 2 - 2 x 105
GO (cm/s) = 4.4 x 109
U* (cal/mole) = 1500
Thermodynamic and Thermal Data
Too - 201 (C)
= Tm-Tg = 417.8 - 231 (C)
4.6.6 Macroscopic Crystallization

On the macroscopic level, one can develop useful constitutive equations to describe isother-
mal and nonisothermal crystallization. Isothermal crystallization refers to the phenomenon
when the spherulite growth process is steady; i.e., the degree of crystallinity (x) is indepen-
dent of the temperature [211, 212]. Explicitly stated:
X = 1 - exp (-BF (4.87)
where B is a time-dependent scaling parameter related to the half-time of crystallization,

ti/i and depends on the temperature, and n is the Avrami exponent. This equation is
commonly known as the Avrami equation of crystallization. Non-isothermal crystallization
on the other hand refers to temperature-dependent crystallization kinetics. Modeling of
this process has led to a temperature-dependent expression for x, which is more complex
than that given by Equation (4.87) and follows from a modified model proposed for this
purpose, the Nakamura model [206]:
I
= nK(T)(l-X)ln (4.88)
dt

where n is the kinetics parameter and K(T) is related to the crystallization rate constant
of isothermal crystallization, k ( T ) , by
K(T] = k(T)l'n. (4.89)
The models for nonisothermal crystallization more accurately describe experimental data
collected on the crystallization of various thermoplastics.
The constants don't have a physical meaning and cannot be easily connected to the
microscopic analysis. However, the constants can be easily determined through differential
scanning calorimetric (DSC) experiments, and no induction time (the time required for the
organization of molecules around a nucleus) factor is necessary. DSC is a technique used
to determine thermal transition points of various substances. The evolution of the absolute
crystallinity profile within a part during cooling can be predicted by coupling the model
with a heat transfer analysis [203]. This is done by representing the source term in the
energy balance equation by pcpHrdx/dt which tracks the heat evolved during solidification.
4.7 Permeability
Permeability characterizes the ease with which a fluid can flow through a porous medium.
In almost all composite processes that use a thermoset resin as the matrix material, the
resin has to be either infused into a fiber preform in processes such as liquid molding or
extracted out during consolidation as in autoclave processing. This motion of the resin is
usually modeled as flow through a porous medium in which the fiber network constitutes
the porous medium. The empirical Darcy's law [213] governs the flow of the resin as follows:
Q = ^ . (1.90)
Here Q is the flow rate across the cross section A, T] is the viscosity of the liquid, dP/dx is
the driving pressure gradient and K is the permeability of the porous medium.
This law allows the modelers to describe a macroscopic relationship between the flow
rate and the pressure gradient needed to drive the flow instead of using the momentum
conservation equations. If one wanted to use the momentum equations, one would have
to describe the geometry of every channel present in the fibrous network and solve the
momentum equations inside them to find the flow rate and pressure inside these channels.
There can be a network of over a million channels created by the arrangement of the fibers.
This task would be impossible to approach even with a sophisticated computer, and more
importantly we only need to know the overall relationship between the pressure drop and
the flow rate and not the details of the pressure at each and every location within every
channel while processing such materials. Thus, Darcy's law lumps the ease of flow within
these channels into a parameter called permeability which characterizes the mobility of the
resin through the fibrous porous media.
Permeability is a function of fiber network, fiber volume fraction and also the type of
sizing applied to the fibers. Also, as the porous medium formed by the fibrous network
will be anisotropic (it will offer different resistances in different directions) , the practice has
converged on generalization of Darcy's law to account for it:
u=-—-VP (4.91)
77

Resin velocity profile \
Volume averaged Darcy's velocity
Figure 4.26: Volume averaged Darcy velocity within a porous medium.
where u is the volume averaged "Darcy velocity" (see Figure 4.26), r\ is the viscosity of the
fluid, VP is the pressure gradient, and K is the permeability tensor of the preform. Here,
K is now a tensor instead of a scalar and can be represented as
K= "•yy K-yz (4.92)

Kzx Kzy Kz
and the three-dimensional form of Darcy's law is expressed in matrix form as follows:
Kxy Kxz dP/dx

= --! K,, Kyy Kyz dP/dy (4.93)
f\ &zy -K-zz dP/dz
The Darcy's law that now substitutes the momentum equations can be written down in
three directions as follows (by using Cartesian coordinates):
K^d_P_ _ K^d^ KxzdP
(4.94)
T) dx 77 dy r) dz '
KyxdP _ KyydP _ KyzdP
(4.95)
TI dx TI dy rj dz '
Kzx dP Kzy dP Kzz dP
(4.96)
T] dx rj dy TI dz'

Thus, for a given stationary porous medium of a fiber preform, one needs to know six scalar
values (assuming that K{j — Kji) to determine the full permeability tensor.
However if the selected coordinate direction is along the principal directions of the
preform as illustrated for a two-dimensional case (where the direction 3 is normal to 1,2
plane), in Figure 4.27 then Equation (4.93) can be simplified to
Ku 0 0 \ / dP/dxi \
0 #22 0 dP/dx-2 . (4.97)
0 0 K33 ) \ dP/dx3 )
Here, the local principal coordinate system X i , x % , x 3 is along the principal axes of the
preform which coincides with the major and minor axes of the ellipsoid formed by the resin
volume injected as shown in Figure 4.27. Thus, by choosing the coordinate directions along
Figure 4.27: Local in-plane principal axes in the plane of a preform along the major and
minor axes of the ellipsoid formed by the injected resin volume.
the principal axes of the fiber preform, one can measure the principal permeability values of
the preform. Then by coordinate transformation, one can calculate the non-diagonal values
if one knows the flow direction with respect to the principal permeability direction.
Example 4.5: Coordinate Transformation [214]

One-dimensional injection of resin through a preform is shown in Figure 4.28. The resin
moves from left to right, and the flow front is a straight line. This can be achieved by
having a point injection gate inside an air channel between the preform and the mold

>• Flow direction along x\
Figure 4.28: Coordinate axes (x[, £ 2 ) and principal axes (x\, x2) of the preform. One
dimensional resin flow from left to right.
cavity wall. Resin fills this section first due to negligible resistance to the flow. The
significant flow through the preform starts after this air channel is filled. Note that no
significant racetracking channel should exist between the preform and horizontal mold walls
(see Figures 8.22, 8.23, and 8.24 for definition of racetracking). Consider the two coordinate
systems: (i) the principal axes x'y', and (ii) mold axes xy. The two-dimensional (in-plane)
permeability tensor is given by
Kn 0
(4.98)
0 K22
if x\ is along x\ and x'2 is along x2 . However, if x'x is at an angle 6 to the principal x\
axis, then the components of the permeability tensor in the x'y' frame can be calculated by
tensor transformation
L
n K(12 (4.99)
where
K22 = Ku sin2 9 + K22 cos2 9 (4.101)

K{2 = K21 = (- + #22) sin (9 cos 6>. (4.102)
Thus, if one knows K22 and 9, one can find the permeability tensor in any new
coordinate frame.
How can you find KH and K22 if 9 was not known a priori?
Solution
The one-dimensional experiment shown in Figure 4.28 will allow one to relate flow rate to
pressure drop as follows:
dP dP (4.103)

u'2 = — [K[2—r + K22—T } = ° ( no now in 2/ direction). (4.104)
77 V ox^ ox2J
Equation (4.104) can be rearranged to yield
K(12
(4.105)
\dx(J
Equation (4.103) is divided by dP/dx^, which results in the following expression:
, dx'
(4.106)
dx' dx'
Substitute Equation (4.105) in Equation (4.106) to get
12
1
- (4.107)
Now using Equations (4.100)-(4.102), we can write Equation (4.107) as follows:
= KU cos 9 (4.108)
dP\
+1
WJ tan2 9
where /3 — K^/Kn- u'i and dP/dx'^ can be measured accurately only if the ratio of
Kii/Kyz is small or if K\i is small. Three experiments should be carried out at angles 9,
9 + A#i and 9 + A$2 where A$i and A$2 are two distinct and known angles such as 15 and
30 degrees, respectively. This will change the right hand side and now we will have three
equations and three unknowns to solve for 6, KU and K^ for a given preform [214]. •
4.7.1 Permeability and Preform Parameters

In all liquid molding processes we need to know the value of permeability in order to predict
the flow behavior of the resin as it impregnates the preform. In processes such as autoclave
molding, thermoset pultrusion and filament winding, an estimate of permeability will allow
one to predict the resin pressure. If the resin pressure is low, insufficient consolidation could
occur and lead to growth of microvoids. Permeability is a function of fiber architecture that
characterizes the channel network. As the fibers usually govern the mechanical properties,
it is advantageous to increase the fiber volume fraction in the composite. One approach
to increase fiber volume fraction is to apply a force on the network of fiber preforms and
compress them. As this network is compressed it blocks or constricts many channels of the

porous medium and thus reduces the mobility of resin flow or the permeability. This reduc-
tion of permeability with fiber volume fraction needs to be characterized as it plays a very
important role in processing. Many constitutive models that use the physics of lubrication
flow or flow through capillary tubes have been developed to describe this relationship. The
earliest one was known as the Carmen-Kozeny equation and was developed by adopting the
capillary model from the soil mechanics literature. It may be expressed as follows:
~ (4.109)
where Vf is the fiber volume fraction and K is the principal permeability component in the
flow direction. The constant A is supposed to be a function of the fiber network. However,
it was found that one needed a different value of A for the same network at different fiber
volume fractions. Also for flow across an aligned bed of fibers, once all the fibers touch each
other one would expect the permeability to be zero in that direction. However, the model
was not able to capture that physics either. More constitutive equations were developed by
[215, 216] to explain some of these shortcomings.
Bruschke and Advani [216] found that one could use lubrication theory and the cell model
concept to describe permeability across an array of fibers more accurately as a function of
fiber volume fraction
K
where L2 = 4V//7T, and r is the radius of a fiber. Note that no empirical parameters were
needed.
Gebart [215] used similar logic to develop principal permeability values as a function
of fiber volume fraction in both along the fiber direction and perpendicular to the fiber
direction:
K
\\ = |r (l ~v^ (4 m)
-
5/2
(4.112)
In all cases, one finds that permeability of the preform decreases as fiber volume fraction
is increased. This results in reduced empty space between the fibers; hence, the resin will
face more resistance to impregnating this preform. However, there is no universal formula
for the relation between the preform permeability and the fiber volume fraction. This
relation is mainly a function of fabric type (i.e., whether it is a glass or carbon) and fabric
structure (i.e., whether it is stitched, woven, random, etc.). A typical graph showing the
change in permeability with fiber volume fraction is shown in Figure 4.29 for a plain weave
glass fabric. Furthermore, the detailed structure of a preform is different depending on
whether it is draped over a tool surface with double curvature and/or whether it has some
nesting and racetracking channels. All these changes will affect the permeability.
4.7.2 Analytic and Numerical Characterization of Permeability

Closed form expressions for the permeability as a function of the fiber diameter, fiber
arrangement, and fiber volume fraction have been developed by adopting the capillary model

1 E-09 • -
1 E-10 - -
Fiber volume fraction, Vf
Figure 4.29: A typical graph showing the change in permeability with fiber volume fraction
for a plain weave.
from the soil mechanics literature, and by using an analogy of flow along and across an array
of cylindrical tubes. However, as none of these idealized geometric arrangements resemble
the preform geometries realistically, computational approaches to solve for the flow/pressure
drop relationship in a unit cell with periodic boundary conditions offer the possibility of
extending the calculations to find the permeability of complicated fiber arrangements as
shown in Figure 4.30 [217, 218, 219, 220, 221]. However, these approaches do not comment
on the unresolved issues of the influence of surface tension [222], fiber wetting, and void
entrapment on permeability predictions. Also nesting of fabrics can influence the perme-
ability, shown in Figure 4.31, as can the addition of binders and stitches that hold the
fabrics together, hence the need to express the permeability and its relationship to fiber
volume fraction and the preform type empirically.
Since it is impractical to solve for the detailed flow field in the interstices between
the medium particles, the basic assumption to formulate a predictive analytic model for
permeability is that the porous medium is homogeneous, and one expects to find a repetitive
arrangement of the idealized geometry of the pore structure. This repetitive arrangement
is also called a unit cell. All approaches assume that Darcy's law holds on a macroscopic
level, and by choosing a geometry that closely resembles the repetitive fiber arrangement
a relationship between the flow rate and the pressure drop in the selected geometry of the
unit cell may be calculated. By comparing it to Darcy's law, one is able to formulate
an expression for the permeability in terms of the parameters of the selected geometry.
This approach can improve one's understanding of the flow through small gaps and help
develop a more science-based constitutive relationship between the preform permeability
and compaction of the preform.
4.7.3 Experimental Characterization of Permeability

Permeability has the units of either cm2 or m2. In 1856, Darcy had a column of sand as
shown in the Figure 4.32 that was subjected to a constant pressure gradient of water, and
he measured the flow rate of the water [213]. Knowing the viscosity of water, he calculated

Figure 4.30: Magnified unit cell of a 4 x 5 weave fabric for permeability predictions [219].
Figure 4.31: Modeling permeability of more than one fabric layer [223].

the permeability of the sand bed by using the following simple equation:
K= Q (4.113)
AP/L
The porous medium was considered isotropic so one needed just one value of permeability
for a given architecture of the porous media.
3.5m
Figure 4.32: A column of sand that was used by Darcy in 1856 in order to measure the
permeability of sand [213].
Fiber preforms offer different resistances in different directions due to their architecture.
Hence, one needs to find the complete permeability tensor for such preforms. Three different
methods have been developed to measure permeability of fiber preforms. They are one-
dimensional linear flow, two-dimensional radial flow and three-dimensional hemispherical
flow. In all the experiments, one needs a flow rate measurement method and a pressure
drop measurement device. The one-dimensional experiment is the easiest to comprehend.
By guiding the flow along one of the principal axes of the preform, one can determine the
permeability by monitoring the flow rate and the pressure drop, as shown in Figure 4.33(a).
The pitfalls to watch out are racetracking along the edges and bending of the mold plates
(which makes the fiber volume fraction of the preform uneven).
While one-dimensional flow is from a line source as seen in Figure 4.33(a), two-dimensional
flow is usually a radial flow from a point source. The shape of the ellipse and the direction
of its major and minor axes allows one to determine the in-plane permeabilities as shown in
Figure 4.33(b). However, one needs to conduct some analysis to calculate these values. De-
tails are given in the book chapter by [214]. Three-dimensional permeabilities can be found
in a similar way by using a point source as shown in Figure 4.34. The details are given in
[223, 224]. Two- and three-dimensional measurements usually require recording of how the
flow front moves with time. This could be accomplished by video taping the experiment in
plane using a transparent mold or digitizing the flow front or using a SMARTWeave sensor
system [225] to extract information about the flow front in three dimensions.

Figure 4.33: Experimental set-ups for preform permeability measurements under (a) one-
dimensional, and (b) two-dimensional radial injection -[226].
Side view
% IfcMh^v^t'^x "«. ^^-&.WA*%t<
^/i **
'' i
Bottom view Top view

Figure 4.34: Side, bottom and top view of three-dimensional permeability measurement
set-up [227].

Permeability measurements are usually not very accurate or repeatable. Ten to twenty
percent error in measurements is common for the same preform in the same laboratory. The
results could differ by as much as 50% from one controlled laboratory to another. More
analytic and numerical predictions need to be coupled with experimental measurements to
get a better handle on values of permeabilities of fiber preforms. Coupled with this issue
is that the woven and stitched preforms exhibit two different length scales in the preforms,
one of the order of fiber diameter in microns and the other of the order of fiber tows in
millimeters. Thus, one is trying to assign a single permeability value for a dual scale porous
medium, and this may not be the correct approach. The solution may be to have two
different permeability values for the two different scales [228, 229].
4.8 Fiber Stress

Fiber stress influences processing. However, how one models this contribution is a function
of the type of resin and whether it contains short or continuous fibers. If the fibers are
short, the contribution of fiber stress appears in enhancement of the viscosity of the resin
as expressed by Equations (4.67) or (4.68). For thermoplastic materials containing long
continuous fibers, the approach is similar where the fiber and the resin are treated as one
material with their combined rheology treated as a continuum and defined by a constitutive
equation, as discussed in Section 4.3. However, for thermoset materials in which the fiber
beds are subjected to loadings and resin then impregnated, one needs to be able to define
the relationship between stress and compression in such fiber networks.
Advanced composites use very high fiber volume fractions. Consequently, the interfiber
spacing is very small (of the order of microns), which leads to multiple fiber-fiber contacts
when consolidation forces are applied during processing.
Some examples of processing geometries are shown in Figure 4.35. They clearly show
that the fiber bundles and the preforms may be subjected to complex three-dimensional
stress during processing. For example, when fiber bundles are under tension in processes
such as filament winding or pultrusion, their fiber volume fraction increases, reducing their
permeability. In molding, the transverse compression will play a key role.
Almost all advanced composites contain fibers in bundles that are woven, stitched or
arranged in the desired form by some other means. As the interest is in the average behavior
of the fiber bundle, it is treated as a continuum because a section of a fiber bundle is much
smaller than the overall dimensions of the composite. As shown in [6], one can denote the
stresses on a fiber bundle element in a material coordinate system as shown in Figure 4.36.
The stresses are carried either by the fibers or by the pressure in the resin as shown in
Equation (4.114)
Tij = Tij - prSij + (Tij (4.114)
Here <5jj is the Kronecker delta, where 8ij = 1 when i = j and zero otherwise. The stresses
carried by the fibers are represented by <Jij and are due to elastic deformation stresses. The
viscous stresses arise due to the viscous deformation of the material and can be represented
by the stress tensor in the fluid as shown in Chapter 3 (T^ = rfjij}. The elastic deformation
stresses can be further subdivided into an axial stress and a bulk stress. The axial stress
is along the fiber direction, and the bulk stress is usually the compressive transfer stress in
the 2-3 plane. The axial stress can be positive or negative, but the bulk stress is always
compressive (negative).
The axial behavior of a fiber bundle is important during processes such as making of a
prepreg, filament winding and pultrusion. When one applies an axial force or tension to a
fiber bundle, Gutowski proposed a nonlinear relationship between the force and the fiber

Compression Molding Pultrusion
On-line Consolidation Vacuum Bagging
Figure 4.35: Examples of geometries in which fibers are compressed during processing [6].
Figure 4.36: Stresses on a fiber bundle element.

volume fraction [230] as shown in Equation (4.115):
A0V0
(4.115)
Vf
where modulus E represents the bending stiffness of the fibers, VQ is the volume fraction
under zero stress, Va is the maximum volume fraction that can be achieved, and j3 is
a constant that defines the state of the bundles. AQ is the initial cross-sectional area
across which the load is applied. This relationship is plotted in Figure 4.37. It shows how
tensioning of the fiber bundle increases the fiber volume fraction.
Figure 4.37: an versus Vf for various Va values [6].
In many other composites manufacturing processes bulk compressive stresses are applied
to the fiber bundle. For example in autoclave processing, one can derive the relationship
between the bulk stress azz and the fiber volume fraction as shown in Equation (4.116). The
plot reveals the rapid load transfer from the resin to the fibers during processing. Lower
resin pressure can promote the growth of the initiated voids, which is detrimental to the
composite.
lvf
3TTE
a-,-, = (4.116)
Note that the above two equations are derived but are based on the assumption that
the fibers are aligned inside a tow and make multiple contacts and have a slight waviness

of a sinusoidal character. This is then translated to a deformation of a slightly curved
fiber in a cell that has a length of 100 times that of the fiber arch as shown in Figure
4.38. The slopes at the end are assumed to be zero. Thus, although based on some of the
physics of continuum mechanics, this equation still requires one to find the constant j3 in
Equations (4.115) and (4.116) by conducting experiments at different fiber volume fractions
and matching the results with the model results.
h\
Figure 4.38: Deformation of a slightly curved fiber in a cell (redrawn from [6]).
Recently, Chou and Chen have addressed the compaction of woven and stitched fabrics.
They have adopted a unit cell approach to develop the stress and compaction relationship
and also allow for nesting of the fabric [231, 232, 233]. This compaction of fabrics and
nesting effects also influence the flow of resin as the permeability of the preforms change.
See [234] for more details.
4.9 Exercises
4.9.1 Questions
1. Why do we need constitutive laws?
2. What is the viscosity of a fluid?
3. What are the dimensions of viscosity in terms of mass (M), length (L) and time (T)?
4. What are the three common constitutive models for viscosity of shear thinning ma-
terials, such as thermoplastics? Sketch typical viscosity versus shear rate profiles for
these three models as well as for a Newtonian material.
5. What is the mathematical expression for the magnitude of the strain rate tensor?
6. What are the two common devices used to measure the viscosity of fluids?
7. For shear thinning materials at low and high shear rates, the power-law model gives
physically incorrect values of viscosity whereas the Carreau model correctly captures

the -behavior of the materials. However, the power-law is commonly used. Explain
the reason.
8. What device is used to measure the viscosity of long discontinues fiber reinforced
composites in their melt state?
9. What process variables are dependent on the viscosity of a short fiber suspension in
processes such as injection molding, extrusion and compression molding?
10. Does the viscosity of a fiber suspension have the same or different values in (i) steady
uniaxial elongation flow, and (ii) steady simple shear flow? Explain.
11. If the fibers are initially random, does the viscosity of a fiber suspension have the
same or different values in (i) unsteady simple shear flow, and (ii) steady simple shear
flow? Explain.
12. Why is a cure model of a resin system needed? Which process parameters and vari-
ables are designed using this model?
13. What is the "gel point" of a resin system? What happens if the composite part is
de-molded before the gel point? What is the disadvantage of demoding the part much
later than the gel point?
14. What is the differential scanning calorimeter (DSC) technique?
15. Describe the two commonly used methods of DSC under isothermal conditions. Which
one of these methods should be utilized for reactions with very small exotherm heat?
16. Describe the three commonly used methods of DSC under nonisothermal conditions
(dynamic mode) by discussing whether a single or multiple experiments are needed,
and what different values are measured in those methods. Which one of these methods
should be utilized in order to get reliable results?
17. Suppose that there are two experimental setups available in your laboratory for the
measurement of degree of cure during resin systems for the entire cure cycle: DSC
(differential scanning calorimeter) and TEA (torsional braid analysis). Which one
would you use? Or would you use both of them for different stages of the cure
reaction? Explain.
18. What are the reasons for using inorganic fillers in thermosetting resins?
19. Suppose that you run two sets of experiments to measure the rate of cure of (i) a
resin alone and (ii) a resin with the presence of fibers. Would you expect a significant
variation in the results, or not?
20. What is the difference between solidification and crystallization?
21. Sketch the graphs of (i) enthalpy versus temperature and (ii) specific heat versus
temperature, during the phase change for both a semicrystalline polymer and an
amorphous polymer.
22. What are lamellae?
23. Describe the formation of spherulites.

24. Describe the primary and secondary crystallizations.
25. What does the permeability of a porous medium mean? If a fabric preform is assumed
to be a porous medium, then what affects the permeability of the preform?
26. Write down one-dimensional Darcy's law. Explain each term. What are the dimen-
sions of each term.
27. Write down three-dimensional Darcy's law. What do principal axes physically denote?
Rewrite three-dimensional Darcy's law using the directions of principal axes.
28. What is the difference between isotropic and anisotropic porous madia in terms of (i)
the permeability tensor and (ii) the flow of a resin through these media?
29. Visually how do you find the principal axes of permeability tensor of a reinforcing
preform during its impregnation with a resin?
30. Is there a unique set of principal axes of permeability tensor for a reinforcing preform?
Explain.
31. One student writes the following on his/her lab report: "My supervisor asked me
to measure the permeability of a preform with 10 layers of fabric 'X' which has 4
and 5 tows per inch in the warp and weft directions, respectively. I measured the
permeability of a single layer fabric as 4.0 * 10~9 m2 by using a single one-dimensional
experiment. Then, I stacked 10 layers of this fabric and placed them inside a mold
with varying thickness. I injected resin from a gate. My experimental results (flow
front shape and injection flow rate under constant injection pressure) deviated very
significantly from the mold filling simulation results in which I used Kxx = Kyy =
4.0 * 10~9 m 2 . I wonder what I did wrong." Can you help him/her? As a supervisor,
what additional work would you ask the student to do?
32. Describe the commonly used constitutive equations for the permeability K of a porous
layer when a viscous fluid flows through it. Do they accurately represent typical fabric
preforms?
33. The advantage of constitutive equations for the permeability of porous layers is that
they have simple closed-form solutions. Are there any shortcomings?
34. What is the "unit cell" method in calculation of permeability of a fabric preform?
What are the assumptions? What are the applied boundary conditions?
35. Explain how Darcy measured the permeability of a sand bed for the first time in 1856.
36. What are the different methods to measure the permeability of preforms? What are
their advantages and disadvantages compared to other methods?
37. Suppose that you are given an isotropic fabric preform and you are asked to mea-
sure the in-plane components of the permeability tensor at a specified and uniform
fiber volume fraction. Explain your procedure if your laboratory has (i) only a one-
dimensional experimental setup, or (ii) a two-dimensional experimental setup?
38. Explain the reasons why the values of permeability measurements have big variations
from one laboratory to another, and from one experiment to another in the same
laboratory.

39. Describe the three-dimensional permeability measurement method. For what ap-
plications is the three-dimensional permeability tensor needed instead of the usual
two-dimensional?
40. What causes the fiber stresses in composite manufacturing processes? Are these effects
the same or different in processes such as compression molding, RTM, filament winding
and pultrusion?
41. Describe how the fiber stress is shared between the resin and the fiber preform during
autoclave processing.
4.9.2 Fill in the blanks

1. Commonly used units of viscosity are Poise (P), centiPoise (cP), and Pascal-times-
second (Pa.s). The relations between them are given as follows: 1 P = cP, 1
P= Pa.s.
2. Water, corn syrup, liquid metals and other short chain molecules are called
fluids because the viscosity of such fluids can be characterized by a single value which
does not change with its rate.
3. In general the viscosity is a function of , , ,
rate, and if there are particles or fibers suspended in the resin then the
fraction and of the particles if their aspect ratio is greater
than one.
4. As thermosets cure, their viscosity as one would need more force to move
a molecule that is Thus, equations to describe the cure
kinetics and dependence of viscosity on degree of cure are necessary for thermosets.
Before the initiation of the cure, viscosities of thermosets are usually between
cP and cP.
5. Most of the polymer composite processing and manufacturing methods are modeled
using the Reynolds number flow assumption or flow as-
sumption, in which one neglects the force in favor of the
force.
6. The resistance to flow can dramatically decrease due to the change in the structure
under applied shear load reducing the viscosity by orders of magnitude. Such liquids
are known as shear fluids, where the viscosity with shear
rate.
7. Thermoplastics belong to a class of fluids.
8. One checks the Deborah number (De) to gauge the importance of viscoelasticity. De
is the ratio of effects to effects. If De -C 1, one can safely
ignore the effects of the thermoplastic polymer.
9. The viscosity of thermoplastics will usually decrease by one to two orders of magnitude
as the temperature of the material increases from the temperature to a
few degrees higher than the temperature.

10. The relationship between the stress tensor of a material r_ and the strain rate tensor
of that material 7 is given as j_ = 777 where rj is the viscosity of the material. For a
Newtonian fluid, the viscosity is a and can be expressed as r] =
11. For shear thinning materials, such as thermoplastics, the change in viscosity with
shear rate is expressed with one of the three commonly used phenomenological models.
These models are called the power-law model, truncated model, and the
model. In the power-law model, 77(7) = where m and n are
material constants of the resin system and determined experimentally.
12. For Newtonian fluids, the value of the viscosity should be at different
shear rates.
13. is usually a suitable device for viscosity measurement at low shear
rate. is suitable to measure viscosity at high shear rates.
14. Almost all of the thermoplastics display a at low shear rates, and
then a with the increase in shear rate and again a
at the high shear rates.
15. The shear and extensional properties of long discontinuous fiber reinforced composites
in their melt state are difficult to obtain using traditional rheological techniques such
as cone and plate and capillary rheometers due to the presence of continuous or long
fibers. One way to characterize their shear behavior is to use flow to
characterize the bulk transverse shear viscosity of these highly filled viscous resin sys-
tems. This flow is invoked by placing the material between two impermeable platens
and applying a normal force. One may characterize the material under constant ap-
plied or under a constant rate of the platens. Such
industrial testing devices are referred to as the " " or " "
16. For transversely isotropic bundle or laminates, the two dominant shear modes are
shearing and shearing.
17. Experimental squeeze flow studies on polymeric liquids indicate that under slow load-
ing rates, their behavior can be well approximated through the shear dependent vis-
cosity. However, under rapid loading, viscoelastic effects may become evident. The
magnitude of the material's Deborah number (De) is often used as a determinant of
its response. De is defined as the ratio of the fluid's time to a charac-
teristic time of the squeezing process. Low values of De correspond to
fluids while high De corresponds to fluids with an response.
18. Fibers in a suspension can be approximated as uniform cylindrical rods with a length
L and diameter D. The number density of the suspension, n is the number of fibers
per unit volume. There are three regimes: dilute, semi-dilute and concentrated. The
suspension is dilute if n is much less than The suspension is concen-
trated if n is greater than If n is between these two values, then the
suspension is said to be in the semi-dilute regime.
19. All commercial composites fall into the regime.
20. The most important action of a fiber in a suspension is to resist stretching of the
fluid along the axis. All fiber suspensions have high viscosities for
stretching in the direction.

21. Fibers add very resistance to a shearing motion either parallel or per-
pendicular to the fiber axis. Shearing flow tends to make the fibers align
to the planes of shear, where they exert resistance to the deformation.
As a result, fiber suspensions have much viscosities in steady simple
shear than in steady uniaxial elongation.
22. The curing reaction of thermoset resins forms a three-dimensional cross-linked net-
work. The reaction can be activated either (i) thermally by heating up the
or (ii) chemically by the addition of
23. The degree of cure is usually proportional to the fraction of the
The reaction is an one, so the evolved needs to be con-
vected out of the composite.
24. Modeling of resin cure and heat transfer between the mold and composite allows
the engineer to predict the history of the composite during manufac-
turing and to design appropriate and cycles for the
material. If an appropriate system is not designed, the polymer can
due to the excess heat generated by the reaction.
25. When a pure metal melt is cooled it always crystallizes. When a thermoplastic is
cooled it either (i) crystallizes, or (ii) solidifies into a glassy state, depending on
whether the cooling is or , respectively.
26. The two-dimensional flow of resin that is injected from a point source to impregnate
a fabric preform, will have or flow front shapes if the
preform permeability tensor is isotropic or anisotropic, respectively.
4.9.3 Problems
1. The following empirical equation was proposed by [88, 89, 90] for the viscosity of a
thermoset resin system:
NQ+6a
(E^f aa
= A exp
" « (Rr)(^t
where the constants of the equation are listed in Table 4.2. (i) For RIM2200 resin,
plot 77 as a function of T, 30 < T < 90 for three different values of degree of cure,
a — 0, 0.05 and 0.10. (ii) Repeat (i) except that the resin is commercial DSM resin,
and temperature domain is 30 < T < 60. (iii) Repeat (i) except that the resin is
DGEBA and TETA resin, and the temperature domain is in 70 < T < 90.
2. Consider the reaction between two chemical groups denoted by A and B which link
together two segments of polymer chain PI and P% as follows: PiA + PaB = PiABP2-
The kinetic equation is ^ = k0 exp (~E/RT)CAO(l - C*)(A - C*) where C* =
A
^~ A and A = CBO/GAO- Plot C*(t) if the rate constant fco = 4, the ratio of
activation energy for the reaction E to the universal gas constant R is E/R = 250,
the temperature of the polymer is held constant at T = 450K, A = 1, and the initial
concentration is CAO = 0.4, How long does it take for C* to reach values of 0.5 and
0.99? How do the results change if the temperature is increased to 500K?

3. Write the Kozeny-Carman equation for the permeability of a capillary tube arrange-
ment. Is this equation valid for the flow along or across a set of parallel capillary
tube arrangement? Plot K/A versus Vf when 0.50 <V/< 0.80 by assuming that the
coefficient A in this equation doesn't change with the fiber volume fraction. In this
model, what is the upper limit of Vf when the capillary tubes are arranged so that
they touch each other? At this critical value of Vf, what does the Kozeny-Carman
equation predict for K? What would you expect K to be at this critical Vf? What
are the reasons for this deviation?
4. One decides to use the Kozeny-Carman equation for a nominal fiber volume fraction
of Vf = 0.5. If Vf has a tolerance of ±0.01, what is the corresponding tolerance on
K?
5. What is Darcy velocity? Write an equation to calculate the Darcy velocity by using
the local velocity profile u(y] of a one-dimensional flow along x direction within a
channel of height h.
6. A resin is injected into a preform. The permeability tensor of the preform is given as
**• x
K * 10-10m2.
(i) Calculate the principal permeability components K\\ and Kyi- (ii) Draw the x-
y and 1-2 coordinate systems, and indicate the angle between the two coordinate
systems, (iii) Draw a typical flow front indicating the aspect ratio of the elliptical
shape.
7. You are to conduct two experiments of mold filling in a rectangular mold. The flow will
be constrained to be one-dimensional as the injection will be through a line injection
gate as shown in Figure 4.39.
Figure 4.39: One-dimensional flow in a rectangular mold.
In the first experiment, you place in the mold a preform that occupies 25% of the
mold, and you are given that its permeability for a fiber volume fraction of 25% is

1 * 10~9 m2 in the direction of the flow. Find the time it takes to fill the mold. In the
second experiment, you use a different preform that occupies 50% of the same mold,
and you are told that its permeability is also 1 * 10~9 m2 when it occupies 50% of
the mold. Do you expect the filling time to be the same as in the first experiment,
as they have the same permeability? Explain your answer. The length of the mold
is one meter and the viscosity of the fluid is 0.1 Pa.s. The injection pressure is held
constant at 2 bars.

Chapter 5
Model Simplifications and Solution
5.1 Introduction
A model is an idealized mathematical representation of a physical process or a system. The
intent of this book is to teach the fundamentals involved in building process models for
polymer composite manufacturing methods such as injection molding, pultrusion and resin
transfer molding.
Manufacturing of composites has relied on experience and trial-and-error methods to
design, develop and fabricate a product. However, this approach has proven to be expensive
in time and money to develop new prototype geometries, which usually translates into high
risk, and therefore has hindered the use of composite materials in many potential industrial
applications. Use of process models can accelerate the path from conception to prototype
development and make these materials and their processing operations competitive with
metal and other materials in terms of their cost.
Composites processing models are built on the foundation of physical laws and appro-
priate assumptions and boundary conditions based on the understanding of the physical
phenomena and constitutive laws derived from experimental data. Once the model is well
posed in mathematical equations, the next step is to examine the behavior of the model
in response to changes in the process and material variables. This information can prove
to be very useful to design a mold or a die for the manufacturing method or to alter the
manufacturing process to create a successful part. To investigate the behavior of a com-
posite manufacturing process in a routine manner and with minimum effort, the process
model can be incorporated into a computer simulation. A computer simulation or a virtual
processing scenario is a combination of an idealized process model expressed in mathemat-
ical equations, a numerical method to solve the equations, and the computer software to
carry out the solution and display the results graphically, mimicking the physical behavior
of the process. Thus, such virtual composite process scenarios can provide valuable and
detailed information about the process and improve the understanding.
Example 5.1: Filling a Simple Mold

An L-shaped mold needs to be filled without any "dry spots" (regions with no resin) and
in minimum time. You have three choices for injections as shown in Figure 5.1. Which one
will you choose?

P = 5 bar
(b) (c)
VentS
Ventl
Ventl Ventl
Fill time = 51 s. Fill time = 118s. Fill time = 169s.
Figure 5.1: Different mold filling scenarios with resin injection from three different locations
in an L-shaped mold. The mold filling simulation depicts the location of the flow fronts and
can indicate the filling time to completely saturate the mold. The filling times are 51, 118
and 169 seconds for the three selected injection gates.
Solution
Different gate locations/conditions can be investigated to achieve the mold filling goals.
In the L-shaped mold shown in Figure 5.1, three different gate locations under the same
injection pressure are filled to find which location results in the minimum filling time. A
mold filling simulation based on flow through porous media may be used to simulate all
three cases. The results show that the filling times vary considerably: 51, 118 and 169
seconds, in (a), (b), and (c), respectively. Instead of conducting trial and error in actual
mold filling, investigating different simulations will save considerable design time and hence
filling time. It can also save the part from "dry regions without resin" by choosing the
gate location appropriately, and placing the vent(s) at the last points to be filled. In this
example, 3, 1 and 2 vents are needed in (a), (b) and (c), respectively, as shown in the same
figure. •
5.1.1 Usefulness of Models

Process models are very useful as they can quantify understanding and the knowledge
about a process [235]. Moreover, a reliable mathematical model will reduce the scope of
experiments by combining the effect of different variables and testing unproven design ideas.
Finally, models provide more detailed information than the experiments and thus can be
used to investigate which experiments will be interesting to conduct. Models can provide
information about important variables that cannot be directly measured. Models do not
replace experiments, but together with experiments, mathematical theory and physical laws,
models assist engineers and scientists to understand the process and manipulate and tailor
it to meet their requirements.
Resin transfer molding (RTM) provides an excellent example of the uses of process
models. Even if we consider just the filling and curing of an RTM part, many physical
phenomena transpire. For example, a viscous polymer flows through a network of channels
created between the fiber preforms to fill the mold cavity.' Heat may enter the cavity by
conduction from the mold walls. The resin molecules may start to react and form a cross-
linked network, increasing the viscosity of the resin and also releasing heat, which needs to

be convected away. All these factors will determine if the cavity will fill completely, how
long the part should be left in the mold, whether the part will warp due to residual thermal
stresses, and what the final properties of the manufactured part will be.
As one cannot "see" inside a closed mold, it is difficult to know if the resin occupied
all the empty spaces between the fibers and if the part had cured sufficiently to retain its
shape to de-mold the part. A process model can let the engineer or the scientist "see" the
filling pattern and the curing rate, thus quantifying the knowledge of the filling process.
As the engineer learns more about the filling from the process model, he or she does not
have to conduct many experiments to find the best location for injection by trial and error
using prior experience. The model can provide a few possible locations which reduces the
scope of experiments. Thus, a reliable model can reveal the performance and outcome of
different mold designs, just as an experiment would, without the added expense and time
of fabricating and testing every design. So, process models can help save cost and time in
developing new designs.
RTM simulations provide further benefits. From experiments, one can measure the
inlet pressure and maybe the flow rate. If one had a few sensors inside the mold, one
could monitor pressure or temperature at those locations. A process model provides de-
tailed information about the pressure field, flow front shapes, temperature, cure profiles and
velocity fields. These can be graphically displayed and easily interpreted to improve the
understanding of the process and identify difficult issues. However, computer simulations
must be validated and verified if they are to represent the physical world. Also, one needs
to conduct experiments to characterize permeability and cure kinetics that are used as in-
puts into the model. Thus, experiments are a necessary component in the construction of
a process model.
In this section, we have explained why models are useful, and next we will provide the
approach to build them, introduce simplifications and represent material and phenomeno-
logical behavior. We will also present the tools to simplify and analyze the behavior of a
process model. It is important to validate the model to justify the assumptions and the con-
stitutive laws used to construct the model. Various approaches to validation and revisions
will also be discussed.
5.2 Formulation of Models

Models may vary from each other, but one can build them by following the plan outlined
in Figure 5.2. As a model is a mathematical representation of the physical process, one
must be able to define it, develop the equations and boundary conditions that describe
the process, and solve the equations to calculate the important parameters of interest so
that one can assess the accuracy and usefulness of the model. Finally, model revision is an
important step as it allows one to refine the model and move it a step closer towards the
physical process.
5.2.1 Problem Definition

The purpose of a model is to predict the behavior of a process for a range of inputs and
conditions [236]. Hence, one must define the physical process and its inputs. The physical
process may not represent the complete composite manufacturing process but may focus
on a small aspect of the process, or on a processing operation during manufacturing. For
example, in injection molding, mold filling is only one aspect of the manufacturing process.
The model here may treat the screw and the runner and the spruce as only a source of

Objective Define System
Problem Definition
Identify
Boundary Conditions
Important Parameters
Physical Laws
Empirical Laws
Build Model Assumptions
Analogies with
Other Systems
Simplifications
Analytic Methods Solution Numerical Methods
Experiments
(How well physics
Solution to Equations
is described?)
Validation Model Assesment Verification
Check
Check Assumptions
Boundary Conditions
Model Revision
Check Check
Constitutive Equations Solution Method
Figure 5.2: Modeling flowchart.

fiber suspensions at a given flow rate. Thus, an important step is to define the system that
one is modeling and draw a boundary around it. The other parts of the process, which can
be modeled as other sub-systems, can interact with the system only by what they supply
across the boundary [102].
The aim of the model will influence what aspect of the model is emphasized and hence
should also be defined. It is useful to identify the important responses of the process and
what conditions and inputs the model requires. Depending on the aim, different models for
the same physical process give different answers. For example, in processes such as resin
transfer molding, some models only relate the flow rate to the pressure, while others may
provide detailed information about the flow front locations in a complex geometry. Other
models may be limited to a few cavity shapes. Some models may even provide temperature
histories and predict residual stresses. Other models may only focus on the curing phase
and ignore filling. Thus, there can be a multiplicity of models for the same process. Which
model one wants to choose or build will depend on what issues are important and how much
time and effort one can devote to finding the answers. Thus, it is crucial to choose or build
a model for the situation of interest if it is to prove useful in enhancing the understanding
of that aspect of the process.
5.2.2 Building the Mathematical Model

Once the system is defined and the important quantities are identified, one can build the
model from analogies with other systems or from one or more of the following: physical laws
or empirical and phenomenological observations. A mathematical model, which represents
the physical process, describes the system behavior by a set of mathematical equations
with the quantities of interest as primary or secondary variables. Interactions between
the selected system and the surroundings are introduced as boundary conditions for the
mathematical equations.
Most composites manufacturing process models combine the fundamental physical laws
of mass, momentum and energy conservation with empirical observations such as viscosity
and permeability laws. Sometimes, the models can become complicated if one wants to
include every known effect. The skilled modeler will try to simplify the model by making
assumptions that will retain the important effects. This will make it is easier to solve the
mathematical equations and also easier to understand the system. Typically, simplifying
the model will also require fewer parameters to be determined. For example, the flow in
resin transfer molding is important only in the in-plane direction when filling thin cavities;
thus one can simplify the governing equations from three dimensions to two dimensions. To
solve the equations, one needs to provide the permeability tensor. For a two-dimensional
case, one needs only two permeability values, whereas for a three-dimensional case, one
will need the permeability value in the thickness direction in addition. The case for use of
a resin viscosity model is similar. If one simplifies the material behavior to a Newtonian
fluid, one needs only one material parameter for the resin. However, if one chooses to use
the Carreau fluid model, one needs to determine four material parameters. In addition, the
equations become nonlinear and difficult to solve. Thus, simplifications are necessary in a
model, but one must make sure that simplification does not lose the important effects to
be captured.
5.2.3 Solution of the Equations

The formulated mathematical model may be a simple ordinary differential equation with one
independent variable and one dependent variable, or it may be a system of complicated and

coupled nonlinear partial differential equations with two or more dependent variables (such
as resin pressure, temperature and degree of cure, and fiber orientation) that rely on more
than one independent variable (such as time and spatial coordinates). The simple equations
could be solved analytically if appropriate boundary or initial conditions are specified. For
models with partial differential equations to be solved in a complex geometry, one can select
standard numerical methods such as finite difference, boundary element or finite element.
Special techniques may be required in moving boundary problems of processes involving
mold filling. The objective of the model also determines the method to be selected for
solution, since the numerical method determines the time and cost of setting up and running
a simulation. When implementing a numerical solution, it is important to pay attention to
pragmatic issues such as reliability, portability, efficiency and user interface of the computer
software.
5.2.4 Model Assessment

Model assessment must consist of two parts: verification and validation. Verification alludes
to whether or not the selected method provides the correct solution to the formulated set
of equations with the prescribed boundary conditions. Hence, one must always verify that
the numerical technique does not have any programming errors or inconsistencies that can
lead to inaccurate solution of the governing equations. There is a cliche about "garbage
in-garbage out." Verification studies can definitely address this type of criticism. There
are many approaches to verify the method. If one has implemented a numerical solution,
it can be compared to analytic or classical solutions for simplified geometries or for steady
state situations. If no analytic solution is available, one can refine the time step or the grid
size over the domain and check for convergence of the solution. One can also perform global
mass and energy balances over the domain to check if they are being conserved on a global
scale. This will help the modeler to verify if his/her numerical method is implemented
properly.
Validation refers to how well the process model describes the physics of the selected
phenomenon in the process mathematically. In formulation of the process model and its
simplification, one makes many assumptions and introduces empirical relationships and
approximate boundary conditions; hence it is imperative to check that the important physics
we want to model is still retained in the model. Validation allows us to also check if we
have missed any important phenomena in the process. At the same time, validation will
uncover insignificant influences that we have included in the process model that may not
be necessary.
How does one validate a process model? The most common approach is with experi-
ments. One can approach this at two levels.
First, to ensure that the process model is capturing the correct physics, it is important
to carry out a controlled laboratory experiment or a model experiment. For example, if
the goal is to validate the fiber orientation model that predicts fiber orientation due to
flow in a Newtonian fluid, one could use a model fluid such as silicone oil and nylon fibers
with tracer fibers to understand and record the orientation behavior. If one compared
the model results directly with fiber orientation measurements taken from injection molded
plaques, other effects such as viscoelasticity, fiber breakage, cooling of the polymer and fiber
clustering may play a role in influencing fiber orientation in addition to the flow. Hence it
would be difficult to separate the influence due to flow on fiber orientation from these other
effects which were not included in our process model.
Thus, model experiments can usually reveal the underlying physics in a processing sit-
uation and block out the noise or deviations due to other effects. However, it is important

to make sure that other factors are only noise and not important effects in the process
that our model is ignoring or overlooking completely. It is necessary to perform controlled
experiments of the process and identify and monitor the important variables to make sure
that the process model is capturing the relevant physics because a successful process model
will always predict the outcome of experiments.
Although model experiments will provide useful information and also help in validation
of the "idealized model" one would still like to know how well the idealized model represents
the reality of the factory floor. Hence, the second level of experiments should mimic the
manufacturing situation to see how good a job the idealized model does. For example, one
can use random preforms in model experiments to demonstrate how well Darcy's law can
capture the physics of the flow in closed molds in thermoset processing. However, in the
manufacturing of composites, stitched or woven preforms are often used as the reinforcement
choice as one can increase the fiber volume fraction in the composite part. Hence, it is
important to validate if these materials also exhibit Darcy's law, and if not, how far do
they deviate from it? Questions such as "Is it necessary to develop a new model for such
materials?" or "Can one estimate the error introduced due to the dual scale nature of the
preform?" have to be addressed.
5.2.5 Revisions of the Model

If the model agrees with the experimental results, one has a successful model that can make
useful predictions. However, in most cases there will be disagreement between the model
and the experiments. It is important to methodically explore the cause of the discrepancy,
as there can be many. First, one must check that the solution method used is not imperfect.
This requires looking for errors in the implementation of the solution method for the gov-
erning equations. Next, one must check if there are deficiencies in the model. The model
may have used an erroneous assumption, an inappropriate empirical law, a false hypothesis,
an over simplification, or an inaccurate boundary condition. For example, if one assumed
that the fiber-fiber interactions during the flow are not important and ignored them in the
fiber orientation model and the results did not agree with the experimental outcome, one
might have to reexamine this assumption in the model. Thus, it important to separate the
deficiencies in the model from those in the numerical methods as both of these are packaged
into a computer program and it is very easy to regard them as one entity.
Other simple causes of disagreement could be inaccurate characterization of material
parameters. For example, in RTM, the model may use a constant value for the permeability
of the preform in the mold. However, in the experiment one may have slight variations in
the permeability, or in some cases large variations. The result is that the experimental fill
times or inlet pressures will be very different from the predicted ones due to these variations.
Thus, the process model may be correct, but incorrect specification of material parameters
can cause disagreements as well. It is also useful to make certain that the physics embedded
in the process model is the physics being described by the experiment. There is a common
saying that when a modeler is presenting results from a model, nobody believes them except
for the modeler. However, when an experimentalist presents the results, everyone believes
them except for the experimentalist. Thus, it is important to make sure that the experiment
was conducted under the same conditions assumed in the model and that it was free from
issues such as inaccurate calibration of the measurement probes, other experimental issues
such as leakage of the pressure, fluctuations in the flow rate, etc., as these can make the
experimental boundary conditions different than the ones assumed in the model and could
be the root cause of disagreement.
The moral is that models routinely disagree with experiments and revisions should be

considered as a natural and necessary component of the modeling approach. The revisions
sometimes can also focus on inclusion of additional physics in the model to the observations
made in the experiments, and thus, continue to refine the model and bring it closer to
mirroring the physical process.
5.3 Model and Geometry Simplifications

Once the model has been posed correctly in mathematical terms with appropriate boundary
conditions and before one plunges into solving the equations, it is always beneficial to explore
simplifications. However, the simplifications depend not only on the process, but also on
the material being processed, the phenomena of interest and the objective. There are many
approaches to simplifications and one can realize them by reducing one or more of the
following [237]:
1. the number of equations to be solved
2. the number of terms in the governing equations and/or in boundary conditions
3. the degree of non-linearity in the equations and/or boundary conditions
4. the degree of coupling between the equations
5. geometric complexities in the solution domain and boundary conditions
6. complexities in the material behaviour constitutive law
7. complexities in the mathematical and solution methods
However, one must guard against oversimplification as it could result in omission of the
important effects one wants to capture in the process model [237]. Several tools can be
used to simplify the model. For example, consider simple shear flow of a composite material
between two parallel plates as shown in Figure 5.3.
=T
H
->^>^>^>^>^>i.
^* T=TL
Figure 5.3: Non-isothermal simple shear flow of a fiber suspension between two parallel
plates.
Resin temperature is T0 everywhere initially. The lower plate is at temperature TL and

the upper plate is moving at a velocity t/o in x direction, and is at temperature TH- As
the resin viscosity is a strong function of temperature and there may be appreciable viscous
dissipation, the momentum and energy equations are coupled. To find the velocity and
temperature profile of the resin, one has many options. One can solve the coupled systems
of PDE (partial differential equations)
»„
(5.1)

(5.2)
OT
• VT = fcV2T + r : (VU) + R. (5.3)
which are the conservation of mass, momentum and energy equations, respectively with the
following boundary and initial conditions:
ux — U0, uy = uz = 0 at y —h (5.4)
ux = uy — uz = 0 at y =0 (5.5)
at y=h (5.6)
T = TL at y =0 (5.7)
T = T0 at t =0 (5.8)
This full system will require investment of many hours and computer resources. One
could simplify the system by assuming that the flow and/or temperature profile is fully
developed. One could simplify it further by assuming that viscous dissipation is negligible
and solve for the temperature profile before solving for the momentum equation, or one
could assume that the dependence of viscosity on temperature has no effect on the solution.
If the aim of the model was to capture the effect of temperature boundary conditions on
the flow rate and if one chooses the last option, one has made an assumption that will not
result in capturing this effect.
Example 5.2: Temperature Dependent Viscosity

Consider flow of a polymer suspension between the extruder screw and the barrel. As the
gap between the barrel and the screw is usually one to two orders of magnitude smaller than
the radius of the barrel, one can model this as flow between two parallel plates separated by
a distance h as shown in Figure 5.4. The velocity of the barrel is U0. The viscosity of the
suspension is temperature dependent. The objective is to find the influence of temperature
dependent viscosity on the velocity profile.
Barrel
Screw T = TL
Figure 5.4: Flow of a polymer suspension between the extruder screw and the barrel.
Solution
If we assume a steady-state and fully developed velocity and temperature profile, it will
allow us to represent velocity and temperature profiles as
u = u(y), v = w =0 (5.9)
(5.10)

where u is the component of velocity in the x-direction. From the equation of motion
(Equation (5.2))
r\T
^=0 (5.11)
dy
which results in the following:
Txy=Cl. (5.12)
One can assume a linear stress-strain rate constitutive law

du
rxy — fj, — (Newtonian Law). (5.13)
dy
As viscosity is temperature dependent, one can represent it as a constitutive law
M = ê-'P1-^ (5.14)
where /j,0 is the viscosity at a reference temperature TO, and a is a material constant.
Substitution of Equation (5.14) into Equation (5.13) leads to
The energy equation (see Chapter 3) in which we use steady-state and fully developed
assumptions and retain the influence on temperature due to viscous dissipation allow us to
simplify the equation as follows:
dy2 \dyj • -
Equations (5.15) and (5.16) are coupled as u depends on viscosity which is a function of
temperature and temperature depends on u. If one further assumes that viscous dissipation
was not important (a good assumption for low viscosity materials but questionable for high
viscosity materials; usually one could estimate the importance of viscous dissipation with
Brinkman's number as we will discuss in a later section) then
•" 1 ( • ) ' - ' \ /

dy2
which results in
I~TT =f (518)
J-H-J-L n
with the use of boundary conditions shown in Figure 5.4. One can now substitute the
temperature dependence in terms of y dependence in Equation (5.15) and integrate
y= du (5.19)
J
where B\ = TH — TL and 62 = TL — TO . Integrating Equation (5.19) results in

Using the boundary conditions,
0 at y = 0 (5.21)
U0 at y = h (5.22)
allows one to find the velocity profile

, a1
(5.23)
For TH > TL, (i.e., 9\ is positive), the velocity profile u(y) is sketched in Figure 5.5 for
061=0.1 061=1
Figure 5.5: Velocity profile for positive >
different aQ\ values. Notice that, the velocity profile becomes linear as aO\ —» 0. This
is not surprising, because as aQ\ —> 0, fj, = /j10e~a(T~T°^ —> \i,0\ hence the dependence
of viscosity on temperature is very weak, and the thermal boundary conditions will not
cause deviation on the linear velocity profile. On the other hand, as aQ\ increases, the
velocity profile becomes very nonlinear. For a better approximation of the temperature
profile with viscosity dissipation included, substitute the derivative of u from Equation
(5.23) into Equation (5.16) and integrate to find the nonlinear temperature profile due to
viscous dissipation. •
How we simplify the model, pose the correct problem and find its solution is an im-
portant aspect in process modeling. We will focus on some important tools that will be
useful in doing so. They are (a) dimensional analysis, (b) common assumptions in poly-
mer composites processing, (c) various simplifications to represent boundary conditions, (d)
simplified geometric models, and (e) mathematical manipulations to simplify the solutions.
5.4 Dimensionless Analysis and Dimensionless Numbers

Dimensionless analysis is a very important tool for reducing the number of equations and the
number of terms in the governing equations and also for estimating the degree of coupling
and nonlinearity. In addition, it can allow us to develop scaling laws for the phenomena of
interest in the process to scale the geometry from the laboratory scale to the production
scale. Every undergraduate fluid mechanics textbook devotes a section or a chapter to
dimensionless analysis and important dimensionless numbers. In this section, we will discuss
the approach to the analysis and the important dimensionless numbers in polymers and
polymer composites processing [237].

First, one must identify all the independent and dependent variables in the set of gov-
erning equations and the boundary conditions. This should be a straightforward task to
accomplish. The second task, which is not so obvious, is to find a characteristic value with
the same dimensional units for each identified variable in the equation. The candidates for
the characteristic value can be an aggregation of known parameters usually related to the
material and the process conditions. For example, if one wanted a characteristic value for
the velocity in a flow through a die, the average flow rate divided by the cross-sectional
area would be a good candidate if the flow rate were constant for the process. Another
qualification the characteristic value should try to satisfy is that the variable divided by
the characteristic value should be of the order unity. If one adheres to this criterion, every
nondimensional term in the equation will be of the order unity. One can then compare the
coefficients in front of each term in the equation to decide which terms play a dominant
role and eliminate the ones that are insignificant.
Sometimes, it may be difficult to identify an obvious choice for a characteristic value,
and much thought should be given to this task. In some cases, it is known that a term is
important but the physical situation does not provide a value for its magnitude. In such
situations, one can use scaling analysis to find its characteristic magnitude. The general
approach is to assign an unknown characteristic value that can later be determined from
the nondimensional form of the governing equation by forcing the coefficient containing the
unknown characteristic value to be unity. For example, consider a pressure driven flow
through a pultrusion die. Usually, the pulling speed is the independent variable; hence the
flow rate is known, so one has a choice for a characteristic velocity but not for the pressure.
If one nondimensionalizes the equation of motion and allows the coefficients in front of the
nondimensional viscous stress terms and the pressure term both to equal unity, it will give
the correct characteristic value for the pressure as will be shown in an example.
However, before we present further examples of dimensionless analysis in composite
processing, we present here general guidelines for casting a dimensional equation into a
nondimensional form [237]. Consider an equation
where T is the dependent variable and t and x are independent variables. k\ to £4 are
coefficients in front of the governing equation. As explained above, to cast this equation
in nondimensional form, one must find characteristic values for each of the variables in the
above equation. The variables are T, t and x. Thus, one nondimensionalizes them using
characteristic values Tc, tc and xc
T* = , t* = - and x* = — . (5.25)
J. c Tc Xc
Here Tc, tc, and xc will be related to some physical situation of the problem. For example,
if x was the variable along the length of a mold geometry, L, then xc = L. If T was the
variable temperature and represented the temperature of the resin, then Tc could be the
temperature difference between the initial temperature of the resin Tj and the mold wall
temperature Tw. Thus Tc — Ti~Tw\ this will ensure that the T* is also of the order unity.
When possible, have all dimensionless variables range from zero to unity.
Thus, the nondimensional form of Equation (5.24) becomes
Tc dT* Tc dT* Tc

Here k-[Tc/tc, k<2Tc/xc, k^Tc/x2 and £4 are coefficients of the dimensionless terms in the
governing equation. At least one of the dimensionless terms should have a coefficient of unity
and it should be the dominant of all the terms in the equation. Divide the non-dimensional
equation by the coefficient of one of the dominant terms, which hopefully should lead to all
the other coefficients in the equation being smaller than or of the order unity. For example,
if kiTc/tc was the dominant coefficient (transient process was important in the model), then
one would divide every coefficient in Equation (5.26) by k\Tcjtc which will result in
^ t c d r * ^ ^ d2T* £4 tc_ = , }
dt* fci xc dx** fci x2 d(x*)
* 22 (
' }
Note that, as the equation is dimensionless and as the coefficient in front of the first
term is unity and dimensionless, all other coefficients (|^ ^-, |^ 1%, and ^ |f ) will also be
dimensionless. Now, one can neglect the terms that have coefficients much less than one.
For example if ^-tc <C x2 and ^-tc <C xc, one could neglect the terms with dT* /dx* and
d2T*/d(x*)2 as the coefficients in front of them ^|% and f^, respectively, will be small.
Thus, the partial differential equation (5.27) reduces to the ordinary differential equation
given below
f + lt- <«•>
Also, if one did not have a characteristic value for tc, one could choose it to be tc = kiTc/k^
by making the coefficient equal to 1. This reduces the nondimensional equation to
dT*
— + 1 = 0. (5.29,
if k3Tc/k4 < x2 and fc2rc/fc4 <C xc.

Thus, by scaling analysis, one can simplify equations and also find characteristic values
for some of the variables. However, beware that one may not be able to satisfy all the
boundary conditions. In the above example, we started with a second order PDE which
should have two boundary conditions in x and one in t, but we simplified the equation to
first order ODE so all we need is one condition in t. The solution will not be far from the
solution to the complete PDE in most of the domain but will be poor near the boundaries
where the boundary conditions were dropped. Near the boundaries, the terms neglected
will be of the same order as the terms retained and should be considered if one wants to
know the exact solution in this subregion. So, we can have two solutions, one in the interior
of the domain, where the other terms are not so important and the complete solution near
the boundaries of the domain. Thus as one goes from the interior to the boundary, one can
match the two solutions using asymptotic expansions in order to get the complete solution.
Example 5.3: Curing of a Composite Plate

Consider the process in which epoxy-carbon fiber prepregs are stacked and placed inside a
metal tool. The metal tool is then placed in a press to heat the composite to initiate cure.
Formulate the simplified equation that you would have to solve to find the temperature.
Find the temperature profile if you assumed that the cure rate was constant throughout the
domain and that the composite had reached a steady state. The dimensions, coordinate
system, thermal coefficients and thermal boundary conditions are shown in Figure 5.6.

h = 2 cm
k =k =10W/m.C
xx yy
k = 1 W/m.C
Figure 5.6: Epoxy-carbon fiber prepregs that are stacked and placed inside a metal tool
with mold walls at temperature Tw = 200°C.
Solution
The energy equation reduces to
T -K — U (5.30)
dx2 dz2
T T
dy<
as there is no flow and no viscous dissipation. Here, kxx, kyy and kzz are thermal conduc-
tivities of the composite in the x, y and z directions, respectively, and R is the volumetric
rate of heat generated inside the composite due to the curing reaction. Also, steady-state
is assumed (usually not a valid assumption).
One can further simplify Equation (5.30) and find its solution as detailed using the
following procedure. First identify independent (x, y and z) and dependent (T) parameters.
Then, form dimensionless variables:
T — T-
x = y =—,
yc z=
and1 1rr* — * (5.31)
here Tc = Tw — Tj (characteristic temperature is always expressed as a difference), xc = L,

yc — W, and zc •— h. Rewriting Equation (5.30) using the nondimensional variables in
Equation (5.31) leads to
kxxTcd2T* t kyyTc32T* , kzzTcd2T*
(5.32)
x2 dx*2 y2 dy*
One can drop the first and second term in Equation (5.32) since
-Ti
andi (5.33)
Physically, this implies that most of the heat is conducted through the thickness direction
as h <C L,W even if kzz is an order of magnitude less than kxx and kyy. Thus, Equation
(5.32) simplifies to
d2T* R h2 , N
(5.34)
dz* -*-i

As the left-hand side is dimensionless, the right-hand side also should be dimensionless:
(flT*
^T = -R" (5-35)
where
R
R* = T _T . (5.36)
JU
Thus, R* is a dimensionless number that compares the volumetric heat generation rate
with the heat being conducted through the composite. The solution to Equation (5.35) is
straightforward if R is assumed to be constant:
dT*
d
-L = -JZV + d (5.37)
+ Clz* + c2. (5.38)

Zi
The boundary conditions are

T* = 1 at z* = I (5.39)
dT*
T* = 1 at z* = -1 or -— = 0 at z* = 0. (5.40)
V ;
dz*
One can solve c\ and c<z by using these boundary conditions. Hence, Equation (5.38) is
rewritten as
2
T*
1 - -^Z* +— + I
~ 2 Z + 2 +1
= -~(z*2-l) + l. (5.41)
The temperature gradient is determined by taking the z*-derivative of Equation (5.41)
dT*
= -R*z*. (5.42)
dz
Thus, the temperature gradient is maximum near the edges, and zero at the center. The
larger the value of the gradient, the greater the chances of developing of thermal stresses.
Hence, it is important to have a low value of .R*. •
Example 5.4: Flow in Thin Gaps
Formulate nondimensional conservation of mass and momentum equations for flow of viscous
Newtonian fiber suspensions in long and narrow channels.

Solution
Injection molding of thermoplastics and fiber suspensions involves flow of viscous fluids
through narrow gaps (H <C L) as shown in Figure 5.7. Before conducting the dimensionless
analysis, one must first list the parameters and characteristic values for all dependent and
independent variables. For the parameters for which a characteristic value is not intuitively
obvious, we use the subscript c to denote the characteristic value that will be selected later.
Assume flow to be uniform in the y (the width) direction. Hence we will consider only 2-D
analysis (x and z directions).
(Per unit width in

y direction)
(L » H)
Figure 5.7: Steady-state flow of viscous fiber suspensions in narrow gaps.

Parameters:
geometry : H, L
material parameters (viscosity, density) : /j,, p
flow rate : q
stresses: TXX,TXZ,TZZ.
Dimensionless variables (shown with hats) and characteristic values:
x
X =
I
z
Z
= H
(note that q is per unit width)
q/H
w
w =
wc
p = p (5.43)
(TXX)C
T??
T,, =
The continuity equation in 2-D incompressible flow,

du dw
(5.44)

can be written as follows in terms of dimensionless variables
_d I £ —n ("5 45)
HL dx H dz ' ^ ' '
Thus, we can make the order of both the terms of the order unity as follows:
^ + ^ =0 (5.46)
dx dz
if we select wc = q/L. Thus, non-dimensionalization of the continuity equation can provide

an estimate of flow in the z direction. Note that if H -C L, then characteristic flow in the
x direction uc ^> wc (the characteristic flow in the z direction).
If we use Newtonian law, constitutive equations provide an estimate for characteristic
stresses:
fxx==2~ (5.47)
if (Txx)c is chosen as -j^.

TZZ = 2 — (5.48)
dz
if (TZZ)C is chosen as ^k
\F>f, HA 2dw
du + /(H_\ rtin' 2
~dz \T) ~dx (5.49)
if (Txz)c is chosen as -j^-. As H <C L, then (rxz)c ^> (TZZ)C and (TXX)C. Thus, nondimension-
alization suggests that shear stress (rxz) is dominant as compared to normal stresses (TXX,
As viscous materials achieve steady-state and a fully developed profile very quickly,
steady-state flow is not an unreasonable assumption when considering conservation of mo-
mentum. Also, one can ignore body (gravity) forces in the equation as viscous forces
dominate. Thus, the 2-D equation of motion simplifies to
f du du\ dP drxx drxz

p(u—+w—\ = -Tr- + 1T~ + ^r~ (5.50)
\ ox dz J dx dx dz
dw dw\ dP drzx drzz
u——h w— = — ——I— 1—-— (5.51)
dx dz J dz dx dz
Equations (5.50) and (5.51) can be rewritten in terms of dimensionless variables as follows:
pq2 (^ dw dw\ Pc ( dP\

u w
ITT)
2 \ "5^ +
HL \ dx ~^l
dz J = 17
H\ ~ -dz
^ rJ-
Now, by considering both equations simultaneously, we should rearrange the terms, by

making the dominant term unity. As shear stresses dominate, and since fj,q/H3 ^> any

other term, as H <C L, Equations (5.52) and (5.53) are rewritten by dividing all terms by
/j,q/H3 which results in
dx^ dzj ~ w L d x ] \ L ) 8x
H3
w +w^dw\ = Pc idP\ + (H\(dtxz + 3tzz\ (5 55)
^) -wU*) U)bi- -0rJ-
#2 \ /
'
One can now choose Pc = p,qL/H3, such that the coefficient in front of the pressure gradient
term in Equation (5.54) is unity. Note that Equations (5.54) and (5.55) are scaled properly
as the scaling term for pressure Pc — [iqL/H3 is the same in both Equations (5.54) and
(5.55). Also, as H <C L, one can ignore all terms that have H/L or their higher powers.
Thus, the complicated equation of motion for flow in narrow gaps simplifies to
(5.57)
5.4.1 Dimensionless Numbers Used in Composites Processing

After one obtains the nondimensional form of the equations, the coefficients in front of
the terms can usually be reduced to one or more dimensionless numbers. This helps in
identifying the role of various physical parameters in the process. From the Buckingham
Pi theorem, one can easily forecast how many dimensionless groups to expect [238]. The
Buckingham Pi theorem states that the number of dimensionless groups we expect is equal
to the number of variables in the system minus four if we encounter all M (mass), L
(length), T (temperature) and t (time) units. If we encounter only three of the four units
in the problem, then it will be minus three and so on. Temperature is always represented
as a difference rather than an absolute value.
For example, the Fourier number measures the importance of transient effects in the
absence of flow. How fast a composite will heat or cool due to conduction is directly
proportional to the Fourier number, which is given by
Fo = ^. (5.58)
a
Lc is the characteristic length in the direction of heat removal or heat addition by conduc-
tion, a is the thermal diffusivity and is given by
a = 4r (5.59)
P^P
where p and Cp are the density and heat capacity of the composite respectively, k is
thermal conductivity of the composite in the direction of conduction, if the composite
exhibits anisotropy.
Most commonly used nondimensionless numbers in polymer and polymer composite
processing are listed in Table 5.1.

Table 5.1: Dimensionless Groups Commonly used in Polymer and Polymer Composites
Processing
Dimensionless Number Definition Interpretation
Brinkman number Br = viscous dissipation

conduction due to AT
Capillary number Ca = viscous forces

surface tension
Damkohler number Da = (OT/dt) from reaction

(dT/dt) from conduction
Deborah number De = elastic effects

R viscous effects
V2 inertia
Froude number Fr = — gravity
gL
Gelling number fill time

trv reaction time
Graetz number Gz = flow direction convection

aL transverse conduction
hD convection at the boundary

Nusselt number Nu = ~k~ conduction of the fluid
Nahme-Grifnth number Na = viscous dissipation

heat required to alter the viscosity
Pearson number Pn =
heat required to alter viscosity
Br heat conduction due to AT
_ pcpLV heat dispersion

Peclet number Pe = heat conduction
k
Prandtl number momentum transfer

k heat transfer
Reynolds number VLp inertia force

viscous force

Example 5.5: Importance of Fourier Number in Nonisothermal Processing
Consider a polymeric composite that one would like to cool from 200°C down to 70°C as
shown in Figure 5.8. The top and bottom surfaces of the composite are kept in perfect
thermal contact with an aluminum tool at Tw = 25°C. After how long should the engineer
remove the part from the tool?
V25C
2h = b = 2 cm When does T reach 70 °C at z = 0?
Figure 5.8: A polymeric composite cooled from 200°C to 70°C.
The thermal conductivity of the polymer is k = 0.1 W/m.C and that of the S-glass used
is k = 10 W/m.C in both the longitudional and transverse directions. The density of S-2
glass is 2500 kg/m3 and Cp is 0.41kJ/kg.C. For the polypropylene matrix, Cp is 2.0kJ/kg.C
and density is 900kg/m 3 . The S-glass fraction in the composite is 50%.
Solution
Parameters:
geometry W,L,h
process AT(=Tw-Ti),
material k,p,Cp,Vf.
Governing equation:
dT
(5.60)
In Equation (5.60), u • VT can be neglected as there is no flow, R is zero as there is no heat

generation, and T : Vu vanishes as there is no dissipation. If we assume fibers are along
the x direction, then the energy equation (5.60) simplifies to
dT_ dT_ d_ 8T_

J- QT - 9 (IkKrr (5.61)
P^ ~nl"
dt — "n~ dx <-> dy dz
dx ay ~d7
For this case, kxx — kyy — kzz = k. Choose characteristic values for independent (x,y,z,t)
and dependent (T) parameters
X y z
(5.62)
L' h' T
-L 111
—T-
-*- 7,

Here tc is a characteristic time value that we hope to uncover from the nondimensional
version of the equation. Substitution of the above variables from Equation (5.62) into
Equation (5.61) will result in the following nondimensional equation:
h2 86
^dl
here a = k/(pCp) where
k = (l- Vf)kies-m + libers (5.64)
and
PCP = (1 - Vf)(pCp)ies-m + Vf(pCp){ibers. (5.65)
As h <C L, h/L and h/W are much smaller than unity, one can safely ignore the conduction
in the x and y directions. Also one can choose tc — h?/a, such that the coefficient in front
of dO/dt will become unity. Thus, the nondimensional form becomes
86 (5 66)
'
The two boundary conditions and the initial condition are given as follows:
at i = 0 (5.67)
at z = I (5.68)
f)f)
— = 0 at z = 0. (5.69)
dz
Note that the temperature distribution is symmetric about z = 0 due to the geometry and
boundary conditions at z = ±1. Hence, one could solve this problem in — 1 < z < I domain
by using #(— 1) = 1 and 6(1) = 1. Or, alternatively, and as we did here, one can use the
symmetry condition and solve the problem in 0 < z < I domain by using dO/dz(0) = 0 and
6(1) = 1.
Equation (5.66) is a diffusion equation. One can apply the separation of variables
technique to solve it along with the boundary and initial conditions
(5.70)
Substitution of Equation (5.70) into Equation (5.66) yields
ZT' = Z"T. (5.71)
Division of Equation (5.71) by ZT results in
TV <7"
Since the left-hand side of Equation (5.73) is a function of t only, and the-right hand side
of Equation (5.73) is a function of z only, Equation (5.73) can be true only if
T' X" , ^
-= — — = constant = -K2Z . (5.73)
J A

By applying separation of variables, the original' partial differential equation was converted
into two ordinary differential equations:
Z ll rp/
—- = — K 2 andJ — — —K2,
or, in more familiar forms:
(5.74)
(5.75)
The individual general solutions are given below
_ J A cos KZ + BSW.KZ,
= \D + Ez,
and
Thus, the product solution is given as
9 = H + Iz + (J cos KZ + K sin Kz)e~K2t , (5.78)

where DG was replaced by H , and so on. The unknown coefficients will be determined by
using the boundary and initial conditions. Let us first apply the boundary condition given
in Equation (5.69)
— (z,t) = I + (— J/tsin KZ + KKCQSKz)e~K t,
(0,f) = 0 = I+(0 + KK)e-K (5.79)
which reveals that 7 = 0 and K = 0 simplifying Equation (5.78) to
0 = H + JcosKze-KZ*. (5.80)
Application of the other boundary condition, Equation (5.68), results in the following:
6(l,t) = l = H + JcosKe-K'2{. (5.81)

Equation (5.81) can hold only if H = 1 and
« =^ (5-82)
where n = 1, 3, 5, . . . , oo. Using superposition gives

oo ~
9(z,f) = l+ £ Jncosê-^/ 2 ^. (5.83)
n=l,3,5,...

Finally, one can use the initial condition, Equation (5.67):
OO A
0 ( z , 0 ) = 0 = l+ £ Jncos^. (5.84)
n=l,3,5,...
By using Fourier series expansion on Equation (5.84), one can determine Jn:
Jn = - - l ] c o s d x . = - (_i)n-2 (5.85)
nvr
for n = 1, 3, 5 , . . . . Hence, the final solution is given by
oo ,
e(z,t) = l- ]T A(_l)(n-l)/2cos^±e-(nu/2ri_ ( 5 _g 6 )
n=l,3,5,...
Note that if we want to know how long it takes to cool the composite from 200°C (9 — 0)
to 70°C [9 = (70 - 200)/(25 - 200) = 0.7429] at the mid point (z = z = 0), one needs to
evaluate and plot 9(z,t) numerically from Equation (5.86) and find out at what t value,
0(0, t) = 0.7429. In order to numerically evaluate Equation (5.86), a simple program can
be written as shown below in FORTRAN, or any other programming languages such as C,
BASIC, or mathematical solvers such as MATHEMATICA, MATLAB or Maple.
c A FORTRAN code to calculate the temperature

c starts here —
open(unit=ll,file='output.dat',status='unknown')
pi = 4.0*atan(1.0)
x=0.0
do 100 1=1,200
t=i*0.01
theta=l.0
err=l. 0
n=l
previo = 999.0
do while(err.gt.0.00001)
theta=theta-( 4.0*(-1.0)**((n-l)/2)/(n*pi) )
? *cos(n*pi*x/2.0)*exp(-(n*pi/2.0)**2*t)
err=abs(theta-previo)
previo = theta
n=n+2
end do
100 write(11,500) t,theta
500 format(2fll.5)
stop
end
c ends here —
Figure 5.9 was prepared, and i was found to be 0.6484. This corresponds to t — tct —
( h 2 / a ) f = (0.012/0.00000358)0.6484 = 18.1 seconds. •

o
CD
O
Q.
0.8
0.7429
o
§ 0.6
2
&
Q.
E
0.4
"CD
c
g
'w
c 0.2
OJ
E
T3
C
O
0.5 1.5
S
o
Nondimensional time, t
Figure 5.9: Nondimensional temperature versus nondimensional time at the center of the
composite part. In order to cool the composite from 200°C (0 = 0) to 70°C (9 = (70 -
200)/(25 - 200) = 0.7429), the part should be kept in the mold for t = 0.6484 which
corresponds to 18.1 seconds.
Example 5.6: Role of Brinkman Number
A polymer suspension flows through a channel of thickness h and length L. The schematic
is shown in Figure 5.10. The temperature of the polymer is T; before it enters the mold.
The mold wall temperature is kept at Tw. Formulate the energy equation that depicts the
importance of viscous dissipation in heating of the suspension.
T = T:
'"• . W 1; .-&
Flow rate, q Az t
(Per unit width in 1 >.x Material parameters: k, p, Cn,(4, h
y direction) I
,,,,,,,,,,,,,,,,,,, T —T
w 'K- •;/•
« - . .. 1 ... k-
(L » h)
Figure 5.10: Nonisothermal flow of a polymer suspension through a channel.

Solution,
Assuming that flow is in the x direction, one can ignore y-direction flow and heat transfer
and write the energy equation in 2-D as shown below,
dT +u
dT\ = id2T
fe
d2T
W
ot ir}
ox J 4 1 + Tl +r:Vu + R. (5.87)
As the flow is only in the x direction, v and w components of the velocity vector u are zero.
There is no internal energy generation; hence R — 0. Also, as h <C L
d2T d2T (5 88)

s? «I? -
as can be seen from previous examples. Also the viscous dissipation term reduces to
du du du dv dv
T' •' \7n
v
*-*
— IT
1 ' XX
—
r\
-i- T —
1 ' XII f^.
4- T
I ' XZ
—
i-\ ' ' 'U& f-\ i ' '(/'(/ *-,
ox ay dz ox ay
dv dw dw dw\ , ,
(5.89J
= rxz— (5.90)
as v = 0, w = 0, and as h < L, therefore, | | > |^, |^, and rxz > r^^, rxy as seen from
the example on flow in thin gaps. One could have arrived at the same conclusion using
dimensionless analysis.
Using the following nondimensionalization of the variables:
u u
uc q/h
AT
X
T — —
L '
Equation (5.87) takes the following form:
/ AT A 8G\
PCP (uc —u - J = -^- ^ J + -^ ^-J (5.91)
here AT = TW — Ti, and a Newtonian constitutive equation TXZ — /j,^ was assumed. We
can select the conduction term as the one whose coefficient should be unity. Hence, division
of Equation (5.91) by kt\T/h2 results in
a \LJ\ dx
89
(5.93)
\ /

where the Graetz number Gz = uch?/(aL) and the Brinkman number Br = jj,
The Graetz number measures the ratio of heat convection to heat conduction. The Brinkman
number measures the ratio of viscous dissipation to heat conduction. If Br <§C 1, then vis-
cous dissipation is not important. If Gz is small and Br3> 1, then all heat generated due to
viscous dissipation has to be conducted. If Gz and Br are large (» 1), then heat generated
due to viscous dissipation is convected faster than it is conducted. •
5.5 Customary Assumptions in Polymer Composite

Processing
Certain assumptions can dramatically simplify a process model. However, inappropriate
simplifications can also lead to process behavior not in sync with observations. Hence, it is
important to justify the assumptions a priori or after the solution is obtained or by validating
the assumption with experiments. We will list the common assumptions employed in one
or more processes, depending on the phenomena of interest. It does not imply that all
processes will employ the same assumptions listed. To model a phenomenon or a process,
one should go through the exercise of justifying every assumption made to simplify the
model [237].
5.5.1 Quasi-Steady State

Physically, a variable such as velocity, temperature or pressure if it is in steady state indi-
cates that, from a stationary reference frame, the variable does not experience any change
with time at that spatial location. Mathematically, steady state can be described by setting
d ( ) / d t = 0 by placing the variable into the (). Quasi-steady state assumption refers to
approximating an unsteady or time dependent flow with small inertial effects as a succession
of steady state flows. So, even if the problem contains time dependent boundary conditions,
one can solve it as a steady-state problem at any instance of time t. By assuming the value
of the time dependent boundary condition, at that instant in time, to be a constant value,
one can solve the steady-state governing equation.
The quasi-steady state approach is reasonable if the momentum transfer from the bound-
ary conditions is immediate and the material inertia plays an insignificant role. The kinetic
viscosity z/, usually governs the rate of momentum transfer. For polymers and polymer
composites, this value is very high compared to that of water, and hence the rate of mo-
mentum transfer can almost always be approximated as immediate at any instant in time.
Another way to describe this is that, when the viscosity is high, the inertial effects will be
insignificant provided the process velocity is slow (low Reynolds number).
For example, if a thermoplastic polymer is squeezed between two parallel disks with a
constant force F, how can we calculate the gap separation between the plates with time?
A quasi-steady state assumption allows one to ignore the inertial terms in the momentum
equation and solve the radial problem as a steady-state problem at any time t for the
instantaneous gap height (which is a function of time). Other examples that use this
assumption are the processes that simulate the mold-filling scenario. In these classes of
problems, the solution domain in which one solves for the fluid pressure is bounded by the
boundaries of the resin in the mold. The domain is bounded by either the mold boundaries
if the resin has reached the mold walls, or the boundaries of the instantaneous resin front
(also known as the flow front) if the resin has not reached the mold boundaries. After
solving for the fluid pressure, one calculates the fluid velocities, advances the resin front

based on the velocity field, and resolves for the pressure for the new domain. This procedure
is continued until the mold is filled. Thus, the quasi-steady state solution of the pressure
is dependent only on the instantaneous material properties and the boundary conditions,
which are functions of time.
Note that the justification of neglecting the transient terms in the equation of motion
follows from the fact that the kinematic viscosity of polymers is high and as the speeds are
low, the Reynolds number is low. However, the thermal diffusivity of polymers is low, so
the heat transfer is much slower and one cannot always ignore the transient terms in the
energy equation. The Prandtl number, which is the ratio of momentum transfer to energy
transfer, is very high for polymers, of the order of 100 or more. Thus, for non-isothermal
processes, one usually cannot ignore the transient term in the energy conservation equation.
5.5.2 Fully Developed Region and Entrance Effects

When a system variable does not change along a certain direction, one assumes that the
variable is "fully developed" with respect to that direction. For example, if the temperature
profile does not change along the x direction, one can physically assume that the tempera-
ture is fully developed along the x direction. Mathematically, one can express this condition
as dT/dx = 0.
"Fully developed flow and insignificant entrance effects" is a widely used assumption
while developing "process models" in polymer and polymer composites processing. This
assumption is again related to the rate of momentum transfer. The higher the kinematic
viscosity, the faster the momentum transfer will be and the sooner the velocity profile will
develop. For example, one can consider flow in a tube with a diameter D from a reservoir
or from a pressure pot as shown in Figure 5.11. The entrance region is the region in which
'//////^////////^////////^///////////^
A
Fully Developed Region
Developing Region
Figure 5.11: Development of velocity profile.
the flow profile is rearranging from plug flow to a parabolic profile for a viscous Newtonian
fluid. Usually, this region is proportional to the diameter of the tube and the Reynolds
number [238]
— = 0.054 Re. (5.94)
If the Reynolds number is less than one, the entrance effects last for less than the tube
diameter, and the assumption of fully developed flow will not influence the important physics
or the solution.
Similarly, if one wanted to assume a fully developed temperature profile along the flow
direction, the following criterion needs to be met [239]:
~ =• (0.03 to 0.04) RePr (5.95)

where Re and Pr are the Reynolds and Prandtl numbers. In composites processing, this
assumption is easy to justify for long tubes or long characteristic flow directions, but not for
short tubes as Pr can be of the order of 1000 for most materials. Also, if the temperature
boundary condition is changing with time, a fully developed temperature profile cannot be
easily justified. The other important number here is the Graetz number, Gz. When it is
small, one can assume that both the velocity and temperature profiles are developed in the
direction of flow.
Fully developed flow is a common assumption used in polymer and composites processing
as compared to the fully developed temperature profile due to low Reynolds number flows.
One of the most common situations in which fully developed flow is used is in conjunction
with the lubrication approximation that allows one to simplify the equations of motion
considerably and retain the important physics of the flow in the process model.
5.5.3 Lubrication Approximation

Osborne Reynolds [240] coined the term "lubrication approximation" when he was address-
ing hydrodynamic lubrication analysis. The key requirements to apply this theory are that
the flow should be viscous (the Reynolds number should be small) and flow should take
place in thin narrow gaps. While processing composites, one is dealing with parts that may
be meters in length and width but only millimeters in thickness. Hence, as they are also
low Reynolds number flows, we can employ the lubrication analysis to simplify the model.
- Actual gap height, h(x)
Tangential direction, x
f Approximate gap height, h(x)
Tangential direction, x
Figure 5.12: Approximation of flow in a thin gap using lubrication theory.
Let us review here how lubrication theory allows one to simplify the equations of motion
for a Newtonian viscous material. The conditions that should be met before applying this
analysis to a flow problem are
• The material should be incompressible.
• The flow should be isothermal.
• The Reynolds number should be less than one (that means the inertial forces should
be smaller than the viscous shear forces).
• The gap height should be very small compared to the in-plane dimensions.
• If the gap height is not a constant, it could vary very slowly with the in-plane dimen-
sions (for instance if the in-plane dimensions were x and y, dh/dx and dh/dy <C 1).

One also assumes that the material does not slip at the walls of the surface. A sketch
where the lubrication approximation will be appropriate is shown in Figure 5.12.
5.5.4 Thin Shell Approximation

If the "no slip at the boundaries" condition is not satisfied, it may be difficult to justify the
lubrication approximation. When you have full slip, it is possible to model the flow as plug
flow through the cavity thickness. For example, when one considers Darcy's law for flow
of thermoset resins through a network of fibers, one assumes a full slip boundary condition
along the mold surfaces. In such cases, it is the ratio of the square of the in-plane dimension
to the thickness multiplied by the ratio of the permeability in the thickness direction to that
of the in plane direction that dictates if one can ignore the flow in the thickness direction.
Hence, if
">2f«l (5.%)
one can ignore the flow in the thickness direction where t and L are the thickness and in-
plane dimensions, and K± and KL are the permeability components along these directions,
respectively.
5.6 Boundary Conditions for Flow Analysis

There are many types of boundary conditions that are encountered during processing of
composite materials. In this section, we will discuss how one models some of them.
5.6.1 In Contact with the Solid Surface

When the material is in contact with the solid surface, the modeler has three options for the
application of boundary condition for the velocity. They are (i) no slip (which implies that
the material sticks to the surface), (ii) partial slip, and (iii) complete slip. Mathematically,
one can express these conditions as a relationship between the velocity and the shear stress
as shown below
ux = -(3rxy (5.97)
where ux and rxy are the velocity and shear stress along the wall, and (3 is a weight coefficient
indicating the amount of slip (see Figure 5.13). When /3 — 0, Equation (5.97) reduces to
the no-slip boundary condition. A nonzero value for (3 implies partial slip. As j3 goes to
infinity, the boundary condition tends to full slip (however, ux is still finite because rxy
approaches zero).
Liquid resin .in the

Composite Material
Shear stress, txy Velocity, ux=-$1xy
Solid surface
Figure 5.13: Boundary condition (BC) along a solid surface.

5.6.2 In Contact with Other Fluid Surfaces
When the composite material with the resin in liquid form or the fiber suspension is in
contact with another fluid surface, one needs to specify the boundary condition at the
interface between the two fluids. Usually, one matches the velocities and the shear stresses
at the interface as shown in Figure 5.14.
= U2 (5.98)
(5.99)
where the subscripts denote the fluid domain.
tangent, t
(Continuity of velocities)
(Continuity of shear stresses)
Fluid 1
Figure 5.14: Boundary conditions along the interface of two fluids.
5.6.3 Free Surfaces

Sometimes, the viscous material in its liquid form will have a free surface. For example, in
the extrusion process, once the material leaves the die, the mass balance requirement alone
can cause the material to expand. When the material is in the die, one can use a no-slip
or slip boundary condition, but as soon as the material is free, one requires a different
boundary condition. Usually, normal stress equal to zero is used.
When the resin is impregnating a preform, or in injection or compression molding where
the flow front is pushing the air, one usually specifies a pressure boundary condition at the
flow front which is usually the atmospheric pressure, P = Patm, as shown in Figure 5.15.
5.6.4 No Flow out of the Solid Surface

For dies and molds in which the resin is injected, if one uses a slip boundary condition along
the wall, one usually specifies no flow out of the mold. Mathematically, this is represented
as
un = 0 (5.100)
where un is the velocity component normal to the mold wall as shown in Figure 5.15. If the
polymer flow is modeled with Darcy's law (u = —-VP), then Equation (5.100) is written
in terms of polymer pressure P as the primary unknown variable of the numerical solution.
Thus,

«„=() !
Dry preform =
un=0
Resin
= UN = nil = INI = mi = . . , , , ,
p— p = mi = mi = mi = ill! Vent to atmosphere
Resin injection or '"•
~mj
= P,
Figure 5,15: Boundary conditions along mold walls, on a free surface and at an injection
point.
where n and t are the normal and tangential directions to the wall.
5.6.5 Specified Conditions

Sometimes, either the flow rate Q or the pressure P at the inlet is specified:
P = -Hnlet (5.102)
or
Q = Q inlet (5.103)
an can
as shown in Figure 5.15. Pjniet d Qmiet be constant, or may vary with time.
5.6.6 Periodic Boundary Condition

At the microscale level, if one encounters a repetitive unit cell geometry, one can sometimes
apply a periodic boundary condition to estimate the unit cell properties. For example, if
one is interested in gauging the resistance to flow of a preform (inverse of permeability)
that has this repetitive structure, one could do so in two steps. First, a pressure gradient is
applied in the x direction, satisfying a periodicity in P and dP/dx along the upper and lower
edges of the unit cell. Pressure and velocity fields are solved numerically within the empty
channels of the fiber bed. By using 1-D Darcy law in the x direction, one can calculate the
effective permeability in the x direction, Kxx. A similar procedure can be repeated in the
y direction, as shown in Figure 5.16.
5.6.7 Temperature Boundary Conditions

The resin is either heated or cooled by the mold walls. One could specify one of the following
as the boundary condition at the walls:

Boundary conditions on unit cell to
calculate permeability in x direction:
P = f(x)
dPldy = g(x)
P=c+AP
= f(X)
Unit cell:
Boundary conditions on unit cell to

Warp 2 CM
calculate permeability in y direction:
1
P =c
P=q(y)
dPldx = dP/dx = r
I Warpt
Figure 5.16: Boundary conditions on a repetitive unit cell geometry [219].
• Fixed temperature (thermal contact) boundary condition, T = TW. This is used

when the composite material and the mold walls are in perfect contact. Then, the
temperature of the boundary of the composite is assumed to be the same as the wall
temperature, Tw.
• Fixed normal gradient boundary condition, dT/dn = c\. When the conductive
heat flux, q, is known between the composite material and the mold walls, then one
can use the 1-D heat conduction equation q = —kndT/dn where n is the normal
direction to the wall, and kn is the thermal conductivity of the composite in that
direction. Thus, one specifies the temperature gradient at the boundary instead of
the temperature.
• Relation between Tw and |^ known. When a fluid is used to heat or cool the
mold, one can express the boundary condition as h(T — TOO) — ~~^ n ^- at the wall.
Here, T^ is the fluid temperature, and h is the convective heat transfer coefficient
which is usually estimated from the fluid flow properties. This is done by relating the
Nusselt number (Nu=^p) to the Reynold and Prandtl numbers [239].
One can develop a general type of boundary condition as was done in [214] for a config-
uration as shown in Figure 5.17. Heating/cooling pipes are at a distance of a from the mold
wall. The heating/cooling fluid flowing through these pipes is at a temperature of TOO. The

corresponding effective boundary condition can be written as [214]
do (5.104)
dn
where 6 ~ T — TOO, and the effective boundary condition constant ( 'be is calculated as
Cbc = T (5.105)
.
km
Here, km is the conductivity of the mold material, h is the heat transfer coefficient between
heating/cooling fluid and the pipes, and k is given as
(kf + kr) + Vf(kf - kr)
K (5.106)
(kf - Vf(kf - kr)
where Vf is the fiber volume fraction of the preform, and kf and kr are the conductivity
of the fiber preform and resin, respectively. When the mold is insulated well (not much
heating or cooling), then Cic approaches zero. The fixed temperature (perfect thermal
contact) boundary condition corresponds to having a large value of C^c. This formulation
allows for the change in the mold surface temperature as experienced in practice. Due
to the exothermic chemical cure reaction of polymeric resin, the temperature of the resin
and hence the mold surface might increase away from the injection ports. Hence, this
formulation allows the modeler flexibility in specifying the boundary condition. Usually the
radiative boundary condition is not employed unless the temperature of the mold or that
of the surroundings is very high.
Heating/cooling fluid flow through pipes
Figure 5.17: Heating/cooling of composite material by circulating a fluid flowing through a

channel network machined inside the mold walls [241].
5.7 Convection of Variables

Temperature, cure and fiber orientation will usually convect with the flow, and one must
account for this phenomenon mathematically by using the material derivative instead of
the partial derivative (see Chapter 3). So, instead of %£, ^ and -^-, one would use
~Dt ~ ~8t + uai" + V~&U + w~^ where u, v and w are components of the velocity of the
moving fluid. Similarly, one would express any variable that is evolving during flow.

5.8 Process Models from Simplified Geometries
In composite manufacturing, one may fabricate simple geometries such as flat laminates
to very complicated net shape structures such as an I-beam of a passenger van or the keel
beam of a helicopter (see Figure 5.18). An ideal mathematical representation will stay
true to the actual physical geometry of the part. For complex geometries, one must resort
to numerical methods to meet this criterion. However, a simplified geometry model offers
many advantages, including the following:
• Basic understanding of the process being modeled with the least investment in time
and effort because it is possible to find analytic and closed form solutions.
• Ability to extract scaleable parameters from a simplified model.
• Ability to check the usefulness and validity of the phenomenological law or constitutive
equation that is used in the process model.
Figure 5.18: Mold filling simulations for complex composite structures. Different gray tones
indicate the location of resin front at different times during mold filling.
It is also possible to take simplified geometries and couple them to represent a complex
geometry. This may geometrically produce an approximate solution, but will be able to
address some of the complexities in the material modeling. Below, we will present results
for Newtonian and power-law fluids for selected simple cases that were studied earlier in
detail in Chapter 3.
Couette Flow
Couette flow is the flow in a rectangular channel induced by a moving upper boundary at
a constant speed V. The no-slip boundary condition is assumed at the lower and upper
solid walls. Hence, the resin velocity is zero and V at the lower and upper boundaries,
respectively. The velocity profile is found to be
ux(y} = — y . (5.107)
which is linear as shown in Figure 5.19.

Pulling speed
Figure 5.19: Velocity profile in a rectangular channel induced by a moving upper plate at
a constant velocity V (Couette flow).
Pressure Driven Flow in a Narrow Slit

This is the same as the previous Couette flow, except that both plates are fixed, but there
is a pressure drop applied between the two ends of the channel as shown in Figure 5.20.
The velocity profile is found to be
e l
ux(y] = (y2 - hy) (5.108)
which is shown in the same figure for Pe < P0.
%> Fixed plate 'y
Fluid
P = Pi
y\
//////////////
yy, Fixed plate
Figure 5.20: Velocity profile in a rectangular channel induced by a pressure drop in the
direction of flow (P; > Pe).
Pressure Driven Flow in a Capillary or a Tube

This is the same as the previous pressure driven flow in a narrow slit, except that the flow
is through a circular tube. The sketch and a typical velocity profile are shown in Figure
5.21. The velocity profile is found to be
(5.109)

which is parabolic, and shown in the same figure for Pe < Pi.
Circular tube
•r Fluid
x
= 2R
Figure 5.21: Velocity profile in a circular tube induced by a pressure drop in the direction
of flow (Pi > Pe).
One-Dimensional Flow in an Isotropic Porous Medium

In order to measure the permeability of a preform in the warp or the weft direction, two
separate one-dimensional experiments are done in those directions. A fluid is injected into
the mold from the left edge to fully saturate the fibrous preform as shown in Figure 5.22.
If the injection is carried out under a constant flow rate Q, then the injection pressure rises
Figure 5.22: One-dimensional flow in x direction in an isotropic porous media [54].
linearly as follows,
P(t) =
Kxx(l-Vf]
«_v (5.110)

where Kxx and Vf are the permeability in the flow direction and the fiber volume fraction of
the preform. Prom the slope of the graph of pressure vs. time, one can calculate permeability
as all other quantities are known.
Radial Flow in Anisotropic Porous Media

In order to measure the permeability of a preform, a radial injection experiment is done from
a tube at the center of the preform. The preform has a circular hole of radius R through
which the fluid enters. This ensures radial flow in the plane as shown in Figure 5.23. If the
preform is isotropic, then the flow front is circular. If it is anisotropic, then the flow front
is elliptical. The aspect ratio of the ellipse (the ratio of the major and minor axes) is equal
Figure 5.23: One-dimensional flow in radial direction in an isotropic porous media.
to the square root of the permeability components in those principal directions. If the fluid
is injected at a constant flow rate Q, then the injection pressure rises logarithmically
P(t] = ^Q
•^yy
where Kxx and Kyy are the permeability components in the major and minor axes, and h
is the mold cavity thickness.
5.8.1 Model Construction Based on Simple Geometries

Example 5.7: Radial Flow of a Newtonian Resin in a Preform
Consider radial flow of a Newtonian resin of viscosity /j, in a preform of isotropic permeability
as shown in Figure 5.23. The resin is made to flow through a plastic tube of radius Rt and
length L and impregnates the preform under a vacuum. Calculate the movement of the
flow front with time.
Solution
From Figure 5.23, we can see that there are two simple geometry flows involved: flow
through a tube and radial flow through the preform. At any time, the pressure difference
between the resin container and the location of the flow front is constant and equal to
(Patm — Pvac}- However, the pressure Pi at the inlet to the mold will vary with time, as the

flow rate into the mold will vary with time. However the flow rate in the tube has to equal
to the flow rate inside the preform at all times. Also we will assume quasi-steady state for
the flow. Hence, although Pi(t) at any instant in time, we will assume that fully developed
flow has been achieved at that time, t. Hence the flow rates in the two models will be as
follows:
Model 1: Tube flow (see Figure 5.24)
R.
Flow rate, Q
Figure 5.24: Tube flow.
Pgtm —
Qt — L
(5.112)
Model 2: Radial flow (see Figure 5.25)
u-
R
Figure 5.25: Radial flow in a preform.
JD
Qr = 2TTR—h(l - Vf) (5.113)
Although the flow rate, Qr may vary with time, at any given time it should be the same
for all r from r = R^ to r = R considering the conservation of mass (see Figure 5.25). Thus,
= ur(2irr)h. (5.114)
From Darcy's law
K_dP_
(5.115)
IJL dr
therefore
Qr = - (5.116)

Note that as Qr is constant with respect to r, we can integrate Equation (5.116) with respect
to r as follows:
f)rT i-Pvac
° OP. (5.117)
2irKhJRi r JPi
Thus
Pj-Pvac(2irKh\
( }
~ '
Equating Equations (5.112) and (5.118), and assuming Pvac — 0, one can find Pi as a
function of R, the location of the flow front.
Pii =
l&KLh
Now, flowrate in the preform is also equal to

jr>
Qr = 27T.R — (1 - Vf)h (5.120)
which is derived by taking the volume of resin in the mold and differentiating it with time
to obtain the flow rate.
Equating Equation (5.120) to Equation (5.112) and substituting Equation (5.119) for
Pi gives us a partial differential equation for R with respect to t:
TTRf
1- Patm. (5.121)
IQKLh
1 +-
The initial condition of R = Rt at t — 0 will allow one to determine R as a function of time.
5.9 Mathematical Tools for Simplification

Various mathematical tools can be used to simplify the governing equations and the bound-
ary conditions, in search of a solution to the process model constructed. As discussed in
[237], we will present four different ways to simplify equations whenever possible.
5.9.1 Transformation of Coordinates

An example of how to transform a coordinate system will be studied below to demonstrate
how one can simplify the calculations.

Figure 5.26: Flow through anisotropic (left) and isotropic (right) medium [223].
Example 5.8: Flow Through an Anisotropic Material

The flow of a liquid through a three-dimensional anisotropic material is shown in Figure
5.26. The three-dimensional Darcy's law is given by
dp
k
***xcr. k'xy
***' dx
dp
ky yy kyz (5.122)
k, kzz »y
op
The liquid is injected from a point source (denoted by O), and the shape of the flow front
is that of the surface of an ellipsoid with major axes forming angles 0^- with the axes of
a general coordinate system x,y,z. The permeability tensor for this case is in the form
used in Equation (5.122). After introducing a second coordinate system with axes x',y',z'
coinciding with the major axes of the ellipsoid, the permeability tensor reduces to the form
fci 0 0
*-] = 0 k-2 0 (5.123)
0 0 k3
where ^1,^2,^3 are the principal permeabilities of the fibrous material along the axes
x',y',z', respectively. After the principal permeabilities ki,k-2,k% are determined, the com-
ponents of the permeability tensor [K] in a general coordinate system can be obtained by
the transformation:
[K] = CT[K']C (5.124)
where C is the matrix of direction cosines of general coordinate axes x, y, z with respect
to the principal axes x',y',z'. To convert the original anisotropic medium into an isotropic
medium with reference permeability k, one can perform another transformation of coordi-
nates to new independent variables X, Y, Z defined by the relations [64, 242]:
2
k\^ 1/2
z
1/2
X=(^-} x',
- (5.125)

where k is a reference permeability. The volume element dx' dy' dz' transforms into
' 2 ] dX dY dZ and the reference permeability is selected such that
or
The result of these transformations is that the general problem of point injection in an
anisotropic medium is reduced to point injection in an isotropic medium with permeability
k = (kik^kz)1^ . The shape of the flow front in this case is that of a spherical surface (see
the image on the right of Figure 5.26). •
5.9.2 Superposition
Whenever the equations are linear, one can superimpose solutions. For example, when one
has a pressure driven flow and drag flow occuring in a cylindrical geometry, one can add
the solutions for the velocity profile to find the combined solution which is helical for this
case.
Example 5.9: Pulling a Fiber Through a Concentric Cylinder

Find the force required to pull a fiber of diameter d from a concentric cylinder containing
viscous polymer of diameter D as shown in Figure 5.27. The fiber is pulled with velocity
UQ . Assume L ^> D, d and that end effects are negligible. Only insignificant amounts of
polymer coat the fibers. Assume the polymer to be Newtonian.
Figure 5.27: Fiber being pulled through a concentric cylinder.
Solution
The important physics to understand here is that we have a combination of drag driven flow
and pressure driven flow. The pressure gradient is created because of flow being constrained
in the z direction. If one neglects the end effects, the velocity profile, uzd due to drag force
will be
(5.12T)
IliK \
as shown in Figure 5.27. Here K = d/D and RQ = D/2. Also Qj, the flow rate due to drag
flow will be
= 2-irR (R - R-}U ' ^ lu K ~ ^ + 1 (5.128)

4(1 — K) IUK

where Ri = d/2. The velocity profile, uzp and the flow rate Qp due to the pressure driven
flow are given by
R],_dP\ (5.129)
uzp = 1-
and
Q p = \ l - K (5.130)
dz
The uzp due to pressure driven flow is shown in Figure 5.28. Hence, the velocity profile in
the annulus is a superposition of drag flow and pressure driven flow as shown in Figure 5.28.
outer cylinder outer cylinder
I inner cylinder |
(a) drag flow (b) pressure driven flow
Figure 5.28: Velocity profile due to drag and pressure driven flow.
Note that we do not know — §f. However, we do know that total Q = 0. Thus,
Q = Qd + QP = 0. This allows one to solve for — ^j and substitute in equation for uzp.
Hence, the final steady-state fully developed velocity profile will be
Mr/RJ 3 (_£)
r
(5.131)
RO 4u V dz /
To find the force, one can calculate the shear stress along the fiber surface (Figure 5.29):
F = (27rRiL)Trz r=Ri. (5.132)
U
o
Figure 5.29: Shear stress along the fiber as it is pulled with velocity U0 from a concentric
cylinder.
For Newtonian fluids

duz
Trz = l (5.133)
~dr

Hence,
(ill
F = (27rRiL)v—^
or
9P
2 ( ^ 1 -^77^ }. (5.134)
,-Ko/
Thus one can use the superposition principle to solve difficult problems more elegantly.
5.9.3 Decoupling of Equations

A detailed process model often will involve a coupled, nonlinear system of equations if
there is more than one dependent variable. If the coupling between the equations and the
dependent variables is strong, one has to solve all the variables simultaneously. This can
be an effort and time intensive project and also difficult to prove that the mathematics will
be stable under all conditions. However, if the equations are weakly coupled, one can solve
them in succession.
For example, in nonisothermal models for injection molding, the momentum equations
are coupled with the energy equation. The coupling will be strong if viscosity is a strong
function of temperature (which makes the viscosity in the momentum equation a function of
the temperature, the primary variable in the energy equation) and if there is a substantial
amount of energy dissipation due to viscous heating (which makes the temperature depend
on the viscosity and the shear stresses). The strength of the coupling is estimated by
the Brinkman and Nannie-Griffith numbers (see Table 5.1). Large Brinkman and Nahme-
Grimth numbers would imply that one must solve for momentum and energy equations
simultaneously using an iterative or a direct solver. A small value for these numbers would
signify that it is a justifiable approximation to solve the momentum equation first and then
use the viscosity and the calculated shear stresses in the energy equation to solve for the
temperature. Thus, the solution is decoupled. If the Brinkman number is small, it implies
that one can solve the energy equation first (if there is not much convection) and then solve
for the momentum equation.
Example 5.10: Nonisothermal Flow of a Viscous Suspension in a Channel

Consider nonisothermal flow of a viscous suspension in a channel (Figure 5.30). The con-
servation of mass, momentum and energy equations are in general coupled and nonlinear.
The viscosity of the suspension is temperature dependent. Under what conditions can we
decouple the equations and simplify the solutions for velocity, pressure and temperature?
Assume flow is in the x direction only and t] — rjoe~^T~To> where t]o is the viscosity at
reference temperature TQ.
Solution
There are four temperature scales here [63]:
• AT = (Tj — TU,), temperature difference between entering and wall temperature.
• The inverse of £, which has temperature units.

Wall temperature, Tw
*" Flow rate, Q
Entering
temperature, Tt
Figure 5.30: Nonisothermal flow between parallel plates.
H
„/ V 1
• Temperature rise k ' due to the balance of dissipation and conduction across the
thickness, H. Here k is the thermal conductivity of the suspension.
• Temperature rise J^WH* ûe ^° ê balance of viscous dissipation and axial convection
along the flow direction. Here p and cp are the density and the heat capacity of the
suspension, respectively.
Hence the three dimensionless numbers listed in Table 5.1 are important:
kWL 4fcW 2 £T 2 |AT|'

Now if Gz<C 1 and Na«C 1, this implies that transverse conduction dominates axial con-
vection, so the temperature field is fully developed, and thus the entry temperature Tj
is irrelevant and Br is of no consequence. Because Na<C 1, the effect of heat generation
is too small to change the viscosity significantly. Hence one can completely decouple the
momentum and energy equations.
If Gz» 1, Na<IC 1, the temperature field is underdeveloped and the transverse conduction
is unimportant, one can assume adiabatic conditions and ignore Tj.
When Gz^> 1, Na^> 1, the temperature field is underdeveloped and transverse conduc-
tion is important in a thin boundary layer by the wall.
When Gz<C 1 and Na3> 1, the temperature field is fully developed, but as Na^> 1, the
heat generation does influence the viscosity; hence the equations are coupled. •
5.10 Solution Methods

After the governing equations and the corresponding boundary conditions are formulated
and have been simplified to the satisfaction of the modeler, the next step is to select a
solution method to predict how the dependent governing variables behave as a function
of the independent variables. The solution method can range from a simple back-of-the-
envelope calculation to very sophisticated numerical algorithms. The choice of the method
will depend on
• the type of governing equation

• if it is an ordinary differential equation or a partial differential equation
• whether the equation or the boundary conditions are linear or non-linear
• if the geometry is simple such as a pipe or a straight channel, or complex with inserts
and ribs
• the number of variables that need to be solved, and if there is weak or strong coupling
between them
• the nature and the stability of constitutive equations used.
One can broadly divide solution methods into two categories: closed form solutions
and numerical solutions. In most situations of practical interest, one will have to resort
to a numerical solution, but an analytic or a closed form solution should not be dismissed
altogether. There are many situations in which the availability of a closed form solution
can be beneficial. We will first discuss the merits and situations for which one might want
to seek a closed form solution and then discuss briefly the merits and pitfalls of computer
modeling with numerical methods.
5.10.1 Closed Form Solutions

Analytic and closed form solutions can be very useful in gaining insight into the physical
processes occurring during composite manufacturing operations without unnecessary confu-
sion caused by excessive geometric complexity or inclusion of detailed secondary influences
in the equations. Simplified geometry models can reveal phenomena that can be easily
missed by numerical solutions. Flow and heat transfer in a narrow gap provides a good
example. Under certain combinations of the Graetz, Nahme-Grifnth and Pearson numbers,
the temperature and velocity profiles change rapidly inside the thin boundary layer near
the wall [235]. A numerical solution will miss this layer unless the mesh or the grid is made
extremely fine. Secondly, analytic solutions can be used as benchmarks for verification of
sophisticated numerical solutions. Thirdly, closed form solutions can allow the modeler to
easily recognize the nondimensional parameters and the approach to scale the process from
the laboratory to the production scale. Finally, analytic solutions are often easy to con-
struct and hence inexpensive in terms of time and computer resources. This makes them
attractive for use in design and optimization of the process and material parameters as one
can carry out many solutions by varying the parameters quickly. Also, if one is interested
in on-line control of the process, the availability of instant prediction of the variables for
the next time step makes it possible to integrate the solution with the strategic or tactile
controller of the process. This allows the controller to compare the predictive behavior with
the actual behavior and make adjustments to the process parameters to drive it towards a
successful outcome.
The analytic solution usually comes at the price of simplifying the geometry and/or
the governing equations. A skillful modeler will make sure that the important physics is
retained during these simplifications. It is usually easy to identify simplified geometric rep-
resentations. For example, many molding operations involve flow through narrow confined
channels [63]. Usually these channels will involve basic simple geometries. The four most
common ones are listed below.
(a) Pipe or tube:
5 135
u, =
?(-£)
4/j,\dzJ <- >
dP AP PR - R
(5.136)
L
dP
Q = (5.137)
(b) Channel or parallel plates:
(5.138)
h 8/i V dx
dP AP
(5.139)
L
9.
W
= (5.140)
(c) Radial driven flow in a disk:
(5.141)
4/j.rh
dP
(5.142)
dr TT
P(r) = Pi- (5.143)
P = Pi at r = Ri. Solution not valid near r = 0. (5.144)
(d) Pressure driven flow in an annulus:
1-
v, = 1- (r/Ro) (5.145)
ln(l//e) dz J
5PN
Q = 1-K4- 4
(5.146)
8/j, \ dz J
where
dP AP _ Pe-Pj
(5.147)
~T ~
K —
_ (5.148)
R0
(e) Tangential annular drag flow between two concentric cylinders where the outer cylin-
der is rotating with angular velocity fi:
— fir where K = (5.149)

(i)'

(f) Axial annular drag flow between two concentric cylinder where the minor cylinder is
being dragged with velocity UQ:
2K2 In K - K2 + 1
Q = 2nR0(R0-Ri)u0 (5.151)
4(1 — K) In K
The assumptions made are as follows:

1. A long circular pipe of length L and radius R, where R -C L.
2. A long and wide rectangular channel of length L, width W and thickness /i, where
h <C L and h <C W, which allows one to approximate the channel as two parallel flat
plates.
3. A concentric disk of inner radius Ri and outer radius R0 and height h <C (R0 — Ri), so
that one can ignore inertia and elastic effects if present, and consider the radial flow
as one-dimensional.
4. A long, concentric annulus of length L, inner radius Ri and outer radius R0 <C L. If
the common additional assumption that (R0 — Ri) -C Ri is also made, the annulus
can be unrolled into a channel of length L, width n(R0 + Ri) and height of (R0 — Ri).
One can increase the range of shapes that can be modeled if one of the dimensions varies
slowly along one of the coordinate directions. For example, one can model a conical shape
as a slowly varying pipe in the z direction (i.e. if dR/dz <C 1), and a wedge shape can be
represented by a slowly varying channel, etc. Such simplifications with obvious choice of
the coordinate system can lead to closed form solutions as long as the governing equations
and the boundary conditions are linear.
5.11 Numerical Methods

It is almost routine to see polymer composites being processed into complex shapes. It
may be necessary to represent these shapes accurately to capture the important physics
especially around inserts and corners during such composites manufacturing operations.
This usually will require the governing equations to be solved numerically. Sometimes even
the geometric simplification can be assumed, but the nonlinearity in the governing equations
and boundary conditions will warrant a numerical solution. Finite difference, finite element,
boundary element and spectral methods are some of the numerical methods that are used to
obtain a solution. Each of these methods has its own particular strengths and weaknesses.
We will not discuss the details of each method, but refer the reader to Chapters 6-8 of the
computer modeling by [243] for background and demonstration of its applications. In this
section, we will highlight some of the important characteristics of each method and state
their strengths and weaknesses.
All numerical methods use discrete values at selected locations in space called nodes to
represent the continuous solution of the field variables such as pressure, velocity and tem-
perature over the geometry, or the domain of interest. Finite elements and spectral elements
can represent virtually any geometry and there are many finite element and spectral element
codes that use mesh generation modules to speed the development of the mesh, allowing
the modeler to build the discrete representation of the domain. Mesh generators are very

effective tools for two-dimensional domains, but building and verifying three-dimensional
domains can still be time consuming. Boundary element methods can be very attractive for
three-dimensional problems as in such methods only the boundary of the domain (which will
be only a two-dimensional surface), and not the complete domain, needs to be discretized.
However, in the boundary element formulation, the differential equation must first be
transformed into an integral equation over the domain boundary. The transformation is
straightforward if one knows the kernel solution or Green's function for the differential
equation. Without the kernel solution, there can be no boundary element solution. Usu-
ally, when there are nonlinearities in the material properties or the governing equations,
either one does not have a kernel solution or one has to convert the nonlinearities into a
body force term which requires some sort of discretization over the domain, eliminating the
major advantage of boundary elements. While traditional finite difference methods can eas-
ily handle domains that are two-dimensional rectangles and three-dimensional boxes, they
cannot model complicated shapes. Numerical grid generation and finite volume methods
remove some of these obstacles, but are still far from being able to handle multiple con-
nected domains. For example, finite difference may be able to handle a rectangular domain
with one circular insert in it as it is a simply connected domain. But if it had two or more
inserts, it will not be able to represent this with ease as finite element or spectral methods
can. Hence, finite difference methods require formidable effort to model complex shapes,
but they are very useful in developing solutions with new equations in simple geometries,
as they take the least amount of time, and are very easy to implement.
Mesh refinement locally and globally is an issue that can be easily handled by finite
elements and spectral methods. Finite element modeling discretizes the governing variable
either linearly or with a second order polynomial over the element. So, by refining the mesh
and making the elements smaller and smaller, one will be able to approach the continu-
ous solution more accurately especially if the solution varies rapidly over the domain. Some
problems however have regions where the field variables change rapidly combined with large
regions where the field variables change slowly. Obtaining an accurate solution in such cases
requires a fine mesh in the region where the variable is expected to change rapidly and a
coarse mesh in the rest of the domain. Spectral methods usually use a coarse mesh but a
very high polynomial to interpolate over the coarse element, and therefore can capture the
rapidly varying variables with ease. Many composites processing models exhibit nonlinear-
ity. Nonlinearity can enter governing equations through nonlinear terms in the equations
such as a convective term in the momentum equation, through material properties that de-
pend on field variables of the governing equations, such as temperature-dependent viscosity,
through nonlinear constitutive equations or boundary conditions that may be nonlinear.
Finite element methods are the most powerful methods for nonlinear problems, especially
when solving the equations with the Newton-Raphson or one of its variant methods. The
solution will usually converge rapidly, but requires additional programming to implement
the method.
The overall recommendations once you have a model for the process at hand are as
follows:
1. To solve a moving boundary problem, use the method most suited to handle moving
boundaries.
2. For geometrically simple domains and to develop a quick solution for new equations,
use finite difference methods.
3. There are many packages available that can solve general fluid flow and heat transfer
problems, and one can modify the process model such that one can use the multi-
purpose code to find the governing field variables. Some of these codes will allow you

to input your own subroutines for viscosity and cure kinetics. Whenever possible, one
should use this approach.
5.12 Validation
Almost all process models that are developed involve one or more assumptions, and many of
them use constitutive or phenomenological equations to represent material behavior. Thus,
it is important to do a reality check and see if the model predictions agree with experiments.
Hence, there is a need for validation.
If a simulation of a model has been developed, it can provide many details such as
the pressure and temperature distribution, fiber orientation state at every location, etc.
However, one can only measure finite quantities from an experiment. Hence, the choice of
which variables to measure and where to measure them become important considerations.
5.12.1 Various Approaches for Validation

There are many ways in which one can validate the model. One may choose to monitor the
history of just one of the governing variables in the experiment, or all the field variables and
compare them directly with the predictions. For example, one may monitor the temperature
of the resin at the midpoint of the mold as a function of time in the injection molding process
and compare it with the predictions from nonisothermal simulations. Another approach may
be to indirectly compare experimental findings with predictions. For example, in curing of
a thermoset composite, one may monitor the final state of the cure after the composite is
demolded by performing DSC analysis on various samples that are cut from the fabricated
composite, and compare the resulting cure distribution with the predictions of the model.
So, although it does not validate the dynamics of the cure process, it allows one to compare
the final cure state after demolding. A similar approach can be adopted for verification of
the model for prediction of the cystallization state or fiber orientation state.
However, it is important to compare apples with apples when performing validation
experiments. For example, let's consider the issue of validating the model for flow induced
fiber orientation. To accomplish this, a simulation of injection mold filling is performed,
and fiber orientation is predicted. The simulation is based on assumptions of no variations
in fiber concentration and fiber length distribution and a constitutive rheological model.
Next, the results are compared with the fiber orientation state measured from injection
molded samples. This is not a good validation of the flow induced fiber orientation model
as in the experiment there are many other parameters such as fountain flow, fiber length
distribution, etc., that may have influenced the fiber orientation pattern which were not
accounted for in the simulation. However, if one created a suspension of fibers in simple
shear flow or other well defined flows, and measured the orientation of the fibers in such
flows, without complications introduced due to other assumptions, it will help validate the
flow induced fiber orientation model. Moreover, it will also elucidate fiber-fiber interactions,
which could lead to refinement of the model.
Hence, the type of experiment is also an important factor in validation studies of the
formulated process model. Process models usually consist of many phenomena and sub-
steps with assumptions at every sublevel. If possible, one should try to validate every
submodel independent of the overall model. For example, in filament winding, there are
many submodels such as thermochemical, fiber motion, stress and void models. It will be
useful to independently validate these models, instead of just comparing the final predicted
mechanical properties with the measured properties. However, it is sometimes not feasible

to validate every submodel, in which case, one may want to consider indirect validation of
such submodels.
It is also crucial to validate the overall process model, in addition to validating individual
submodels, as it sheds light on the accuracy to which one has modeled the interactions
between the various submodels. One may validate every submodel of the process model
and assume that the process model is validated, but there may be assumptions about the
interactions between the submodels that may not have been verified. Thus, the validation of
a process model is not complete until one also validates the final results with the predictions.
If the,model predictions agree with the experiments, one has created a successful model
that can be used for design, manufacturing and control situations instead of trial and
error approaches. However, there will be many situations in which the predictions and
the experimental results won't agree. In such cases, what should be the next step for the
modeler?
The modeler should revisit his or her assumptions and make sure the validation exper-
iments honor those assumptions. By this time, the modeler should have also verified that
the simulation or the model has been verified with a closed form solution or with mesh
refinements. Next, the modeler should question the constitutive law that is being used to
represent the phenomena. Sometimes, the modeler can learn from the experiments that
will allow him or her to modify the law based on further physical insight. For example,
if the model is using a power-law fluid to represent the material behavior, and the experi-
ment involves very low shear rates, the experimental results and predictions won't match.
This may be because the experiments involved very low shear rates, and we know that the
power-law fluid model will not do a good job of capturing the physics. One may have to
refine the model by using a Carreau fluid.
In the same way, we may have represented the fiber-fiber interaction with a constant
parameter in a flow-induced fiber orientation model. However, the model experiments may
show that the expected orientation behavior seems to be slightly off from the predictions.
This may induce the modeler to think that maybe the interactions cannot be constant under
all fiber orientation states. One would expect the fiber-fiber interactions to be higher when
the orientation state is in complete disarray or random as compared to when all the fibers
are aligned. Thus, the modeler can use this insight to improve the fiber orientation model.
Usually, models can be improved or refined at the expense of including more material
parameters. For example, in the cases suggested above when we go from power-law to
Carreau fluid, we need three parameters instead of two. Similarly, if we make the fiber
interaction parameter dependent on orientation, we may need an additional equation that
will allow us to determine this relationship. At other times, one may need to completely
reformulate the constitutive law to accommodate the new phenomena being observed. For
example, a random fiber preform clearly obeys Darcy's law as it has been validated many
times. However, some of the stitched or tightly woven fabrics have two scales of pores:
very small ones between fibers and large ones between fiber tows as shown in Figure 5.31.
Thus, when the fluid impregnates these preforms, the pores between the fiber tows are
filled at a much earlier time than the smaller pores between the fibers. This would require
reformulation of the model as one has discovered that the saturation of the porous medium
is not instantenous as in random preforms.
Sometimes, the culprit may be the incorrect application of the boundary condition or an
unknown boundary condition. For example, if one has a convective heat transfer boundary
condition on the outside of the mold, one would have to specify a convective heat transfer
coefficient which itself requires a constitutive law. One tip is to create validation experiments
that do not use this boundary condition, instead using specified temperature or heat flux.
Thus, this chapter has discussed tools and approaches that help build a process model

and create a simulation. The next three chapters will focus on implementation of some of
these tools in formulating models for polymer composite manufacturing processes.
Figure 5.31: (a) Schematic of a simple porous medium exhibiting a single length scale, (b)
Schematic cross section of a woven fabric unit cell, demonstrating the dual length scale
porous medium.
5.13 Exercises
5.13.1 Questions
1. What are the advantages of using a mathematical model and its analytical or nu-
merical solution, compared to relying on a trial and error approach during composite
manufacturing?
2. What are the main ingredients of a mathematical model of a manufacturing process?
3. What are the major steps in developing a model? In order to rely on the results of a
model, what criteria should be satisfied?
4. Should models be accepted as representing the real process exactly?
5. Why do modelers usually make simplifying assumptions in their models instead of
retaining all the physical details? How can a skilled modeler decide on which simpli-
fications are acceptable?
6. Why do modelers need to verify and validate their models with controlled experi-
ments? What is the difference between validation and verification?
7. What are the important considerations when comparing results from a model with
the experiments?
8. Can a model be a good representation of a physical manufacturing process used in
one production plant but not in a different plant? If so, do you need to adjust your
model? How?
9. Is there a unique model for a particular process?

10. Does a higher number of parameters in the constitutive equation translate into greater
accuracy of the model?
11. If there is more than one model available for a particular process, how would you
determine which one to use?
12. Compare the advantages/disadvantages of sophisticated models without simplification
that require numerical solution with simplified models with closed form solutions.
13. Explain what this means: "Virtual composite manufacturing scenarios based on mod-
els are very useful mold and process design tools." Give some examples.
14. Suppose that you are asked to design a mold for resin transfer molding (RT'M) process
for a given part geometry using a numerical mold filling simulation, (i) What material
property data do you need in the model? (ii) Is the accuracy of that data important
for your design? (iii) If you use this data from a database, is it necessary to question
under what conditions the data was obtained?
15. For exactly the same part dimensions, can there be completely different mold and
process designs? Explain this by considering the requirements of two different indus-
tries such as aerospace and automotive.
16. Suppose that two simulations are available for mold filling in the RTM, one is for 2-D
flow and the other one is 3-D. What is the advantage of using a 2-D model over 3-D?
Under what conditions should you use a 3-D model?
17. When do you need to use constitutive equations for resin viscosity?
18. Considering the polymeric suspension flow between the extruder screw and barrel,
(i) how can you model the geometry of the flow channel? (ii) What simplifications
are possible in the conservation of momentum and energy equations? (iii) How does
the velocity profile change if the resin material property a (that appears in /j, —
p10e~a(T~T':ef') and the temperature difference between the barrel and screw, change?
19. Why is dimensionless analysis very useful? How does one decide in choosing char-
acteric values? Can there be more than one characteristic length value in the same
analysis? How does one decide what terms to drop in a governing differential equa-
tion?
20. What dimensionless numbers are commonly used in isothermal composite processing?
21. What are the major advantages/disadvantages of different numerical methods such as
finite difference, finite element, finite volume and boundary element methods, to ob-
tain solutions to mathematical models? How would you treat moving free boundaries
such as free surface of a liquid composite material impregnating a mold containing
fiber preforms?
22. Under what conditions (in terms of values of some dimensionless numbers), is quasi-
steady state assumption acceptable?
23. If a quasi-steady state assumption is used in a model of the mold filling process, how
would you solve the resin flow front location as a function of time?
24. What does "fully developed velocity" mean?

25. If the flow of a polymer through a circular tube has a Reynolds number of 1, what is
the approximate length of the velocity developing region (in terms of tube diameter)?
What is the approximate length of the thermal developing region (in terms of tube
diameter) if the Prandtl number is 1000?
26. What do the Reynolds, Prandtl, Brinkman, Froude and Graetz numbers represent
physically?
27. Under what conditions can the lubrication approximation be applicable?
28. Under what condition can one ignore the flow in the thickness direction within the
thin shell approximation? Do you compare only the ratio of the dimesions in the
thickness and in-plane directions, or are there additional considerations?
29. What are the boundary conditions, in mathematical form, if the liquid composite
material has a contact with a solid surface with no/partial/full slip? Explain your
answer in terms of the tangential and normal components of velocity.
30. If the liquid composite material has contact with another fluid, what is the corre-
sponding boundary condition along the interface?
31. What boundary condition is used on the free surface as the liquid composite material
(fiber suspension) propogates within a mold? Does your answer depend on whether the
free surface is directly connected to a ventilation tube to outside air? For example,
if the flow front traps some air not directly connected to a vent, what boundary
condition can be applied on that free surface?
32. What different boundary conditions can be used at the injection ports?
33. When are periodic boundary conditions assumed? Give examples.
34. Explain what these thermal boundary conditions physically correspond to (i) fixed
T = Tw, (ii) fixed normal gradient dT/dn = ci, and (iii) difference of temperatures
=
•* J- surroundings
ngs C2 .
35. What are the mathematical tools to simplify governing differential equations and
boundary conditions? Explain briefly.
5.13.2 Problems
1. Consider a large polymeric composite plate with a thickness of 2cm. Suppose that one
would like to cool it from 300°C down to 70°C. The top and bottom surfaces of the
composite are kept in perfect thermal contact with an aluminum tool at Tw = 25°C.
Considering typical composite material data, how long should the part be kept in the
mold?
2. Considering flow through a circular tube, what dimensions and properties of the prob-
lem do you need in order to calculate the length of the entrance region? When is this
length significant?
3. For what values of Graetz number, Gz, are velocity and temperature profiles assumed
to be developed in the direction of flow in a tube? Explain.

4. In flow modeling, a thin shell approximation is often used in order to simplify and
speed up the computation. What are the criteria for this approximation to be valid?
If the thickness of the composite part is much less than the in-plane dimensions, can
you always use this approximation? Explain.
5. Consider Example 5.9. If there are two setups in which K\ — d\/D = 0.7 and
KI = di/D — 0.8, find the ratio of required forces to pull the two cylinders. Leave
your result in terms of JJL, U0 and D only.
6. What simplified flow problems can be useful for Newtonian fluids while studying flow
of liquid composite material through narrow channels? What are the corresponding
closed form solutions for velocity profiles?

Chapter 6
Short Fiber Composites
6.1 Introduction
The polymer processing industry creates at least 30% of the objects that we see around
us. There is a good chance that these objects were fabricated using one of the following
three manufacturing processes: extrusion, injection molding or compression molding. They
are all high volume production processes. Extrusion is a continuous process, injection
molding is an automated process and compression molding is a semiautomated process but
can manufacture large and complex parts that cannot be easily accomplished by injection
molding or extrusion. Most of the components fabricated are for nonstructural applications
as the polymer structure can withstand only a limited amount of load and stress.
These methods were also being used to process food which had solid particles imbedded
in a viscous fluid. Hence it was natural to extend these manufacturing methods to process
fiber suspensions as well. Fiber suspensions refer to chopped fibers suspended in a polymer
melt. Compression molding involved placing the material containing fibers and resin in a
solid form called the charge inside the mold cavity. Usually, the heat conduction mode is
employed to heat the charge by direct contact with the mold platen to melt the polymer
and create a suspension of fibers in the polymer melt. This suspension is compressed by
the platen to occupy the mold and take the form of the mold cavity. After solidification,
the part is removed from the mold. Unlike compression molding, which uses a mold platen
to melt and displace the material, the extrusion and injection molding process use a screw
to melt and move the material. The function of the screw in both these processes is similar
to some extent during preparation of the suspension. Examples of screws used are shown
in Figure 6.1.
The screw by its rotation can generate shear flow which causes viscous dissipation that
melts the polymer and mixes the fibers with the polymer melt at the same time. The
screw also acts as a pump that can push the polymer melt suspension into a die during the
extrusion process, or into a mold during the injection molding process. However, modifica-
tions need to be made to the screw material and design to ensure that it can withstand the
abrasive environment created by the fibers. The channel depth of the screw is also usually
increased to avoid excessive fiber length attrition, as fiber length plays a crucial role in load
transfer.
The goal of the screw is to produce a well-mixed suspension suitable for forming op-
erations. In extrusion, the suspension is pumped through an opening into a die to form
a continuous product, whereas in injection molding the suspension enters a mold through
one or more inlet gates and takes the shape of the mold. In extrusion, one does not need

Constant-pitch metering screw
Feed section Transition section Metering section
Varying-pitch flighted mixing head
Figure 6.1: Examples of screws used in extrusion and injection molding for mixing and
pumping the fiber suspension into a die or a mold [102].
Assign suspension
properties
v V
Calculate Newtonian
flow field (or input
initial guess)
r v ^ ^
Output velocity and Calculate orientation
orientation values states based on
streamlines
j
\
r ^
Update Theological
properties of the
suspension
^ )
Calculate flow field

based on new
properties
V }
_—-— ^^\~~~~~~.
•-> Decoupled Solution
Output velocity and
-*• Coupled Solution orientation values
Figure 6.2: Decoupled and coupled solution approaches to describe the flow and fiber ori-
entation in a fiber suspension [244, 245].

vents to let the displaced air out, whereas in the injection mold one must provide vents for
the displaced air to exit. On the other hand, compression molding does not involve gates
but requires the material, that will fill the mold cavity, to be preplaced in the mold and
squeezed until the top and bottom mold platen meet. During this process there is much
less attrition of the fibers as the material is not subjected to large-scale deformations.
All the above processes involve flow of fibers along with the polymer melt to form the
shape of the die or the mold. It is important to know how these suspensions flow into the
mold or the die as the final properties of the product are determined by the flow history
and the orientation state of the fibers when the polymer melt solidifies.
The solution methodology to calculate the flow and fiber orientation states is shown in
Figure 6.2. There are two approaches: (i) decoupled and (ii) coupled. In the decoupled
approach, the flow field is assumed to be unaffected by the presence of fibers.
In this chapter, we will first present the modeling of flow and heat transfer in the
compression molding process. Next, we will briefly discuss the screw design in the extrusion
process and present an analysis to calculate the pressure drop and flow rate relationship
due to the presence of the die. Finally, in injection molding, we will focus on modeling the
filling stage in the mold.
6.2 Compression Molding

Compression molding is one of the oldest technologies for processing polymers and hence
was a natural candidate to manufacture near-net shaped, thin-walled composite parts at
relatively low costs [246, 247].
6.2.1 Basic Processing Steps [I]

While there may be slight variations in this process, the basic steps can be defined as fol-
lows. First, during the material preparation stage, premeasured raw material, or "charge,"
is placed inside a preheated matched-die mold. The raw material can be either sheet mold-
ing compound (SMC), bulk molding compound (BMC), long fiber-reinforced thermoplastic
sheets (LFTs) or glass-mat thermoplastics (GMTs). Polypropylene is usually the resin used
in thermoplastic systems such as LFT and GMT [248, 249, 250]. SMC has been the widely
used material because of its versatility [247, 251, 252]. SMC, which has been used since the
early 1950s [248] is the generic name of a broad class of thermosetting resins reinforced by
randomly oriented chopped fibers. Uncured SMC sheets are typically 4-6 mm thick with
fibers 25 mm long. These are fiber bundles consisting of around 200 filaments each. Fiber
volume fraction is 20-50%, while resin makes up 30% of the volume. The remainder of the
bulk is comprised of mineral fillers such as calcium carbonate which are used to thicken
the resin paste [247, 18]. Resin matrices used include unsaturated polyester, vinyl esters,
epoxy, and phenolics [247, 251, 18, 249, 253]. Unlike SMCs which are in the form of sheets,
BMCs are available as a gunk or soft log with typically low fiber contents (approximately
20%) along with a particulate mineral filler. There is a variation that uses chopped resin-
coated fibers containing only the fiber reinforcement and no fillers [247]. Most of these
material systems are reinforced with glass fibers. Limited compression molding is done
with carbon-BMI and epoxy prepregs, and with carbon-epoxy BMCs and SMCs.
Once the charge is placed inside the mold cavity, then the two halves of the mold are
closed to heat the resin paste and pressure is applied through a hydraulic press, causing the
resin to flow and be squeezed into the shape of the mold cavity. The mold platens move
towards each other until they meet. After the mold has been filled, the part is allowed to

cure before it is cooled, then removed from the mold and possibly trimmed to remove flash
[247, 251, 18].
There are slight variations in compression molding of thermoplastics. The obvious one
is that no curing is necessary. Also, as thermoplastics are more viscous than thermosets,
one usually requires higher pressures to make the material flow into the mold cavity. Ther-
moplastic composites are also used in compression molding operations such as stamping
and forming where the flow is usually insignificant. In stamping, or rapid compression
molding, the charge covers 95-98% of the mold cavity; hence the flow is insignificant and
the fiber orientation within the material is retained. Stretch compression molding, wherein
the heated sheet is clamped in a frame and forced to stretch as it changes shape, is another
variation of compression molding of thermoplastic composites [254].
Mold temperatures range between 135 and 160°C for thermoset materials [247, 251],
whereas it has to be above the material's melt temperature if thermoplastics are used. Heat
is usually supplied by pumping hot oil or by condensing saturated steam in heating lines
drilled through the mold platens [251]. Press speeds are typically 5-10 mm/s while the
applied pressure is in the range of 3.5-15 MPa [247, 251, 254]. Cure usually takes only 30-
40 seconds and the entire cycle time can range from under a minute to 6 minutes, depending
on the degree of automation incorporated into the process [247, 251, 248].
A recent variation of the compression molding process is the injection-compression mold-
ing process which combines conventional injection molding and compression molding to in-
corporate the advantages of both manufacturing processes. The resin is introduced into the
cavity with the mold platen separated by a larger gap than the thickness of the part. Hence,
the pressure requirement for injection is low. After injection is completed, the suspension
is compressed to close the gap to the desired thickness of the part. The advantage of this
process is that it can be done under low molding pressures which reduces residual stresses,
sink marks, warpage, and density variations, and improves dimensional accuracy. However,
the process has not been popular as the control required in processing is more complex and
would require substantial investments in equipment to automate the process [255].
6.2.2 Applications [1]

Compression-molded parts are usually used in the automotive industries where high-volume
production of moderately strong, stiff, corrosion resistant, lightweight parts with good sur-
face finish and short processing times are needed [251, 252]. The process is particularly
suitable for handling fiber-reinforced materials with high reinforcement loadings as longer
fibers can be used in compression molding than in injection molding [253, 256]: Automo-
tive body panels have been the primary application for compression molded components
[251, 18, 249, 253]. For example, the front end of the Ford Galaxy and VW Sharan are com-
pression molded from SMC while the Passat's is made from LFT. VW's Golf II has a GMT
inner front end [248]. Pickup truck boxes and certain components of the tailgate are made
from vinyl ester SMC. Several automatic transmission components are compression-molded
from phenolic materials while compression-molded epoxy SMC is used in other more stressed
components. Large floor components for a station wagon are also compression-molded from
polypropylene GMT [251, 18, 249, 253]. The first structural application in automobiles
was a leaf spring in 1979 made using continuous unidirectional glass fibers. The latest
automotive use is for a composite wheel [247].
In aerospace applications, compression-molded components are usually used only in
secondary structural or nonstructural parts as short fibers and low volume fractions do not
meet the mechanical property requirements for primary structures. In commercial aircraft, a
number of covers, fairings, panels and housings are compression-molded from epoxy SMC to

replace aluminum parts. Wings, control surfaces, bulkheads and nose cones are made from
high content epoxy. Phenolic SMC and some thermoplastic materials with their superior
high temperature and smoke generation properties are currently being evaluated for future
aircraft applications [247].
Consumer industries also utilize compression-molded short fiber polymer composite com-
ponents. For example, several office copiers utilize compression-molded end caps on the
copier fusor roll. Embossing dies and counter dies are compression molded from phenolic
rubber mats and from epoxy SMC. Even major elements of a centrifugal pump are com-
pression molded from glass-reinforced epoxy or vinyl ester SMC [247]. Lamp housings have
been reported to be compression molded as well [248].
6.2.3 Flow Modeling

Compression molding involves a modest amount of flow. Although the amount of flow may
be small, it is critical to the quality of the part. The flow will control the orientation
of the fibers, will influence the heat transfer and hence the curing of the composite, and
will also influence the material properties if weld (knit) lines are formed (where flow fronts
meet). It is beneficial to model the mold filling and curing behavior because, in addition
to understanding the flow and cure during the operation, it can provide us with useful
information such as knit line locations, velocity, pressure and temperature distributions,
and the curing history.
The models developed for flow and heat transfer fall under two categories considering
the thickness of the composite part: (i) thin parts and (ii) thick parts. Parts are classified as
thin if their thickness is at least one to two orders of magnitude smaller than their in-plane
dimensions as shown in Figure 6.3.
Thin parts comprise a large percentage of all compression-molded parts, since they can
be cooled and cured quickly and meet the requirements of low cycle times. Thick parts may
be necessary for some applications where cycle times may not be the driving factor, but the
modeling approach followed is slightly different. We will first discuss thin cavity models.
Figure 6.3: Two typical parts of thickness b, which is much smaller than the in-plane
dimensions.
6.2.4 Thin Cavity Models

The first step in modeling a thin part is to use the concept of the lay-flat approximation. For
example, if the part is a three-dimensional box, one can mathematically and conceptually

"unfold" it in the x-y plane with the z direction being its thickness as shown in Figure 6.4.
This approximation allows one to model any thin three-dimensional shape into an equivalent
flat part, although the domain in the plane may be very complex.
(a) Box (b) Unfolded box
Figure 6.4: (a) A three-dimensional box, and (b) its mathematically and conceptually
"unfolded" version.
The next step is to mathematically describe the material behavior to formulate the
model. The simplest approximation is to assume the material to be Newtonian and isotropic.
However, if the physics and experiments suggest something different, one could refine the
material behavior by including nonlinearities. It is always useful to address the isothermal
case first, as one can understand the important parameters if the complexities are kept to
a minimum. For the moment, one can assume the viscosity to be a function of x, y and z.
With these assumptions, one can now delve into the modeling.
A sketch of a typical compression molding flow is shown in Figure 6.5 with the coordinate
system appropriately attached and some of the parameters such as the in-plane dimension
L, height h and the closing speed s identified. For thin parts, L 3> h. As shown in
Figure 6.5, the flow in the x-y directions is due to the squeezing motion of the upper half
of the mold, which moves downward with a prescribed speed of s which is the same as —h
or —dh/dt. The instantaneous thickness of the part is h(x,y] and the velocity components
of the material are denoted by u, v and w in the x, y and z directions, respectively.
Next, one can carry out an order of magnitude analysis to evaluate the magnitude of
velocities in the x, y and z directions. The mass conservation equation for incompressible
fluids may be stated as
du dv dw = 0 ,6 1 .
7r
ax + 7T
ay + ioz
r - C-)
Using this as the guide, and the characteristic dimensions in the in-plane directions (x and
y) and thickness direction (z) as L and h, respectively, we find that
du Uc dv Uc dw s
(6.2)
dx dy L' ~dz h
where "~" denotes "of the order." We assume that the characteristic velocity, Uc, in the x
and y directions is of the same order and the dimensions in the in-plane directions are of
the same magnitude. Thus, substituting this order in the mass conservation equation, we

Figure 6.5: Coordinate system and nomenclature for compression mold filling analysis.
can show that
u; ~ s, and Uc (in-plane velocities, u and v) ~ s — . (6.3)
These relations will hold everywhere except very close to the edge of the flow domain and
if L 3> h. Most of the flow will be planar and the velocity in the thickness direction u; can
be neglected. However, the velocities u and v are still functions of the z direction. Thus,
to eliminate the z direction dependence, one can integrate the continuity equation in the z
direction
x rh(x,y
^ du(x,y,z] dv(x,y,z) ftl(X,
h(x,y) dw(x,y,z}
dz dz+ / (6.4)
IQ dx JO dy Jo dz
which can be written as
d(uh] d(vh] _
=S (6.5)
dx dy 2=0
because w = 0 at z — 0 and w = — s at z = h. Here u and v are the velocity components

in the x and y directions averaged across the part thickness. Mathematically they can be
written as
u(x,y) = — !
x, y} Jo
u(x,y,z)dz (6.6a)
I r
v(x,y)
,y} =
= 77—r / v(x,y,z)dz. (6.6b)
h(x,y) Jo
Equation (6.5) is the continuity equation for a compression molding situation in which the
lower mold platen is stationary and the top platen is moving down at the speed of s when
in contact with the charge. Thus, this equation must be satisfied everywhere in the charge
domain.

Next, we turn to equations of motion, which if we assume that the inertia and body
forces are negligible, reduces to
a r>
dP a_
dr a_ «~-
xx , dTyx zx
(6.7a)
dx dx dy ' dz
dP
1 (6.7b)
dy dx dy dz
dP 1 &ryz 1 drzz (6.7c)
dz dx dy dz
For thin parts, if one assumes no-slip of the material at the mold walls, the shear stresses
(TZX and rzy) will dominate and one can adopt a lubrication approximation discussed in
Chapter 5 to simplify the analysis. This results in the Hele-Shaw flow model. However,
if one assumes a slip boundary condition at the mold walls, then the dominant stresses
will be the in-plane stresses TXX, rxy and Tyy. This leads to a lubricated squeezing flow
model. These two cases represent limiting cases of thin compression molding. One could
also introduce partial slip and obtain a more general solution, but first we will discuss the
Hele-Shaw model.
6.2.5 Hele-Shaw Model

In the Hele-Shaw model, velocity may be a vector function of x, y and z, but at any (x,y)
location the direction of the velocity vector is not a function of z as shown in Figure 6.6(a).
This allows one to average the velocities u and v through the thickness and track them only
as a function of x and y. This reduces the mathematical problem to two dimensions and
reduces the number of calculations by an order of magnitude.
projections of vectors projections of vectors
Figure 6.6: (a) A typical Hele-Shaw velocity profile in which the direction of the velocity
vector is not a function of z at a fixed ( x , y ) location, (b) A typical non-Hele-Shaw velocity
profile: velocity vector direction changes with z.
In compression molding problems, if one assumes no-slip boundary conditions at the

mold walls, an order of magnitude analysis will show that the velocity gradients in the
thickness direction are much larger than in the in-plane direction. For example,
du du U
— and — ~ —c (6.8a)
dx dy L
du Uc
(6.8b)
!Tz h

Thus, for an inelastic fluid
(6.9a)
dx
Uc
(6.9b)
dz
As h <C L, one can safely neglect Equation (6.9a) as compared to Equation (6.9b). This
reduces the equations of motion to
9P = drzx
(6.10a)
dx dz
OP dr..zy
(6.10b)
dy dz
dP
(6.10c)
Equation (6.10c) implies that pressure varies within the x-y plane only. For isothermal
Newtonian fluids, one can substitute the stress-strain rate relationship
(6.11)
into Equations (6.10a) and (G.lOb) which results in
d_P_ _
(6.12a)
dx
dP__
(6.12b)
~dy~
Since P is not a function of z, Equations (6.12a) and (6.12b) can be integrated twice to
obtain the velocity profile through the thickness
1 dP
—-— (6.13a)
2fj, dx
1 dP
— — (6.13b)
2M dy
The boundary conditions to find the constants are no-slip at the mold platen walls,
u = 0, f = 0 a t 2 : = 0 and at z = h. (6-14)
This gives velocity distributions as
(6.15a)
2/j, dx
1 dp
v= ,22
h (6.15b)
2/z dy

Note that because of the very low Reynolds number in these flows, the parabolic velocity
profile is achieved instantly. Hence, even though h is changing with time, the velocity
profile can be assumed to be parabolic at every time step by assuming a quasi-steady state
as discussed in the section on assumptions in Chapter 5. Note that u and v depend on x
and y as well because dP/dx and dP/dy are functions of x and y.
Before we find an equation for P, note one striking feature of this velocity distribution:
u and v are dependent on z but the ratio u/v is not, as made clear by taking the ratio of
Equations (6.15a) and (6.15b):
-
v
This form states that the magnitude of the velocity vector will vary across the cavity
thickness but the direction will not. Thus, we have proved that this flow is a Hele-Shaw flow
as shown in Figure 6.6(a). Heiber and Shen [257] have shown that even in a nonisothermal
or non-Newtonian case, this type of flow has the characteristics of Hele-Shaw flow.
This simplifies the analysis to a great extent. Instead of calculating u and v at every
x, y and z location, we can instead find the average velocity at each ( x , y ) location. These
average velocities can be obtained by integrating Equations (6.6a) and (6.6b) to give [258,
259, 260, 109, 261, 2, 262]
0 = -^-^ (6.17a)
12/i dx ^ '
= -*-^. y(6.17b)
dy '
For nonisothermal and non-Newtonian cases in which viscosity varies with z, [257, 258, 259,
260] provide the general form
« = -h£ox
£ (0.18.)
, = -S-9^ { (6.18b)
h 8y '
where S is a measure of the ease with which the suspension flows locally and is given by
S= I ( * ~ A ) dz. (6.19)
Jo f]
Here T\ — TI(Z) is the viscosity and A is the value of z at which the shear stresses rzx and rzy
are zero. For an isothermal case, S will be equal to /i3/12/z.
To find the governing equation for the pressure distribution, one can substitute Equa-
tions (6.18a,b) into the integrated mass conservation equation (6.5). This results in
d fS <9P\\ dd_ fS
(S_dP_\
OP _
dx V h dx J dy \ h dy
This equation is a Poisson equation and can be solved for P(x,y), once the boundary
conditions are specified. The physical boundary conditions will be that P = 0 at the free or
moving boundary surface (assuming there is no back pressure in the mold) and dP/dn = 0

when the charge reaches the mold walls (assuming that there is no leakage of flow across
the mold walls) where n is the normal direction in the x-y plane on the mold wall.
To solve Equation (6.20), one may have to resort to numerical methods such as finite
difference or finite element, as the solution domain expands when the material is compressed.
A procedure must also be chosen for tracking the moving flow front and the shape of the
charge and for modifying the boundary conditions as portions of the charge front encounter
the boundaries of the mold walls.
Once the pressure distribution is known, the entire velocity distribution may be found
by rewriting Equations (6.18a,b) and (6.19) [257, 258, 259, 260]
z- A , .
-^ (6.21a)
Z
-dz. (6.21b)
If A is not known a priori, one of the boundary conditions such as no-slip, i.e. u — 0, v = 0
at z — h can be used to find A.
The governing equation (6.20) can be solved to determine pressure and velocity dis-
tributions at any instant in time as we treat this problem as quasi-static in nature. The
time-dependent nature of the pressure and velocity field enters into the problem because
as the mold closes the redistribution of the charge takes place and the flow front position,
where a boundary condition is applied, keeps changing. The usual procedure to predict the
flow in compression molding can be outlined as follows [263]:
1. Specify initial conditions (location of the charge, boundaries of the charge, closing
speed, etc.).
2. Solve for the pressure distribution at t = 0 using Equation (6.20).
3. From the pressure distribution, find the average velocities and advance the material
to form the new boundaries of the charge.
4. Solve Equation (6.20) in the new domain with the new height h and the boundary
conditions.
5. Repeat steps 3 and 4 until the charge touches all the mold walls or until the maximum
force the compression molding machine can generate has been reached or until one
achieves the final thickness in the z direction. To calculate the force required at any
time t to move the platen at a speed s, one must integrate the pressure field at that
t over the charge domain.
The two main assumptions that are used in this model were negligible w and insignifi-
cant in-plane stresses. These assumptions are valid everywhere in the domain except near
the edges of the compressing material. Thus, one can gain tremendous simplification by
sacrificing a little bit of accuracy at the edges. The Hele-Shaw model is always valid as long
as the shear stress terms are larger than the in plane stresses. This implies that
drxz r\wuc drxx t)cuc
(6 22)
-^~-h^^^~^' '
In compression molding, usually a cold charge is molded in a hot mold so the viscosity of
the material near the mold wall, r)w, where most of the shearing dominates, is lower, as

compared to the viscosity near the middle, rjc, where the viscosity is higher as the material
there is still not heated. Thus for the Hele-Shaw approximation to be valid, we must have
The viscosity could differ at the most by an order of magnitude from the surface to the
center. However, usually if L is about an order of magnitude larger than h, which is
definitely true for a part such as an automobile hood, one can usually justify the use of the
Hele-Shaw model.
6.2.6 Lubricated Squeeze Flow Model

If the charge or the mold surfaces are well lubricated, the charge material will slip along
the upper and lower surfaces of the mold. This translates into a slip boundary condition.
One could have a partial slip or complete slip. If one models a partial slip, an additional
parameter to describe the degree of slip will be required. Here, in order to introduce the
model, we will assume complete slip on both of the surfaces. Mathematically, this can be
described as the shear stresses at the mold surface are zero:
r
xz — 0 and Tyz = 0 at z = 0 and z = h. (6-24)
It further assumes that there is no shearing across the thickness. This leads to u and v
being only functions of x and y, and therefore u = u and v = v. The equation of motion
due to this assumption reduces to
dx dx dy
dP
ay = d^
ax + d^
ay (6.25b)
with the boundary conditions that velocity normal to the mold walls is zero and the total
stress normal to the free flow front is zero.
Lubricating squeeze flow solutions can often be trivial, providing bi-axial extensional
flow in the x and y directions. This implies that as you squeeze in the z direction, the
material elongates in the x and y directions equally, until it encounters a mold wall and
then it elongates only in the direction it can as shown in Figure 6.7. The pressure inside the
charge is usually constant. To find this pressure one can use the boundary condition that
the total stress normal to the boundary, ann is zero. If vn is the velocity component normal
to the free flow front boundary and n denotes the normal direction, it can be expressed as
(Jl I
<?nn = ^-^ ~P = 0 (6.26a)
f/1 1
or, 2ri—- = P. (6.26b)
CfiL
Here P is the pressure of the material inside the charge which is not equal to the pressure
outside.

Figure 6.7: Biaxial elongation of a lubricated charge due to compression molding. The
material elongates equally in the x and y directions until it encounters a mold wall.
Example 6.1: Lubricated Squeeze Flow
Consider a polymer charge being squeezed between two parallel disks as shown in Figure
6.8. The disk surfaces are lubricated so that there is a slip boundary condition in the radial
direction. Assume that inertia and body forces are negligible. The thickness of the polymer
charge is h and the radius of the disks, and hence the charge is R. The disks are compressed
in a press with a closing speed of s — —dh/dt = —h.
Closing speed
s =-dh/dt
Figure 6.8: Schematic of a fiber reinforced polymer charge being squeezed between two
parallel disks in compression molding.
Find (i) velocity distribution, (ii) stresses and the pressure in the fluid, (hi) the total
force exerted on the upper disk by the fluid, and (iv) h(t) if /i(0) = h0 and the total weight
of the upper disk and the press is W.

Solution
(i) The symmetry of the problem requires that vg = 0 and d()/d9 = 0 for all the variables.
The continuity equation in cylindrical coordinates reduces to
1 9 , . dvz
The boundary conditions are
vz = — s at z —h (6.28a)
Tzr = 0 at z =h (6.28b)
vz = 0 at z =0 (6.28c)
rzr = 0 at z =0 (6.28d)
vr = 0 at r =0 (6.28e)
arr = -Pa at r =# (6.28f)
where Pa is the atmospheric pressure. Let's assume that vr = vr(r) and vz — vz(z) consid-
ering a thin charge, R 3> h. The assumption of vz — vz(z) meets the boundary conditions
(6.28a) and (6.28c). With these assumptions, the partial derivatives in Equation (6.27)
reduce to ordinary derivatives, and hence Equation (6.27) can be rewritten as
—— (rvr) = -^ — constant = ci. (6.29)

r dr dz
The term ^ -j^ (rvr) on the left-hand side of Equation (6.29) is a function of r only, and the
term — ^f is a function of z only. The equation indicates that these two terms are equal.
This can be only true if these two terms are indeed equal to a constant, c\. Integrating
~<Iz~ = Cl with respect to z yields vz = —c\z + c% where 02 is another constant. Applying
the boundary condition (6.28a) and (6.28c) yields
vz(z] = -~. (6.30)
By substituting dvz/dz = ~s/h into Equation (6.29), we have the following:

d
i r)^ = sr
— (rv —. IK o-n
(6.31)
dr h
Integrating both sides of Equation (6.31) with respect to r, one can obtain
TOr= ^f + C3. (6.32)
The constant 03 is found to be zero by using boundary condition (6.28e); hence

ST
vr(r] = —. (6.33)
Only the continuity equation (conservation of mass) was used to find the velocity field.
That means the equation of motion (conservation of momentum) was not used for the

velocity field calculation. So, the velocity field is the same whether the fluid is Newtonian
or not. Once the velocity field is known, one can find the deformation field.
(ii) The components of the strain rate tensor for this flow field will be (see Table 3.5)
(6.34b)
= Jo* = 7rz = 0. (6.34d)

Hence, the strain rate tensor,
o
/ 1 0
I
0 \I
(6.35)
is a biaxial elongation tensor. If the constitutive law between the stress and strain rate
is known, one can also calculate the stress tensor. We will assume a Newtonian material
behavior to evaluate the viscous stress tensor for the material. The stress tensor is given by
(6.36)
What is the pressure distribution within the fluid (polymer charge)? One can use the
stress tensor in the equation of motion in the r and z directions to evaluate that. The
equation of motion in the r direction is as follows:
dP 1 d IT0e . 9rrz
OTrg
0 = (rr,. r ) 4
dr r dr de r f dz
r
dP I d /iS> I 8(0) (Ais)/h + d(0)
(r
dr ' r dr h )\ + r 89 r dz
0- +0 (6.37)
or rn rn
or, simply dP/dr = 0. The equation of motion in the z direction gives:
6P I d ZZ Idrg, OT
0 = ~-^- + --^-(rrrz)^ --- ^- + ^~
oz r or r oti oz
o = _
dz r dr r dO dz
OP
0 = -— + 0 + 0 + 0 (6.38)
dz
or, simply dP/dz == 0. Hence, P is a function of neither r nor z. So, it is a constant P = C.
In order to find C, we use the boundary condition (6.28f):
oyr = rrr - P
-Pa = ^-P. (6.39)

Hence, the pressure P within the charge is
P = ~T- (6.40)
which is higher than the pressure outside Pa. As seen from Equation (6.40), the higher the
viscosity /j, and closing speed s, the higher the charge pressure P.
(ui) o~zz is the force per unit area exerted on the polymer charge. So, the force F on the
upper disk is the integration of — azz over the disk area:
F = - I azz dA — - 2?rr dr
R
(6.41)
(iv) Force balance on the upper disk (in the z direction) is
= W + TtR (6.42)
force due to atmospheric pressure
force exerted by the polymer charge
Here, we neglect inertia forces. Figure 6.9 shows the force balance. Hence, W —
Pa (Atmospheric pressure)
mum m u
tmtrttmm. (Normal stress)
Figure 6.9: Force balance on the upper disk for Lubricated Squeeze flow Example 6.1.
If a constant closing speed s is desired, then W should be increased with time by increasing
the press force. One can see this mathematically due to the presence of h(t) in the denom-
inator. If W is kept constant, then the closing speed s will decrease with time. In this
problem, W is specified as a constant, and we will calculate h(t). The closing speed of the
disk s is —dh/dt, hence
dh Wh
(6.43a)
~dt

dh___ W
~h~~ (6.43b)
\nh = - (6.43c)
h(t)=c2e (6.43d)
In Equation (6.43b), integration of both sides with respect to t is carried out to obtain
Equation (6.43c). The constant c% (= eci) is found to be ho by using the initial condition
ft-(O) = ho. Hence,
h(t) = h0e LV^r-K'M/ J . (6.44)

As shown in Figure 6.10, h(t) decreases exponentially when a constant press force is applied.
Figure 6.10: The mold gap thickness as a function of time for Example 6.1.
Obviously, this result breaks down at smaller values of h, as the assumptions of slip BC and
no surface tension at the boundaries will no longer be valid. •
6.2.7 Hele-Shaw Model with a Partial Slip Boundary Condition [2]

As we studied in Example 6.1, the lubricated squeezing model is based on the assumption
that there is no shearing across the thickness (TZX = rzy = 0), and the prepreg completely
slips across the mold cavity thickness.

The Hele-Shaw model has been found to give excellent results for thin, homogeneous
polymer parts. The lubricating squeezing model provides unrealistic results for such cases.
The lubricated squeeze flow model predicts that a rectangular charge will stay rectangular
throughout the process until it encounters a mold wall. This type of behavior has been
observed during the compression molding of thicker homogeneous parts, and parts molded
from SMC. The two models can be thought of as providing two extremes, Hele-Shaw pro-
ducing flow with zero slip at the mold boundaries, the lubricated squeezing flow model with
complete slip boundary condition, producing 'plug' flow through the mold thickness, as
Hele-Shaw Model with Partial Slip Boundary Condition

Barone and Caulk [261] proposed an alternative boundary condition at the mold walls to
model the flow of SMC. They provided a model that lies somewhere between the extremes
of the Hele-Shaw and lubrication squeezing models. They allowed for the partial slip of the
molding compound at the wall, by specifying a slip velocity directly proportional to the
shear stress at the boundary. For example:
vi = frji (6.45)
at the mold walls. A schematic of the predicted shape of the velocity profile vr(z] is
presented at the bottom of Figure 6.11.
In the following example, the proposed alternate boundary condition for the Hele-Shaw
model will be investigated through an analytical case study.
Example 6.2: Hele-Shaw Model with Partial Slip Boundary Condition [264]
Investigate the flow induced by the compression molding of a cylindrical charge between
circular plates which can undergo partial slip with respect to the mold walls. The plates
are moving at a speed of h towards each other, and are of radius R as shown in Figure 6.12.
Solution
The position of the charge flow front is defined by R. The equations to be solved are as
follows:
fh
2-xr \ vrdz + Trr2h = 0 (6.46)
Jo
drrz dP (6 47)
-w - ~w -
Equation (6.46) was derived by integrating the continuity equation over the charge volume.
Equation (6.47) is the momentum equation with the assumption that shear stresses are
higher than normal stresses. The boundary conditions are assumed to be
vr = /3 rrz at z=h (6.48a)

vr = P rrz at z = -h (6.48b)
rrz = 0 at z =0 (6.48c)
P = Pa at r=£ (6.48d)

Generalized Hele-Shaw Flow Model:
Lubricated Squeezing Model:
Proposed Partial Slip Model:
Figure 6.11: Velocity profiles vr(z) for various flow models [264].
2h
Figure 6.12: Axisymmetric squeeze flow of a cylindrical charge [264].

where /3 is an arbitrary constant, denning the amount of slip occurring at the mold surfaces.
Here the problem will be solved for Newtonian fluids. The velocity profile is obtained
by integrating Equation (6.47) with rrz = rjdvr/dz, and the boundary conditions (6.48a)-
(6.48c),
dr J \ / \ dr
Then Equation (6.46) is used to find the pressure gradient:
dr o,, , , , , , - (6-5°)
If /3 is given a value of zero, the velocity profile reduces to that of the normal Hele-Shaw
solution. If - —> oo, the velocity profile reduces to that of the lubrication squeezing solution.
Several velocity profiles have been plotted to examine the influence of the arbitrary
coefficient /3 on the amount of slip occurring at the mold walls.
As the velocity profile varies linearly with h, and scales linearly with radius r, all profiles
have been calculated for a single h and radius. Calculated velocity profiles at different plate
separations are shown in Figure 6.13. As the separation of the two plates decreases during
the process, the average radial velocity through the thickness increases. Therefore each ve-
locity profile calculated is normalized to its center line value, vmax. These plots demonstrate
how the amount of slip at the mold boundaries develops as the process continues.
Three different sets of velocity profiles are plotted in Figure 6.13. In each plot, the
velocity profiles have been calculated at h values of 0.1, 0.05, 0.01, 0.005 and 0.001 m. Each
set of velocity profiles has been developed for a certain value of /? in m/(Pa.s).
For Newtonian fluids, the ratio of the slip velocity at the wall to the centerline velocity
increases as the separation of the mold wall decreases. The fluid is slipping more and more
as the mold closes.
The pressure profiles were found by integrating ^-, applying the boundary condition
P — Pa at r — R. For convenience, Pa has been set to zero at this point. For Newtonian
fluids,
The expression for pressure distribution is useful to calculate the force required for
compression of the charge.
The squeezing force required to move the circular disks towards each other will be
calculated. This force was found by integrating the pressure at the mold surface from r — 0
to r = R:
(R
P(r) r dr. (6.52)
Jo
The resultant force for a Newtonian fluid is calculated to be
Squeezing force will be calculated for a particular theoretical experiment. The initial
diameter of the charge is 0.3m, and it has a thickness of 8mm. The closing speed h is

h=0.05m~-
h=O.Q1m -
h=0 005m
h=0.001nv—
h=0.1m
h=0.05in
h=0.01m
h=0.005m
h=0.001m
P =-0.005 m/Pa-s
decreasing h
0.4 0.6
Vr/Vma
h=0.1m—
h=0.05m--
h=0.01m ~
h=0.005m
h=0.001m
: ' ! decreasing -
0.4 0.6
VrA/ma
Figure 6.13: Normalized velocity profiles for compression molding flow of a Newtonian fluid
with partial slip boundary conditions along the mold walls [264]. Top: (3 = 0.0005, Middle:
(3 = 0.005, and Bottom: j3 = 0.05 in m/(Pa.s). In each plot, the profiles are shown for
different values of h in meters.

3mm/sec, and the charge is squeezed to a thickness of 5mm. The process takes 1.0 second
to complete.
Figure 6.14 presents several forces calculated for the experiment described above. Forces
have been calculated for /3 values of 0.0, 0.0005, 0.005, and 0.05 m/(Pa.s). /3 = 0.0 corre-
sponds to the Hele-Shaw flow model with no-slip boundary conditions. The force calculated
using the lubricated squeezing model is also presented; however, this is very small, being
0.009% of the Hele-Shaw result at the end of the experiment.
30000
25000 -
20000 -
8 15000 -
10000 -
5000 -
Figure 6.14: Force required to compression mold a Newtonian material with partial slip at
the mold walls [264].
As f3 is increased from zero, the squeezing force approaches the lubricated squeeze flow
model result. This is to be expected, because the velocity profile approaches "plug" flow
as /3 increases. However, as j3 increases one would expect the Hele-Shaw model to break
down as the in-plane stresses will become as important as or more important than the shear
stresses. Thus, the results for the pressure distribution and the force are valid only at low
values of j3. •
The successful application of the proposed alternate boundary condition depends on

the determination of the arbitrary constant /3. A method must be sought to measure this
quantity, and verify if it indeed is a constant. If this can be done, this altered boundary
condition will prove to be an invaluable tool for modeling large thickness and SMC parts.

In almost all compression molding processes, a cold charge is placed in a hot mold and
the heat is provided to the charge by the mold walls. For thermoplastics, one needs to
provide sufficient heat to melt the charge so it can flow and occupy the empty portion of

the cavity before the cooling cycle is initiated to solidify the component. For thermosetting
composites, one provides the heat to initiate the curing of the composite. Curing is an
exothermic reaction and will generate heat. If this heat is not extracted from the composite
it could lead to degradation of the part. Hence, the thermal mold design is very crucial to
the manufacturing of such components by the compression molding process.
It is also important to note that the filling and the thermal histories in molding are
coupled through the dependence of viscosity on temperature. For example, if the flow is
the Hele-Shaw type, the velocities at the center are much higher than the velocities near
the walls. This will lead to cold material from the center migrating towards the hot mold
surfaces as shown in Figure 6.15(a). On the other hand, if the resin viscosity changes
dramatically with temperature and if there is sufficient slip near the surfaces, one could
expect the material near the surfaces to get ahead of the material near the center. This
would cause the material to flow towards the center as shown in Figure 6.15(b). Hence,
the flow field is important to determine the temperature, the cure behavior in the case of
thermoset, and the thermal design of the mold.
Figure 6.15: Velocity profile and the migration paths of cold material entering a hot mold.
In (a), the no-slip velocity boundary condition leads to migration of the material from the
center to the mold walls. In (b), the slip boundary condition at the walls and temperature
dependence of viscosity cause the particles to migrate from the surface towards the center.
Example 6.3: Nonisothermal Lubricated Squeeze Flow [263].

Consider lubricated squeeze flow of a charge initially at temperature, TO, placed in a hot
mold at temperature Tw. The top mold platen contacts with the charge and is moving
downwards compressing the material with constant speed s. Assume that viscous dissipation
and conduction in the x-y plane are negligible. Find the temperature history as the charge

flows to form the part. The thermal conductivity of the charge in the z direction is k,
density is p, and heat capacity is cp.
Solution
For lubricated squeeze flow, the velocity components u and v do not vary with z; therefore,
du dv
(6.54)
dz dz
Differentiating the equation of continuity with respect to z for an incompressible fluid,
d i du dv dw
(6.55)
x + oy
jr + To =°-
Interchanging the order of differentiation leads to
d i du\ d dv _j_ _ Q
(6.56)
dx\dzj ' dy \dz'
Substitution of Equation (6.54) into Equation (6.56) results in
= 0. (6.57)
The boundary conditions as seen from Figure 6.16 are w = 0 at z = 0 and w — — s at z — h.
Speed, s
T-T (Wall temperature)
Figure 6.16: Temperature boundary conditions for nonisothermal compression molding of

a charge.
This yields
sz
(6.58)
Thus, the motion of the material is uniform compression. If we scale z by introducing a
new coordinate A as
(6.59)
then the fluid or the material particles will remain at the same position A throughout the
flow. However, the particles will move in the x-y plane.

The energy equation with no viscous dissipation or conduction in the x-y direction can
be written as 2
&T
dT dT dT\ , d T
— + v—+w — )=k—^. 6.60
dx dy dz J dz2
As there is no x-y variation in the temperature or boundary conditions, dT /dx and dT/dy
are zero. We can also assume that convection in the z direction is negligible for simplicity,
although one can solve the equation by retaining this term. Using the transformation in
Equation (6.59), Equation (6.60) can be rewritten as
Here dT/dt represents the time derivative at a fixed position A. Equation (6.61) is similar
to the conduction problem of a slab initially at temperature TO, whose walls are exposed
to Tw at t = 0 except the slab is shrinking across its thickness with time. The solution is
given by
= I + 2 £ - - exp -» cos (flnA) (6.62)
Tw — TO
where a is the thermal diffusivity (a = -|-) and the coefficients an are
an — TT I n -\— ] (6.63)
\ £)
and t*(t) is an integrated time
n dt
Here t' is the dummy variable and hf is the final thickness of the charge. The changing
thickness of the sheet warps the time scale, accelerating the conduction of heat as the sheet
becomes thinner, as illustrated in Figure 6.17. •
6.2.9 Cure
In modeling the cure and coupling it with heat transfer, one must usually account for the
dwell time, an initial period when no appreciable curing takes place due to the addition of
inhibitors. Curing will be slow initially but then will rapidly accelerate and eventually level
off. Isothermal curing behavior of unsaturated polyester is shown in Figure 6.18 by plotting
degree of cure c versus time t. The degree of cure is defined as
c =- (6.65)
It
where q is the cumulative amount of heat released from the beginning t = 0 to the current
time t as compared with the total heat of reaction qt- As listed in Chapter 4, there are
many models to describe the cure kinetics. For example,
(l-cT (6.66)

Time [s]
Figure 6.17: Nondimensional temperature at the center of the charge as a function of time
with an initial thickness hi = 10mm, final thickness hf = 3mm, closing speed s = Imm/s,
and thermal diffusivity a = Imm 2 /s.
where k0, m and n are found by characterizing the resin experimentally.

Hence the rate of heat liberated per unit mass is given by
dc
(6.67)
9t
Time
Figure 6.18: Schematic of isothermal curing behavior of unsaturated polyesters.
6.2.10 Coupling of Heat Transfer with Cure

As the cure depends on the temperature, and curing liberates heat into the composite and
hence affects the temperature, the two phenomena are coupled. The heat liberated during

cure can be modeled as volumetric internal heat generation; thus one can write the energy
equation as
DT 2
pCp^- = kV T + S (6.68)
where S = qtdc/dt. At the same time, dc/dt is dependent on cure and temperature as seen
from Chapter 4 and Equation (6.66). Hence these equations need to be solved simultane-
ously if the curing has initiated. The viscosity of the material also dramatically increases
with the cure rate, which makes the flow of the material difficult. Many process engineers
prefer to add inhibitors to the resin so that they can fill the part with low viscosity suspen-
sion, before the resin cure initiates. Therefore, the convective terms on the left-hand side of
Equation (6.68) vanish, and it becomes a transient heat conduction problem with a space
dependent energy generation term.
Example 6.4: Importance of Damkohler Number

Nondimensionalize the energy equation to judge the relative magnitude of heat transfer
due to conduction and reaction. Let us assume that conduction in only the z direction is
important and there is no convection.
Solution
We will assume that the mold is saturated with resin when the resin cure initiates. As the
in-plane dimensions are much longer than the thickness h in the z direction, nondimen-
sionalization of the energy equation is carried out with conduction only in the z direction.
Other variables can be nondimensionalized as follows:
T
T* = - - (6.69)
Jo
(6.70)
c
*' = S I"-71'
where ATb = Tw — TQ (= difference between the wall and initial temperature) and tc =
pcph2 /k is the characteristic time for heat conduction. To make dc/dt dimensionless and
of the order unity, one must use the characteristic time of reaction, tr instead of tc. Thus
-" = «,£ (0.72)
The value of tr will depend on the kinetic equation used. Also the adiabatic temperature
rise just due to the heat released from the reaction can be estimated as follows:
ATr = -^-. (6.73)

pep
One can now write the dimensionless form of the energy equation (6.68) with no convection
and conduction neglected in the inplane direction as
Dar
d(z*Y2 + *- (6-74)

The dimensional group Da is known as the Damkohler number and is given by
Da = (6.75)
It represents the ratio of the rates of temperature rise due to reaction to conduction. Hence,
when Da is large, the reaction kinetics dominate the heat transfer, and if Da is small then
heat conduction dictates the heat transfer. •

When a charge with fibers is compressed, one would expect the fibers to rotate and move
along with the charge. Should we then consider the anisotropy in the viscosity when mod-
eling the compression effects or should we ignore it? It has been found that the change
in viscosity of the material due to the change in fiber orientation is a minor effect in com-
pression molding [265]. Hence, one can decouple the fiber orientation problem from the
flow problem. So once the pressure field is solved, one can find the velocity and velocity
gradients and use those in the constitutive equation to find fiber orientation. However, as
fiber orientation is an initial value problem, it does need an initial condition as will be seen
from Equation (6.207) later in this chapter. In this equation, Daij is a function of a^-, cu^-,
7 and Cj.
Figure 6.19: The convection of fiber orientation during compression molding [117]. The
direction of the line shows the direction of most fibers and the length of the line shows the
strength of the difference between the fibers in that direction as compared to the direction
perpendicular to that direction. Thus a dot would represent equal orientation distribution
of fibers in all directions and a long line will denote that most fibers are oriented in that
direction [117].

Thus, one needs to convect the orientation field as the material flows. Figure 6.19 shows
the convection of fiber orientation during compression molding. The details of this are given
in [117, 119].
6.3 Extrusion
Extrusion is the most important forming method in polymer processing. More polymers
and other materials are converted into useful objects by extrusion than any other method.
An extruder is essentially a pump to displace viscous materials. It is also capable of other
operations such as mixing along with pumping. The extruder can be fed with molten
material or with solid polymer chips, beads or pellets. In the case of composite materials,
the pellets have short fibers embedded in the polymer. A melting operation is achieved few
diameters downstream of the inlet. The operation is called plasticating, and the extruder is
known as a plasticating extruder. If molten material is fed to the extruder, it is known as
melt extruder. If two dissimilar polymers are to be blended, or if the pellets contain short
fibers, an additional operation of mixing is performed by the extruder.
The heart of the extruder is the screw. The details and the nomenclature for the screw
are shown in Figure 6.20. Table 6.1 shows the various geometric relationships. The screw
in the extruder is usually between 7.5 centimeters and 30 centimeters in diameter. The
speed is usually in the range from 20 to 500 revolutions per minute with a working pressure
between 50 and 1000 atmospheres. The flow rate could be as high as 2000 kg/hour. The
length to diameter ratio could be anywhere from 5 to 100.
Table 6.1: Geometric Relationships and Operating Characteristics for an Extruder

Geometric Parameters and Relationships
screw length : L
screw diameter : D
screw speed (revolution per second) : N
channel depth : H
helix angle : tan 9 = LS/-KD
channel width : W = Ls cos 6 — e
spiral channel length : 1 = L/sinO
relative velocities : vz = -nDN cos e, Vx = irDN sin 6
Operating Characteristics
TrDNWH cos 9 WH6 , P2 - PI ,
- 2 12n l L / s i n 6 » J
"( H ' H ' 21 )m
The extruder can be divided into three zones, the solid conveying zone, the melting
zone and the metering (melt conveying zone). The extruder operations can be grouped as
follows: (1) melting, (2) mixing and devolatilization, and (3) pumping. The transport of
the material inside the barrel is similar to a nut held in a wrench with the screw rotating
in the nut. If a rotating screw is prevented from advancing, the nut will slide in the wrench
as shown in Figure 6.21. In a similar manner the material slides between the screw and the
barrel.

Db = Barrel Diameter 8^= Flight Clearance
Ds = Screw Diameter « = Flight Width
Ls = Screw Lead 0 = Helix Angle
H= Channel Depth W= Channel Width
L = Overall Length of Screw P = Inlet pressure
N = Screw Speed (revolutions P = Exit Pressure
per second)
Figure 6.20: Nomenclature and dimensions of a typical extruder screw.
Nut (Material)
obstruction
preventing
IIS screw
;
advancement
Screw
Wrench (Barrel)
Figure 6.21: The principle of material advancement in an extruder can be compared to the
sliding of the nut if a rotating screw is prevented from advancing.

It is important to model the various operations in the extrusion process as it will prove
useful in the design of the screw and help establish the operating conditions and perform
scaling operations from laboratory scale to industrial scale. The objective of the model
may be to focus on various aspects of the extrusion process. For example, if one wants
to monitor how homogeneous the part produced is, the key issue would be to characterize
and model the mixing operation. On the other hand, if one was interested in the pressure,
and hence power and the throughput relationship, one would focus on modeling the flow
of the molten material through the screw and into the die. If one was interested in final
dimensions of the components, then the die swell (a phenomenon that is common with any
fluid once the material leaves the confined die shape and expands due to the surface tension
and normal stress effects) would have to be modeled. Thus, based on the objective, the
modeling for the same manufacturing process can address different issues. In this section,
our goal will be to address the flow rate and pressure drop relationship.
6.3.1 Flow Modeling

An important choice in modeling the flow of the melt is the choice of the coordinate system.
On first inclination, one may be tempted to use the spiral coordinate system, which can
lead to ugly mathematics. A clever way to handle this [102]. would be to hold the screw
stationary and rotate the barrel in the opposite direction. Next, one must "unwrap the
channel of the screw" and fix the coordinate system on the screw. This is schematically
Barrel
Figure 6.22: Schematic of the unwrapped extruder channel and the coordinate system on
the screw.
Next, we need to make simplifying assumptions to pose our problem correctly and
uniquely. For our analysis, we can assume Newtonian fluid, although similar analysis has
been conducted for non-Newtonian fluids. We will assume isothermal conditions. This
allows us to solve the flow in the x and z directions separately and then add the solutions
linearly as the fluid is Newtonian. There is no coupling with the temperature field.
The relative motion between the screw and the barrel becomes equivalent to steady
motion of a plane at an angle 9 to the helical axis z, which is the helical angle of the screw
as shown in Figure 6.20. However, the drag flow is generated in the x and z directions.
With inertia neglected, the equations of motion for Newtonian fluids reduce to:
dP_ (6.76)
dx dx2 dy2 dz2

(6 77)
° = -Ir+^fr+^+S")- -
As the flow is fully developed in the z direction, the last term in Equations (6.76) and (6.77)
vanishes as dux/dz = 0 and duz/dz = 0. This also implies that ux and uz are not functions
of z. It is assumed that the pressure gradient in the z direction is not a function of x and
y. Flow inside this channel is going to be a combination of pressure driven flow and drag
driven flow.
As the flow is fully developed, ux and uz do not change along the channel length; thus
^ and ^j- are all zero. Hence, Equations (6.76) and (6.77) simplify to
T
dx = M ^ +^ r l (6.78)
dP , ~ ^ . ~ u,z , (g 79)
The pressure gradient in the z direction is not a function of x or y, and ux and uz are not
a function of z as the flow is fully developed in the z direction. Thus, in Equation (6.79),
the pressure gradient has to be a constant along the z direction. Hence
' pji '•„,
dz 2r + 2r l' = C - (6.80)
function of z only not & function of
Thus
where PQ is the pressure near the exit of the screw and Pi is the pressure at the inlet. I is
the helical length of the screw and is given in Table 6.1. Now, one can solve
AP d2uz d2uz
T (6'82)
with boundary conditions

uz = 0 at x = 0 and x = W (6.83)
uz = 0 at y = 0 and y = H (6.84)
on all four walls. If W 3> H, one can ignore d2uz/dx2 as compared to d2uz/dy2 and the
solution will be valid everywhere except near the walls at x = 0 and x = W. The complete
solution for Equation (6.82) with boundary conditions (6.83) and (6.84) is given by an
infinite (Fourier) series. However, the most useful result is the volumetric flow rate
f ,- WH
Q= uzdxdy = —-AP(Fp}. (6.85)
JO JO 12/it
where Fp is the shape factor given by the infinite series and is a function of the aspect ratio
H/W [102]. The variation of this function with the aspect ratio is shown in Figure 6.23.

Figure 6.23: Influence of the aspect ratio of the channel on the flow rate in the extruder as
expressed by the shape factor, Fp.
One can combine the drag driven flow in the z direction with the pressure driven flow
in the same direction since the fluid is Newtonian and one is dealing with the isothermal
case. Thus, the flow rate is
1 WH3 AP
(6.86)
where Vz — V cos 9 and I is the helical length as listed in Table 6.1. Note here the pressure
flow is "backflow" in the direction opposite to that of the drag flow. For most extruders
W/H is large; hence Fj and Fp are close to unity. The barrel velocity is V — irDN and
Vx = VsmO and Vz — VcosO and N is the screw speed in seconds.
There is also a transverse flow ux(x,y) due to drag flow in that direction induced by
Vx. For large W/H, ux will have weak dependence on x, except near the walls (the screw
flights). The momentum equation can be rewritten as
dP
0 = -TT-
dx +' ^ 8y2
(6.87)
subject to boundary conditions

= 0 at y = 0 (6.88)
at y = H. (6.89)
The solution is
H
}' —
dx
(6.90)

as dP/dx is not a function of y. Even though the solution ignores the presence of the walls
at x — 0 and x = W, the walls exert one effect that must be taken into account. That
is, there is no net flow of material in the x direction because the screw flights prevent it.
Therefore
/ ux dy = (6.91)
Jo
which allows us to find
_
(6.92)
dx
Hence
U (6.93)
* = W(2--HJ-
This approximation is valid in the middle of the screw, away from the walls. As there is no
net flow, the extruder output flow rate Q is not affected. However, Vx is important from
the viewpoint of mixing and power requirements. The velocity profile that will be created
shown schematically in Figure 6.24. This confinement and the velocity direction helps the
fluid and the fibers to mix easily.
ux(H)=-Vx
Figure 6.24: The velocity component ux as a function of y inside the channel created by
the extruder screw and barrel.
6.3.2 Calculation of Power Requirements [3]

The power needed for driving the screw in the melt zone is given by
LJ = F U
cW
xy UT + T, dxdz. (6.94)
OJO
H H

Here I is the length of the screw, / = L/ s'mO, and W is the flight width. The shear stress
terms are calculated as
The -^ term in Equation (6.95) is zero since a uniform flow in the z direction is assumed,
and the -^j- term in Equation (6.96) is negligible compared to the other term ^ for large
W/H ratios. The velocity components are
6 98
<- '
Hence the power required is
2 2
(6 99)
-
For basic performance, one needs to calculate Q, <1> and AP. Equations (6.86) and (6.99)
are two of the three equations. We need a third equation to uniquely solve for Q, uj and
AP.
If there is no restriction at the end of the screw, AP = 0. That implies that there is no
mechanism to build up the pressure. Normally, there is a die downstream which establishes
the pressure rise down the extruder axis. Hence the additional equation comes from pressure
drop across the die associated with die output.
Kr
Q = —-AP (6.100)
M
where KG is related to die geometry and characteristics. To analyze this further, rewrite
Equation (6.86) as
AP
Q = AN-C - (6.101)
V
where
A = ]-WHFd cos 6-rrD (6.102)
and
WH3
C = ^rFp (6.103)
where the channel length is given by I = L/s'mO, and L is the screw length, and ./V is the
screw speed in seconds, then solving Equations (6.100) and (6.101) simultaneously results
in
(6 104)
11 A
-

as the flow rates in the screw section and die section must be the same. Note that Q does
not depend on \i. Also, Qmax = AN as KG —> oo, and APmax = [j,AN/C as KG —> 0.
6.3.3 Variable Channel Length [3]

Screws rarely have uniform geometry down the helical axis. The depth H varies in some
way depending on the purpose of the extruder and the type of material it handles. As
derived in [102], if channel depth is a function of z, but if the change is gradual, then uz
and ux can still be considered independent of z. However, we can maintain H(z) and dP/dz
as functions of z.
The simplest approximation in such situations is
(6.106)
The flow rate Q, which is normal to the helical axis should still be a constant; hence
(007)
and hence
(6.108)
As H(z) is a function of the screw dimensions, it is a known quantity. For example, consider
a linear approximation
H(z) = E0^
TT/ \ TT ,
(6.109)
as shown in Figure 6.25. Now we can integrate Equation 6.108 as follows:
Figure 6.25: A linear variation in depth of the screw, H(z).
dp
(6.110)

Rearranging the integrated equation for flow rate results in
= lvw HoHl W H0H AP

2 z iff0
AP
= AN-C - (6.111)
I-1
where
A = -irDW <Hi>cosO (6.112)
C = (6.113)
where
6.3.4 Newtonian Adiabatic Analysis [3]

The heating of the polymer depends on the heat supplied by the heaters mounted on the
barrels in the melting stage. The dissipative action of the polymer melt creates shearing
forces that generate heat as well.
Let us assume for the sake of analysis that the barrel is insulated (hence adiabatic
analysis) and no heat exchange takes place with the barrel in the molten polymer zone.
This is strictly not true, but one can get a good understanding of the coupling between the
momentum and energy equations to address the issue of temperature-dependent viscosity.
This analysis follows the one presented in [102].
and
Q = AN--2L%-. (6.117)
fjL(z) az
Integrate with respect to z to obtain the pressure drop AP
rl
o
It is necessary to introduce the temperature rise into the equation
where the last term QdP in Equation (6.119) is neglected as it is small. Prom Equation
(6.99)
w = E»N2l + ANAP (6.120)

where the last term ANAP is neglected, and E is defined as
E =- ^-(l + sin 2 6>). (6.121)
Taking the derivative of Equation (6.120) with respect to I, we have

n/'.}
(6.122)
dl
By equating Equations (6.119) and (6.122), one obtains
T. (6.123)
One can substitute Equation (6.123) into Equations (6.117) and (6.118), which results in
and
,025)
Q is now quadratic with N, and AT enters implicitly. Let us assume that the viscosity
dependence of temperature has the form
H = ae~bT. (6.126)
Recalling that
from Equation (6.123), one can obtain
_
EN2
By multiplying both sides of Equation (6.128) by ebT and integrating with respect to z, the
following equation is obtained:
1 (6.129)
where VQ = ae~bT° is the entrance velocity at z = 0 and AT is the temperature difference

across the channel from z = 0 to z — 1. If we now define a new variable x = e6Ar and
consider that as our primary variable
(6.130)

Now the die equation becomes
Q=K^P
H(Z) = Kc^P
V0
Q can also be written from the screw characteristic equation Equation (6.125):
. ,032)
AT
Now as eb^T = x, one can write AT in terms of x and b
AT = ^ (6.133)
o
and from Equation (6.131)
By inserting Equations (6.133) and (6.134) into Equation (6.131), one can get
pCpKxmx
By eliminating Q from Equation (6.130) and (6.135), one can get
N1 (6.136)
where NI = C/KG and JV2 = (Apcp)/(NlV0bE). For any JVi and N2 one can obtain the
solution for x and hence find Q and AP. The results are plotted in Figure 6.26.
More on the modeling of extrusion can be found in textbook written by Tadmor and
Gogos on this topic [102].
6.4 Injection Molding

6.4.1 Process Description
Injection molding is a widely used manufacturing process for producing parts in a mold
that has a cavity in the shape of the part being manufactured. In this process, solid pellets
containing resin and fibers are fed through a hopper into the barrel, which contains the
screw. It is similar in design to the extrusion process but is the heart of the injection molding
machine. The basic steps of the process are schematically shown in Figure 6.27. During
the melting stage, the heaters attached to the barrel heat the pellets. Simultaneously, the
rotating screw pushes the raw material forward inducing friction and shear. This will melt
the polymer and mix it uniformly with the short fibers, creating a fiber suspension. The
accumulating suspension in the injection chamber moves the screw backwards gradually.
After a sufficient amount of suspension is amassed, the screw moves axially forward acting
as a pump and injecting the suspension into the cavity of the mold through an opening
called a gate. The suspension, which is under high pressure due to the pumping action of

1,2 Z
Figure 6.26: Variation of screw parameters (Ni and A^) for Adiabatic case when the viscos-
ity is temperature dependent [3]. Find x from JVi and N%, and use it in Equations (6.133)-
(6.135) to calculate AT, Q and AP.
Plastication: The screw backs up

while rotating
Injection and packing
The screw is at rest
ejection of
the object
from the mold
Figure 6.27: Basic steps in the injection molding process.

the screw, quickly flows and fills the mold cavity. During the flow, the fibers move freely
in the polymer melt. During flow, the fibers change the positions and orientations thus
evolving the microstructure of the part. The heat from the polymer is conducted to the
cold walls of the mold, as soon as the suspension contacts the walls. The high pressure is
maintained during the packing stage. In this stage, maintaining very high pressure offsets
contraction due to cooling and solidification of the polymer. The injection pressure used is
in the range of 10 to 100 MPa. During the cooling stage, the resin solidifies and freezes the
orientation state of the fibers. Finally the mold is opened, and the part is ejected from the
cavity. The complete cycle takes from a few seconds to less than a few minutes depending
on the volume of the cavity to be filled. As a result, injection molding is well suited for
high volume production parts.
6.4.2 Materials
Both thermoplastic and thermoset polymers can be injection molded. Most often used ther-
moplastics are PE (polyethelene), PPS (polyphenylenesulfi.de) and PA (polyamide), which
are usually glass-reinforced. High-performance thermoplastics such as PPS and PEEK
(polyetheretherketone) might be carbon-reinforced. Unsaturated polyesters and phenolics
are the most common thermosets used. The reinforcement is usually short glass fibers in
the range of 0.5-5 mm in length. The raw material supplied to the barrel of the injection
machine is usually in the form of pellets or powder.
6.4.3 Applications
One of the advantages of injection molding is that geometrically complex components with
highly accurate dimensions can be economically manufactured in high volumes. Also, as
the process is automated, the cost per part will decrease rapidly as the volume increases. It
is not uncommon to make several hundred thousand to a million parts with a single mold.
For example, most plastic household items are produced utilizing this process. Examples of
short fiber reinforced articles are components for light machinery, equipment housings and
sprockets, and a variety of automobile components including appearance parts such as tail-
gates, instrument clusters, lamp housings, oil pumps, water pumps, bumpers and air intake
manifolds. This wide range of applications is constantly increasing. Other possible appli-
cations include replacement of conventional structures consisting of numerous components
(manufactured separately and assembled) with a single, lightweight, net shape composite
part.
The number and variety of parts manufactured by injection molding is large. It includes
items as small as paper clips to as large as automobile bumpers. Nonetheless the applications
are limited to non-load carrying components because of the poor mechanical properties of
the injection molded parts caused by:
• Relatively low fiber volume fraction.
• Short length of reinforcement fibers.
• Not much control over the alignment of the fibers induced by the flow.
• Fiber degradation in the feed screw and injection gate.
Despite these limitations of the injection molding process it has numerous advantages such
as:
Unlimited geometrical complexity of the manufactured parts.

• Size ranging from very small to very large.
• Excellent control of dimensional tolerances and surface quality.
• High volume production.

The most important issues in injection molding arise during the filling and packing stages.
During the filling stage, the cold mold must be filled completely with liquid resin suspension
before it becomes solid (incomplete filling is called a "short shot"). At the same time,
the shear rate and viscous dissipation should not exceed particular values to avoid resin
degradation. The analysis of the filling stage is further complicated because of its non-
isothermal and non-Newtonian character. Usually the mold surface is cold and the polymer
melt containing the fibers is hot. Hence the polymer freezes at the mold surfaces, which leads
to constriction of the flow path and required increase in injection pressure to impregnate
the suspension in the mold. Viscous heating can cause another complication. Because
of high viscosity and small flow channels, the temperature of the resin will increase and
may cause polymer degradation. In addition, the orientation of the fibers in the polymer
resin will continuously change as the suspension flows into the mold. This can lead to
significant variation in the fiber orientation state in the part and across the thickness which
will influence the physical and mechanical properties of the part. Thus, it is important to
understand the relationship between flow kinematics and fiber orientation. In summary,
the mold filling stage is a nonisothermal, non-Newtonian transient flow of fiber suspensions
in a complex geometry. To include all these effects, even in a simple mold, is a formidable
task. In the next section, we will pose the problem with all the governing equations and the
variables that need to be solved. However, it is beyond the scope of this book to provide
a solution. We will provide selected results from research papers that have attempted this
approach. In this chapter, our approach will be to address and solve selected aspects of the
problem to develop a better understanding of some of the observed aspects.
Scientific understanding of the process, expressed in the form of reliable models, is of
great help for example in the design of molds, which tend to be expensive component of the
equipment. Once the mold is made, for it to produce over a million components, it is milled
and treated to handle the wear and tear. A single mold can cost from several thousand to
a million dollars, and take from several days to a few months to fabricate. After the mold
is fabricated, an error in mold design will lead to either incomplete filling or undesired flow
and fiber orientation pattern. This will require one to retool the mold or scrap the mold and
"redesign it for the next trial." This trial and error approach can prove expensive in time
and money. Thus, it is time and cost effective to resort to process models and computer
simulations to guide the mold design and also the injection machine characteristics such as
maximum pressure required and the screw design. The process model and simulations can
provide useful information such as
• Optimal number and positions of injection gates.

• Required filling pressures and clamping force to avoid short shots (incomplete filling)
and flashes (excess material along the edges due to insufficient clamping pressure).
• Filling time: if the mold is filled too slowly, premature solidification may prevent
complete filling; if the mold is filled too rapidly, thermal degradation may occur due
to the heat released from viscous dissipation which is proportional to the square of
the shear rate.

• Temperature distribution: a balanced temperature distribution is desirable to avoid
excessive residual stresses that lead to warpage.
In order to obtain parts with desired mechanical properties, it is equally important to design
the mold and control the process in such a way as to get favorable fiber orientation states.
Thus, models that predict the evolution of the fiber orientation will also be useful.
6.4.5 Model Formulation for Injection Molding

Most injection moldings are thin in one direction compared to their other dimensions.
Hence, one can assume that the part being molded is thin and also flat for simplicity.
The part may have otherwise arbitrary shape as long as there are no abrupt changes in
thickness. Figure 6.28 shows a part that fits these requirements, along with the coordinate
system used. Note that the cavity thickness, 26, may be a function of x and y. We will
first restrict our formulation to a Newtonian isothermal case which will later be extended
to non-Newtonian and nonisothermal cases.
2b
Figure 6.28: Typical dimensions of parts made using the injection molding process.
Newtonian Isothermal Case

A thin cavity translates into velocity in the z direction being insignificant compared to the
velocities in the x and y directions and this results in dP/dz being close to zero. Hence, one
can safely assume that P will be a function of x and y only and we need to be concerned
about fluid motion in the x-y plane only. As with most composite processing situations,
one can assume that inertia and gravity are negligible. For the isothermal Newtonian case,
the equations of motion, N-S (Navier-Stokes) equations will reduce to
OP fd2u d2u d2u .

TTT
dy2 + TrS
2 6.137a
(6.137b)
ay \ ox2 ay

The velocity components u and v vary from zero at the mold walls to a maximum at the
center of the thickness of the cavity along z. One may assume similar variation along the
x-y plane. However, as the distance along the z direction is of the order of b, which is much
smaller than the distances in the x-y plane, dû/dz2 and d2v/dz2 will be much larger than
the other terms on the right-hand side of Equation (6.137). This simplifies the equation of
motion to
— = M ^-±2 (6.138a)
ox oz
=M—I- (6.138b)
Since P is not a function of z, each equation can be integrated twice to give the parabolic
velocity profiles
1 rlP
_i_±L^2 (6.139a)
u= + CiZ + C2
2fjL dx
v =- z2 + c3z + c4. (6.139b)
2^ dy
The boundary conditions are that the velocity gradients are zero at the center due to
symmetry and no-slip at the mold walls. Mathematically,
— = —=0 at z = 0 (6.140a)
oz oz
u =v=0 at z = b. (6.140b)
Thus, the velocity profiles can be written as
U
~ ~2u ~dx
',222
z -bL2) (6.141b)
dy ^ '
This solution looks similar to flow between infinite parallel plates subjected to a pressure
drop boundary condition. However, in this case, the pressure gradient terms, dP/dx and
dP/dy are functions of x and y and are still unknown.
Also, as in compression molding, one can take the ratio of u/v and find that it is not
a function of z, thus exhibiting the feature of Hele-Shaw flows. This allows one to average
the velocities in the z direction at every x and y and simplifies the problem. These average
velocities are
1 fb
u(x,y) = - u(x,y,z)dz (6.142a)
b Jo
i rb v(x,y,z)dz.
v(x,y) = - (6.142b)
o Jo
Once u and v are known functions of x and y, and as one knows the velocity profile in
the z direction from Equations (6.141a) and (6.141b), one can find the velocity as a function

of x, y and z. We find that u and v depend on the pressure gradient as follows:
,= - { (6.143b)
3M dy '
The incompressible continuity equation is
du dv dw , ,,
7T
ax + 7T «- = °'
ay + az °44
This contains the velocity component w which we have ignored so far in the analysis, so we
may be tempted to do so here as well. However, although we know that w will be much
smaller than u and v, this does not imply that dw/dz will be smaller than du/dx or dv/dy.
In fact, as the thickness is much smaller than the other two directions, one can safely argue
that the dw/dz term will not be smaller than the other two terms in the equation. Thus,
one cannot just drop dw/dz. To address this issue, the general approach adopted is to not
satisfy the continuity equation exactly at every location in the suspension. Instead, one can
integrate the continuity in the z direction across the cavity thickness,
,fe = 0. (8.145)
o ox o y o dz
This will ensure no material is lost. Rearranging the order of integration results in
a rb d fb rb
— \ udz+ — \ vdz+ / dw = 0. (6.146)
dx Jo dy Jo Jo
The first two integrals are bu and bv, while the third integral must equal zero (since w
equals zero at z = 0 and at z — b), which results in
^ (6fi ) + 1(^ = 0. (6.147)
Substitution of Equation (6.143) into Equation (6.147) results in the governing equation to
be solved for the pressure distribution
If b is not a function of x and y (if the part is of uniform thickness, 26) and if the viscosity
is constant, the equation can be further simplified to the Laplace equation
Qlp
^=a <6-149'
Hence, by using simplifications and physics of the process, we have been able to reduce the
problem from four variables (u, v, w, P) to one variable P. Once the pressure is found, one
can calculate the velocities. The main issue now reduces to solving Equation (6.149).

To solve Equation (6.149), one needs to apply boundary conditions. As seen from Figure
6.29, at the flow front the polymer simply displaces air. If the mold cavity is well vented, this
mathematically translates into a boundary condition of P = 0 at the flow front (assuming
gauge pressure), where the air is being displaced by the suspension. The boundaries where
the polymer touches the edge of the mold in the x-y plane can be mathematically represented
as dP/dn = 0, where n denotes the normal to the boundary. Physically, this implies there
is no flow through the mold walls. The other important feature in modeling of such flows is
that the flow front is in motion. When simulating mold filling, the approach is to start with
the region near the gate. Solve for the pressure field, find the velocities once the pressures
are known, advance the flow front and resolve Equation (6.149) for the new domain. This
process is repeated until the complete mold is filled with the suspension. Again, in the
solution of this problem, one assumes quasi-steady state. That is, at each time step, we
assume that the process is steady and solve for Equation (6.149). This is a reasonable
assumption as long as the Reynolds number of the fiber suspension is much less than one.
dn
Air
Polymer
dp_ = 0
dn
Figure 6.29: Boundary conditions on pressure for the domain containing the polymer sus-
pension.
To solve these problems for isothermal and Newtonian cases in any arbitrary two-
dimensional geometry, one has to resort to numerical methods. There are many commercial
and research software packages available that implement the model discussed above. The
most commonly used is called C-Mold [266]. However, we will present an example of injec-
tion molding of a center gated disk under isothermal and Newtonian conditions in which a
closed form solution is possible.
Example 6.5: Mold Filling Time for Center Gated Disk [3]
Consider injection molding of a fiber suspension into a radial mold to make disks of radius
R and thickness 2h. The gate is located in the center of the disk and the suspension is
injected under constant pressure (see Figure 6.30).
a) Find the time to fill the mold under the assumption that the suspension behaves as
a Newtonian viscous fluid.
b) What will be the fill time under a constant flow rate injection at Q? Under these
conditions, what will be the maximum pressure?

flow front
2h
Figure 6.30: Injection molding of a center gated disk.
Solution
a) We need to make the following assumptions to simplify the solution to the problem:
• h«R.
• Entrance effects are negligible.
• Fiber orientation influence on viscosity is negligible.
• Quasi-steady state.
• Inertia effects are negligible.
• uz and UQ = 0.
Thus, mass conservation dictates
;!<"*> = » («M)
Therefore,
C(z,t)
3.151)
Equation of motion in the r direction for a Newtonian fluid, when h « R (only shear
stresses being important) reduces to
dP
(6.152)
Since P ^ P(z) and C is not a function of r,

r dP d2C
(6.153)
Integrating C twice using the no slip boundary conditions at the mold walls, which translate
into
C = 0 at z = h (6.154)
dC/dz = 0 at z = 0 (6.155)

results in
Ah2 7
C = ~[l-(^2]. (6-156)
Integrating P with respect to r in Equation 6.153 using the boundary condition of P = PQ
at r = TO results in
P - PQ = An\n.( —). (6.157)
ro
To find A(t}, one can use the B.C. at the flow front, Rf (see Figure 6.30), which assumes
the pressure at the flow front to be atmospheric pressure (P = Patm at r — Rf}. Let us
assume that PQ is gauge pressure; hence P — 0 at r — Rf in terms of gauge pressure. Hence,
Equation (6.154) will become
-P0 = A/iIn(^). (6.158)
ro
As Rf is a function of time, A will also be a function of time. In order to find Rf as a
function of time, first note that the flow rate Q is given by:
rurdz = ^hRf—rt. (6.159)

o at
Substitution of Equations (6.151) and (6.156) into Equation (6.159) and its integration
results in
Thus,
A = -Rf-—l-(-2). (6.161)
Substitute Equation (6.161) in Equation (6.158) to get
One can integrate Rf with respect to t to find how the flow front moves with time to
fill the mold. When Rf = R, that value of time will give us the fill time.
If one defines
r* = ^ (6.163)
P* = —^~ (nas units of I/time) (6.164)

3i
fcr
r>
and z* = —*- (6.165)
then Equation (6.162) can be integrated to give
*9 i / *\ 1 / *9 ,. \ î-L £
^>*2 (6.166)

The mold is filled when Rf = R, which translates into x* = ^. Substitution of this into
Equation (6.166) gives tfm, the time to fill the mold,
fill rj T")* L V / oV /J * \ " /
For example, if PQ = 5 atmospheres, r0 = 1 cm, R — 10 cm, h = I mm and p, = 1000 Poise,

then tfui = 5.4 seconds.
b) If the injection was done under constant flow rate, the fill time can be calculated
from the information of flow rate and the volume of the disk that needs to be filled. The
engineering quantity of interest for the constant flow rate case is the maximum pressure
requirement.
For constant flow rate case,
t/iu = ^ ^ (6.168)
where Q is the prescribed flow rate. Also from Equation 6.159

dRf_ = Q
1 v ;
dt 47T/i
One can integrate this equation as Q is constant with B.C. that Rf = ro at t — 0 to give
Rn2 _
f-^ht+r°- (070)
Q f , 2 (e -i n\7
Thus,
3D// Crt
(6.171)
As seen from Equation (6.171), the maximum pressure PQ will be when t = tfm.
See [267] to include the influence of fiber orientation on the flow velocity and the con-
ditions under which it is important. •
Nonisothermal and Non-Newtonian Case

The cavity filling stage is rarely isothermal. One always has hot resin injected into a cold
mold. Moreover, the viscosity is a function of the temperature. So, energy and momentum
equations are coupled. Also, most polymer melts are shear thinning in nature, so one must
also pay attention to this in engineering analysis of injection molding.
First, one can rewrite the energy equation in terms of temperature and heat generation.
The heat is generated because of the viscous dissipation of the resin in the narrow cavity if
the resin is a thermoplastic resin. The heat is generated due to cure-kinetic reaction if the
material injected is a thermoset.
dT\ { dT_ dT_ dT_\ _ d_(^ dT\ d f„ dT\ d
dx dy dz) dx
transient convection conduction
F
dz 1 + (ir
\dzjl + ?• (6-172)
cure kinetics
viscous dissipation

Note that we have retained terms of very high shearing in the viscous dissipation term. One
may also ignore the conduction in the x and y directions. Using dimensionless analysis, one
can easily show that the conduction in the z direction is at least two to three orders of
magnitude higher than in the x and y directions (assuming the thermal conductivity is of
the same order). For thermoplastics, q = 0. For thermosets, usually the viscous dissipation
term contribution is minimal, due to their low viscosity.
Almost all research text conveniently ignores the term wdT/dz, although by dimension-
less analysis, you could prove that the unsteady term and all three convective terms are of
the same order. Hence to be consistent, the wdT/dz term should be retained. However,
when we solve for flow, we do not solve for w, so it creates the problem of how to find
w. So, the assumption is made that the convective contribution due to w, at least in the
mid region, is zero, as w is identically zero in that region. It is a reasonable engineering
approximation. This assumption breaks down near the inlet gate or near the flow front
where one will encounter entrance and exit effects respectively.
In addition, the viscosity is temperature dependent, so one should account for its change
in the momentum equation. As in the compression molding case, one does so in an average
sense by integrating the viscosity through the thickness direction [268]
=0 (6.173)
ux \ UJL, / uy \ uy /
where
S= \ — dz. (6.174)
Jo rj
S is a measure of the fluidity, with b denoting the cavity half thickness in the z direction
and 77(7, T,P) denoting the shear viscosity of the molten polymer. For example, in terms
of the power-law model
r? = m(T, P) -y"-1 (6.175)
where
( r ) exp(bP) (6.176)
it follows that
S=I(—^y)^ (6.177)
where
A =
and
rh z ,
X = / z(-^-)ndz (6.179)
•A) g(T)
with
m(T, P) = m0g(T)ebp (6.180)
and
g(T) = exp(^ - p). (6.181)
Note that if the power law index was n — 1/4, the fluidity index as expressed by Equation
(6.177) will be proportional to the cube of the pressure gradient, which will make Equation

(6.173) highly nonlinear. Under such conditions of coupled momentum and energy equation
with nonlinearities present, it is difficult to solve such problems in an analytical manner.
However, one can use dimensionless analysis to estimate the role of coupling and also the
extent of heat dissipation.
Example 6.6: Flow of a Thermoplastic Suspension in a Thin Cavity

Consider the flow of a thermoplastic suspension in a thin cavity of height 2h as shown in
Figure 6.31. The suspension is injected under a constant flow rate of Q m 3 /s. The surfaces
of the mold are held at a constant temperature T\. Assume that the viscosity does not
change much with temperature and that steady state in flow and heat transfer has been
achieved inside the long mold. Plot the Tmjdpiane as a function of flow rate for a suspension
of viscosity 77.
x 2h
Figure 6.31: Flow of a thermoplastic suspension in a thin cavity of height 2h.
Solution
As the viscosity, r\ is assumed to be not changing significantly with temperature, one can
first solve the velocity distribution by using the equation of motion alone. Secondly, the
calculated velocity distribution is used in the energy equation to solve the temperature
profile.
Together with the assumptions made above, we will assume no-slip boundary conditions
at the mold walls. These will lead to a Poiseuille flow. However, the flow rate Q is specified
instead of the usual pressure drop AP along the channel of a length L. The equation of
motion for this one-dimensional, steady-state flow is
dP du2
0 =- (6.182)
dx
For this fully developed flow, the pressure gradient in x direction is constant and can be
written as dP/dx — dP/dx — AP/L — (Pe — Pi)/L, where Pe and Pi are the exit and inlet
pressures and L is the length of the channel. One might object to this by saying that the
values of Pe, Pi and L were not specified in the problem. What we will do here is that we
will first solve for u(z) in terms of AP/L, and then calculate the corresponding flow rate
Q taking the integral of u(z) across the thickness per width W. Then, we will rewrite u in

terms of specified flow rate Q by eliminating the AP/L term. So, let's rewrite Equation
(6.182) as
2
(6 183)
'
which can be integrated twice in z to give

AD
u(z) = —7z2 + clz + c2. (6.184)
2r)L
Symmetry of the profile requires that du/dz = 0 at z — 0 hence c\ = 0. The no-slip bound-
ary condition is u = 0 at the walls z = ±h. This can be satisfied if c% = — APft- 2 /(2r/L).
Hence the velocity profile is given as
z2
~h2}' (6 185)
'
.The flow rate can be calculated as follows:

n
rh rti
= W I u(z] dz = 2w
u(z}dz u(z) dz
-h JO
= 2W
o
(6.186)
where W is the width of the channel. By replacing APh2/(2r]L) term by -3Q/(4W//i3) in

Equation (6.185), we have the velocity profile in terms of Q
(6 18T)
M J' '
One can introduce nondimensionalized variables as follows:
'i. (6.188)
Equation (6.187) can be rewritten in nondimensional form as follows:

J, / J, \ O
(6.189)
In order to solve the temperature profile, the energy equation will be used
dT 82T fdu\2
u7r = k--^ + r)( — ) . (6.190)
ox ozz \oz J
Assuming u(dT/dx) is negligible compared to the two other terms, Equation (6.190) can
be simplified to
(6.191)
dz2 k \dz '

By introducing a nondimensionalized temperature as follows:
d=J (6192)
~J^'
Equation (6.191) can be rewritten in nondimensional form
^dz
where the nondimensional coefficient A is given by
(6.194)
One can write A = BQ2 where B = r//(fcTiVF 2 /i 2 ) to easily see the effect of Q on 9 and
hence T while plotting the mid-plane temperature versus flow rate.
One can evaluate du*/dz* = —3z*/2 from Equation (6.189) and then substituted into
Equation (6.194) to have
6 195
^=-¥<-•>'• <- '
By integrating both sides of Equation (6.195) twice with respect to z*, one gets
9(z*} = (-2*)4 + c^z* + 04. (6.196)
The symmetry of the temperature profile about the mid-plane can be mathematically ex-
pressed as 39/dz* = 0 This requires 03 = 0. The other constant c4 is evaluated by using
the boundary condition 9 = (T\ — T\)JT\ — 0 at z* = ±1. Hence, the resulting profile is
given by
. . . O _/i
The nondimensional mid-plane temperature is

q x oo
Vidplane = &(** = 0) = — = — Q2 (6.198)
as a function of Q.
Equation (6.198) can be rewritten as follows:
Tmidplane = T(z = 0) = TI fl + (6.199)
for the dimensional temperature at the mid-plane as shown in Figure 6.32.

Q)
Q.
I
CD T-i
0 Flow rate, Q
Figure 6.32: Mid-plane temperature, Tmjdpiane = T(z — 0), of thermoplastic material versus
flow rate Q. The material is injected at a flow rate of Q and the upper and lower mold
walls are kept at a constant temperature T\.

As the molten polymer and the fibers are injected through a gate under high pressure (1
MPa to 10 MPa), they flow as a suspension into the mold cavity. As the suspension flows,
the fibers are transported along with the resin and change orientation during the flow.
The frozen-in orientation of the fibers determines the microstructure and properties of the
composite. Hence, one of the key issues is to find the orientation of the fibers as they flow
into the mold cavity. However, the flow and fiber orientation are coupled. We have already
seen how the deformation of the suspension can influence fiber orientation state and how
the flow is influenced by fiber orientation, as the fluid stresses will change with changes in
fiber orientation as shown in the constitutive equations in Chapter 4, and will influence the
viscosity of the suspension which influences the flow field.
Qualitatively, fibers align in the direction of shear and stretching. It has been observed
that many injection molded parts exhibit a skin/core effect. That is, near the surface the
fibers are aligned in the flow direction and in the core they can be oriented transverse to
the flow direction [269]. The reason for this effect can be understood if one models the
fiber orientation and the flow kinematics. Using simple fluid mechanics and the fact that
shearing and stretching align fibers, we will explain this behavior with an example.
Example 6.7: Skin Core Effect in Injection Molding

Consider a circular disk being molded with short fiber suspensions from a gate in the center
as shown in Figure 6.33. The disk is of radius TO and thickness 26, where 2b is much smaller
than TQ. Assume that the suspension behaves as a power law fluid. Discuss qualitatively
how the skin core structure is formed during injection molding of short fiber composites.
Solution
We will consider the isothermal case for simplicity. The suspension is injected through the
center gate at a known flow rate. It makes perfect sense to choose a cylindrical coordinate
system with its origin at the center of the disk, and z = ±b are the surfaces of the disk. As

Figure 6.33: A circular disk being molded with short fiber suspensions injected through the
gate in the center.
the flow would be radial, under the assumption of creeping flow and fully developed flow,
the only nonzero component of the velocity will be vr. Except near the entrance and at the
flow fronts, the velocity can be written as
C
vr = — (6.200)
r
where C depends on the flow rate. The power-law index n is represented as l/s.
The rate of deformation tensor for this flow field has the form
2e0 0 70
0 -2e0 0 . (6.201)
70 0 0
Thus, the flow is a shearing/stretching flow. There is shearing of the flow along the walls at
±b due to the no-slip boundary condition along the walls of the mold. Along the midplane,
away from the walls (close to z = 0) the flow will stretch or elongate in the tangential (9)
direction due to the radial nature of the flow. If 7 is the shear rate, it can be easily found
by using equation 70 = dur/dz + duz/dr from Table 3.5,
7o = - (6.202)
r
If we label the stretch or elongation rate by e'o, one can use the definition of elongation rate
from Chapter 3 to find the stretch rate
— z 3+ 1 (6.203)
Stretching will align the fibers in the transverse direction, while shearing will align them in
the flow direction. The ratio
(6.204)
V
'

can be thought of as the shear/stretch ratio. When it is close to zero, the fibers will be
aligned in the transverse direction and when it is very large, the fibers will be aligned in
the flow direction. Near the surfaces, the shearing dominates; hence, the fibers align in the
flow direction and near the mid plane (z = 0) , the shearing is very low and the stretching is
more prominent, thus inducing the fibers to align along the transverse direction. In between,
the principal fiber orientation direction is determined by the shear/stretch ratio. Hence, a
simple analysis like this explains the reason for the formation of the skin/core structure in
short fiber injection molded parts.
Why is the thickness of the core different for different materials and flow rates? The
gapwise velocity profile plays a key role in the determination. If the velocity profile is
uniform across the thickness (power-law index tending to zero), then the stretch dominated
region will be larger and one would expect a thicker core of transversely aligned fibers.
The opposite is true if the velocity profile is more parabolic as is the case for Newtonian
fluids. The temperature influence on the viscosity will also change the velocity profile and
influence the skin/core distribution. Changes in the rheology of the suspension can also
influence changes in the orientation. •
The objective is to determine the velocity field and fiber orientation of flow of fiber
suspensions not only through the thickness but also in the plane. There are two approaches
that can be followed depending on whether the flow and orientation fields are coupled or de-
coupled. If one considers a coupled approach, one cannot use the Hele-Shaw approximation
and hence Equation (6.173) cannot be used to find the pressure and derive the velocity field.
This is because in the coupled approach the shear and normal stresses are also functions of
fiber orientation.
The general form of the constitutive equation to describe the stress tensor as a function
of the strain rate tensor and the fiber orientation tensor is given according to [265] as:
Tij = r/s7ij + r]scjkiaijki + B pyâ^- + %•%•] + C%- + 2FaijDr (6.205)
where 7^ = (duj/dxi) + (dui/dxj) is the rate of deformation tensor, r]s is the viscosity of
the solvent, c is the volume fraction of particles, A, B, C, F are material constants, Dr is the
rotary diffusivity due to Brownian motion, a^ and a^ki are second and fourth order tensors
describing the orientation state of the fibers and defined as: a^ = (piPj) = f PiPj'lP(p) dp,
and dijki = (piPjPkPl) — I PiPjPkPli)(p) dp, where ijj(p) is a probability distribution function
P(9i < 0 < 9i + dO, </>i < 4> <</>! + d(j)} sin Q\ dO d<j), p is a unit vector aligned with the axis
of symmetry of the fiber as shown in the Figure 6.34. More details are given in Section 4.4.
The rotary diffusivity term can be neglected [265] when the fibers are slender (which is
usually the case in injection molding) Equation (6.205) can be written in the form
T
ij = rii [jij + Np%iaijki + Ns {jikakj + aijjkj}] (6.206)
where Np is a dimensionless parameter, called the particle number, and ??/ contains isotropic
contributions to viscosity from the solvent and the fibers.
In addition, one needs a constitutive equation to predict and calculate fiber orientation
from flow. According to [119], the equation of change for the second order orientation tensor
a,ij can be written as:
~ - " - + - A (jikakj + aik-jkj - 2jkiaijki) + 2C/7(c% - Sa^-) (6.207)
where u>kj = (duj/dxk] - (duk/dxj) is the vorticity tensor, 7 = ^jij'jji is the scalar
magnitude of the rate of strain tensor. C/ is interaction coefficient, measuring the intensity

P
Figure 6.34: Definitions of 0, <j>, and p t o denote the direction of a short fiber.
of interactions between the fibers in the suspension. In order to solve Equation (6.207) a
closure approximation of the fourth order tensor aijki in terms of the second order tensor
dij is necessary. There are many such approximations available [270, 271]. Table 6.2 lists a
few.
Table 6.2: Closure approximations for a^ki in terms of the second order tensor
1
Linear closure
(Hand [272])
7
Quadratic closure dijkl — dijdkl
(Hindi and Leal [273])
1 - f
Hybrid closure avkl ^ V*< 1 • * , < 1 ^
(Advani and Tucker [274])
7
Under certain assumptions about the fibers and the flow, one can formulate the com-
plete set of governing equations to solve flow and fiber orientation simultaneously. We will
describe the procedure here for an isothermal case. For a nonisothermal case, one must also
include the energy equation such as Equation (6.172) in which the viscous dissipation term
is expressed as T : VU instead of just the velocity gradients multiplied by the viscosity.
Other assumptions that are reasonable are that fibers are considered rigid axisymmetric
particles that are smaller than any length scale of the flow field, the fibers are large enough
to neglect Brownian motion, and inertia and body forces are ignored due to the highly
viscous nature of the suspension. Thus using the continuity equation,
V-U = 0 (6.208)
and the equation of motion with inertia and body forces neglected
0 = -VP + V - r (6.209)
and combining the above two physical laws with the constitutive law for the stress and
fiber orientation, one has to solve the complete set of equations expressed by Equations
(6.206)-(6.209).

The dependent variables to be determined are pressure P, velocity U, stress tensor TIJ
and orientation tensor a^j. Because T^J and a^-are symmetric and the trace of a^ is equal
to 1 the total number of unknowns is fifteen (P,u,v,w, Tn,Ti2,ri3,T22,T23,T33, an,ai2,«i3,
022,023).
As is clear that even considering the isothermal problem is quite involved with non-linear
relationships and many dependent variables. In addition, as this is a moving boundary
problem, one must continuously update the domain that is continuously being filled with
the suspension. One also requires boundary and initial conditions to solve this problem.
Hence, any simplifications are usually welcomed by the modeller.
If NP52 <C 1, where 6 = pz (z component of the vector p) then one can safely decouple
the orientation problem from the flow problem. This allows one to solve for the flow of
the suspension independent of the fiber orientation state and then integrate the orientation
field along the streamlines using Lagrangian description. One may use Equation (6.207)
or the physical laws (Equations (6.208 and (6.209)) to solve for the pressure and velocity
field first. And then a Lagrangian viewpoint is adopted [245]. The convective part of the
material derivative in Equation (6.207) drops out which allows the system of 5 evolution
equations to be integrated along the streamlines and the orientation state to be determined
at various points. The flow charts depicting this are shown in Figures 6.35(a) and 6.35(b).
Material Parameters Material Parameters

Geometry Geometry
Process Boundary Process Boundary
Conditions Conditions
Suspension
Flow Field Flow Field
Rheology
Fiber Orientation Fiber Orientation

Field Field
1t
Mechanical Mechanical
Properties Properties
(a) (b)
Figure 6.35: The approach to solve (a) decoupled and (b) coupled orientation field.
What does one do with the fiber orientation information? This information is quite
useful in prediction of thermal or mechanical properties of a short fiber composite. For
example, one can write the stiffness tensor in terms of the orientation tensors. For details,
see [119].

6.5 Exercises
6.5.1 Questions
1. What is similar between the extrusion and injection molding processes?
2. What are the functions of the screw used in the extrusion and injection molding
processes?
3. Why are vents needed in the mold during the injection molding process?
4. In the extrusion and injection molding processes, during the transportation of fibers
and polymer melt, why is it important to predict how the suspension flows and what
the fiber orientation will be? What is the difference in the two solution approaches:
(i) decoupled and (ii) coupled?
5. What is "plasticating" in the extrusion process?
6. What are the three zones of an extruder?
7. What are the assumptions of the model that result in the following expression for the
power needed for driving the screw in the melt zone?
Describe each term that appears above.

8. In order to understand the coupling between the momentum and energy equations to
address the issue of temperature dependent viscosity, how would you model the heat
transfer between the barrel and the screw in the extrusion process?
9. Describe the different stages of the compression molding process.
10. Why is it important to correctly premeasure the amount of raw materials, or charge,
and then place it inside a preheated matched-die mold in the compression molding
process? What will happen if the exact amount of charge is not placed inside the
mold?
11. In the compression molding process, usually uncured SMC sheets are used. These are
fiber bundles with uncured resin and mineral fillers such as calcium carbonate. What
is the purpose of using mineral fillers?
12. What types of resin matrices are commonly used in the compression molding process?
13. What is the difference between the compression molding process using thermoplastic
and thermoset matrices?
14. What are typical ranges of mold temperatures for thermoset materials in the com-
pression molding process?
15. From which two processes was the injection-compression molding process recently
developed? Describe this new process.

16. What is the major reason that the injection-compression molding process has not been
popular, although it has some advantages such as improved dimensional accuracy and
low molding pressure requirement?
17. In which high-volume manufacturing industry are compression molded parts usually
used? Give examples of typical parts.
18. In aerospace applications, why are compression molded components usually used only
in secondary structural or nonstructural parts, but not usually suitable for primary
structures?
19. Why is it beneficial to model the mold filling and curing behavior in the compression
molding process?
20. What are weld lines in the compression molding process? How do they affect the
material properties of composite part being manufactured?
21. What is the concept of lay-flat approximation in compression molding process mod-
eling? For what types of composite parts can it be applied? What is the benefit of
using this approximation?
22. For thin and homogeneous polymer parts in the compression molding process, which
one of the models is more realistic to apply: the Hele-Shaw model, or the lubricating
squeezing model?
23. In the compression molding process, when a charge with fibers is compressed, the fibers
change orientation and are convected along with the charge. Do the experiments show
major or minor effects on the anisotropy in the viscosity of material due to the change
in fiber orientation? Are the flow and fiber-orientation problems strongly coupled, or
decoupled?
24. Describe the injection molding process by using all of the following words: solid pellets,
resin, fibers, hopper, barrel, screw, melting stage, heaters, friction, shear, suspension,
action of pump, gate, fill, mold, cavity, solidify, high pressure, cooling, ejection.
25. What types of thermoplastic and thermoset polymers are commonly used in injection
molding?
26. What are the advantages of injection molding?
27. Give some examples of injection molded parts from daily life.
28. Why do injection molded parts usually have poor mechanical properties, and hence
are used as non-load carrying components?
29. Are small dimensional tolerances and good surface quality achievable by injection
molding?
30. What are the critical issues in the injection molding process? Describe each of the fol-
lowing terms, what causes them, and what are the effects of them: short shot, flashes,
resin degradation, difficult mathematical modeling and its solution, and variation in
the fiber orientation and mechanical properties.
31. Why is it important to develop injection molding process models and computer sim-
ulations?

32. In the injection molding process model, what assumptions are used in order to obtain
the governing differential equation: ^^ + ^-^ = 0 which is a Laplace equation for
the material pressure, P? What boundary conditions are usually used to solve this
equation? Describe the solution procedure.
33. Describe the mathematical model and its solution for a nonisothermal and non-
Newtonian now of a suspension in the injection molding process.
34. As the molten polymer and the fibers are injected into a mold cavity under high
pressure, do the fibers usually align in completely random directions, or in some
preferential direction?
35. What is the skin/core effect?
36. Why is it important to know the fiber orientation distribution in a short fiber com-
posite?

1. The screw acts as a pump by pushing the polymer melts suspension into a
in the extrusion process, and inside a in the injection molding process.
2. There are different models of the extrusion process to address different issues. If one
wants to monitor how homogeneous the part produced is, then the key issue would
be to characterize and model the operation. On the other hand, if one
is interested in the pressure and hence power requirement, then one would focus on
modeling the of the molten material through the and into the
If one is interested in the final dimensions of the components, then he/she
would have to model the phenomenon called which is common with any
fluid once the material leaves the confined die shape and expands due to
and effects.
3. An important choice in modeling the flow of the melt is the choice of the coordinate
system. On first inclination, one may be tempted to use the spiral coordinate system,
which can lead to ugly mathematics. A clever way to handle this would be fix the
and rotate the in the opposite direction. Next, unwrap the
channel of the and fix the coordinate system on the
4. The relative motion between the screw and the barrel is equivalent to steady motion
of a at an angle 6 to
5. In extrusion process modeling, the flow could be assumed to be the combination of
two flows: flow and flow if the fluid is assumed and
the isothermal case is considered.
6. The heating of the polymer depends on the heat supplied by the mounted
on the close to the melting stage. The action of the polymer
melt creates forces that generate heat as well.
7. The raw material (charge) could be either (SMC),
(BMC), (LFTs), or (GMTs).

8. If thermoplastic material is used in the compression molding process, then the mold
temperature must be above the temperature.
9. In the compression molding process, press speeds are typically , the applied
pressure is in the range of , resin cure usually takes only and the
entire cycle time can range from to , depending on the degree of
automation incorporated into the process.
10. For thin parts being manufactured in the compression molding process, if one assumes
no-slip of the material at the mold walls, the shear stresses will dominate and one can
adopt a lubrication approximation. This results in model. However, if one
assumes a slip boundary conditions at the mold walls, then the dominant stresses will
be the in-plane stresses. This leads to a model. These two cases
represent limiting cases of thin compression molding problems.
11. In the Hele-Shaw model, the of the velocity vector varies across the cavity
thickness, but the does not.
12. In the Hele-Shaw model, because of the very Reynolds number in these
flows, a velocity profile is achieved Hence, even though the gap
height h is changing with time, the velocity profile can be assumed to be
at every time step by assuming a
13. In the Hele-Shaw model, the physical boundary conditions are as follows:
at the free or moving boundary surface (assuming there is no back pressure in the
mold), and when the charge reaches the mold walls (assuming that there is
no leakage of flow across the mold walls) where n is the normal direction to the mold
wall.
14. In the lubricating squeeze flow model of the compression molding process, as you
squeeze the material in the z direction, the material elongates in the x and y directions
, until it encounters a and then it elongates only in the direction
that it can. The pressure inside the charge is usually To find this pressure,
one can use the boundary condition that the total normal to the
is
15. In the compression molding process, cold charge is placed in a mold and
is provided to the charge by the mold walls. If the charge is ,
one needs to provide sufficient heat to it so it can flow and occupy the
empty portion of the cavity before the cycle is initiated to the
component. For charges, one provides the heat to initiate the of
the composite. Curing is an reaction and will generate If this
heat is not extracted from the composite it could lead to of the part. Hence,
the thermal mold design is very crucial to the manufacturing of such components by
the compression molding process.
16. If the flow is the Hele-Shaw type, the velocities at the center are much
than the velocities near the walls. This will lead to cold material from the
migrating towards the hot On the other hand, if the resin viscosity changes
dramatically with and if there is sufficient near the surfaces, one
could expect the material near the to get ahead of the material near the
This would cause the material to flow towards the

17. In the compression molding process, many process engineers prefer to add
to the so that they can fill the part with low suspension, before
the resin initiates.
18. In the compression molding process, when the Damkohler Number (Da) is large, the
dominates, and if Da is small then dominates.
19. In the injection molding process, models and simulations can provide useful informa-
tion such as (i) optimal number and positions of , (ii) required filling
pressures and (iii) clamping force to avoid and , (iv) filling time
to avoid premature due to slow filling, or thermal due to too
fast filling, (v) temperature distribution to avoid excessive that
might lead to , and (vi) fiber orientation states to obtain parts with desired
mechanical properties.
20. In the injection molding process, will align the fibers in the
direction, while will align them in the direction. The ratio ?2- =
can
bi+^~-zs+i be thought of as the / ratio. In this equation, 70
is , €Q is , r is , s is , z is , and b is
When this ratio is close to zero, the fibers will be aligned in the ^_
direction and when it is very large, the fibers will be aligned in the direction.
Near the surfaces, the dominates; hence, the fibers align in the
direction, and near the mid-plane (z = 0), the is very low and the
is more prominent, thus inducing the fibers to align along the direction.
21. In the injection molding process, if the velocity profile is across the thick-
ness, then the dominated region will be larger and one would expect a
core of transversely aligned fibers. The opposite is true if the velocity pro-
file is more as is the case for fluids. The temperature influence
on the will also change the velocity profile and influence the
distribution.
6.5.3 Problems
1. The approximated governing equation for the extrusion process was found to be
AP
L^J. ff-ii
\J Uiy ff"ii z
\J Ujy
= £. _| -
2
/j,L dx dy2
with boundary conditions on the four walls: uz = 0 at x = ±W/2, and uz = 0 at

y = ±H/2. The complete solution for the the volumetric flow rate Q was found to be
[H WH3
Q=
Jo ' 12/j.L
where Fp is the shape factor which is a function of the aspect ratio H/W, and plotted
in Figure 6.23. If W ^> H, one can ignore d2uz/dx2 as compared to d2uz/dy2 and
the solution will be valid everywhere except near the walls. Calculate the volumetric
flow rate Q by assuming W 3> H, and ignoring 02uz/dx2. Compare your result with
the more accurate result for W/H = 100, 10, 5, and 2.

2. A polymer charge is squeezed between two parallel disks, and the disk surfaces are
lubricated so that there is a full slip boundary condition in the radial direction, and
inertia and body forces are neglected.
(i) What is the velocity distribution as a function of thickness of the polymer charge
h, at a closing speed of plates s = —dh/dt — —/i, and the radius of the disks and the
charge being equal to R?
(ii) What is vr if there is a partial slip with coefficient j3 between the walls and the
material? Check your result by taking the limit as j3 —> 0 and then comparing your
result with the result of part (i).
(iii) If the polymer charge is squeezed between two parallel rectangular plates instead
of disks, would your answer to part (i) change away from the plate edges?
3. While answering part (i) of the previous problem, one student writes on a paper the
following:
Volume — Trr2s = f r (27rr)/i
and then simplifies that equation as vr = rs/(vr/i). Explain what each term corre-
sponds to. What physical law was used? Which of the two models, Hele-Shaw or
lubricating squeeze flow, was used? Is the material- considered to be compressible,
or incompressible? Is this solution valid for a Newtonian fluid as well as for a Non-
Newtonian material?
4. If the material is Newtonian in the previous problems, then what is the required force
F to compress the material by moving the upper plate? (i) If the closing speed of the
disks, s is constant within a time interval, does the required force F stay constant,
increase, or decrease with time? Express F mathematically, (ii) If the applied force is
kept constant, and the initial thickness of the material is h0, then how many seconds
does it take to reduce the thickness to 0.75/i0 and 0.50/i0, respectively? You can
express your answer in terms of F, R, Pa, and fj,.
5. A polymer charge is squeezed between two parallel disks, and inertia and body forces
are neglected. Consider (i) full slip, (ii) no-slip, and (iii) partial slip with (3 = 0.02
where vr — f3rrz, and determine the required compression force on the upper plate to
squeeze it to half its thickness. Express your answer in terms of the closing speed of
plates s = —dh/dt — —h, material viscosity /j,, coefficient /3 and RI the radius of the
disks.

Chapter 7
Advanced Thermoplastic
Composite Manufacturing
Processes
7.1 Introduction
To predict how a material will behave under deformation applied in any manufacturing
operation will depend on the approach selected to describe its macroscopic behavior. For
most thermoplastic materials containing continuous fibers, fiber preforms, or collimated
fibers (long discontinuous fibers in an oriented fiber assembly), one can treat them as a
homogeneous material with anisotropic viscosity or transversely isotropic viscosity with
inextensibility in the fiber direction. However, at the microscopic level there are many phe-
nomena taking place that are conglomerated into constitutive constants at the macroscopic
level to allow for prediction of the deformation rate relationship with the applied force.
The microscopic phenomena that influence the constitutive equations at the macrolevel
are resin percolation, interply (in between the plies) and intraply (within a ply) slip and
shearing. Resin percolation and redistribution are functions of the fiber volume fraction and
the load applied, whereas the shearing within the ply or in between the plies is limited to the
resin rich areas. Experimental studies [275, 111, 276] suggest that this flow of the resin in
between the fibers is a truly viscous flow phenomenon and can be modeled in that fashion.
If the process time scales are large and viscosity is low as in the case of thermoset resins,
shaping operations can squeeze excess resin out. However, as the resin viscosity is high
and usually the process time scales are low for thermoplastics, if one does not understand
the deformation behavior the reinforcing fibers will not be able to adjust to the flow and
buckling and distortion may result. The resin flow is schematically illustrated in Figure 7.1
within a unidirectional fiber bed and fabric tows of a mat, hence the need to understand
the behavior of such materials.
Another change that the thermoplastic reinforced material undergoes is the level of
crystallinity. The rate at which the material is cooled to below the glass transition temper-
ature is the primary process variable, which governs the crystallization in the matrix. The
presence of fibers also provides nucleation sites and can cause secondary crystallization.
In addition to influencing the crystallinity of the matrix, cooling can also cause internal
stresses that can lead to microcracking. The internal stresses are caused due to four major
factors: the mismatch of the coefficient of thermal expansion between the resin and the

(a) (b)
Figure 7.1: Schematic of resin flow through (a) unidirectional fiber mats and (b) woven or
stitched fabrics.
fibers, temperature gradients between the laminates, the orientation of the fibers and the
shape of the part to be manufactured. Usually as the composite is cooled from its processing
temperature below its glass transition temperature, the resin tries to shrink which is resisted
by the stiff inextensible fibers. This places the fibers in compression and the resin in tension.
Similar logic applies to the composite. The composite is cooled from outside to the center.
This would shrink and solidify the outside first, and then the interior is constrained during
its solidification. This puts the outside under compression and the interior under tension.
Hence controlled cooling is an important process parameter during manufacturing of such
materials.
In summary, the inextensibility of the fibers coupled with the high viscosity of the resin
limits the deformation processes that one can attempt for manufacturing operations to shape
these materials into useful end products. The challenges are to be able to model this material
and to ensure that stress build up during cooling is minimum. We will consider modeling
of three thermoplastic composites processing methods in this chapter that underpin the
technology of advanced thermoplastics composites manufacturing. They are sheet forming,
tape layup (also known as fiber tow placement) and thermoplastic pultrusion.
7.2 Composite Sheet Forming Processes

The basic operation in sheet forming is to deform sheets of material into curvilinear shapes
with the help of tools or molds. Sheet forming using isotropic materials or unreinforced
polymers can shear and deform in all directions equally well and allow for formation of
complex structures with compound curvatures. Usually, the material used in advanced
thermoplastic sheet forming is a polymer sheet preimpregnated with unidirectional contin-
uous fibers. A schematic of a lamina, which is an assembly of unidirectional fibers and a
polymeric matrix, is shown in Figure 7.2. This material is highly anisotropic and shows
strong directional effects. Such a material cannot stretch in the fiber direction. Shearing
in other directions has to compensate for inextensibility in the fiber direction to form the
curvilinear shape. The deformation becomes even more complicated when there are several
of these sheets stacked together in different directions to form the composite. The defor-
mation behavior of such laminates of unidirectional fibers oriented in different directions
and stacked together is similar to the use of woven or bidirectional fabrics impregnated

Figure 7.2: A composite lamina of unidirectional fibers impregnated in a polymeric matrix.
in a polymer sheet and stacked together to form the laminate that is then deformed to
contour to the shape of the tool or the mold. Long discontinuous fiber (LDF) material was
introduced to accommodate the stretching mechanism, as the fibers were long and aligned
but the discontinuous nature could create room for stretching.
There are four main composite forming processes: diaphragm forming, matched die
forming, stretch forming and roll forming. Many details of these processes are given in
chapters on sheet forming by O'Bradaigh in [277]. and Bhattacharrya [278]. Here we will
re-iterate the important features of these processes in terms of the deformation mechanisms.
7.2.1 Diaphragm Forming

As shown in Figure 7.3, a laminate of the composite material is sandwiched and heated
between two sheets of diaphragm, and a vacuum or a positive pressure is applied to form
the composite. The edges of the material are not clamped as the inextensibility of the
material can cause fiber wrinkling. The diaphragm material should be able to stretch
without rupture at the forming temperature of the composite. It provides the composite,
which is unrestrained, a guide to adhere to the shape of the tool and also consolidates the
composite. This process allows for the formation of a wrinkle free composite with excellent
thickness tolerance. However, one is limited to the deep draw ratios that can be achieved
due to the inextensibility of the fibers and the inability to find diaphragms that are stiff
enough to prevent the buckling of the laminate and also be flexible enough to stretch to large
extents. Upilex-R material [279, 280] is one of the commonly used diaphragm materials.
The process modeling issues that can be addressed here are consolidation of laminates,
rheology of the material in elongational flows, viscosity dependence on temperature, stretch-
ing/shearing motion of the material, type of boundary conditions to be applied between the
diaphragm and the composite, etc.
7.2.2 Matched Die Forming

In this process, the composite laminate or sheet to be formed is held between two tool sur-
faces and stamped similar to sheet metal forming as shown in Figure 7.4. The advantages
are that one can use the existing metal forming equipment with a few modifications and the
process takes very little time. The disadvantages are that the process is nonisothermal as
the heat has to be transmitted from the metal mold platen and can cause nonuniformity in
the material flow. Also, as the tools are rigid, it can lead to localized high pressures instead
of uniform pressure distribution. Thus, due to nonuniform pressure and temperature distri-

Upper Diaphragm
P+
Lower Diaphragm
Composite Layup Free to Move

Between Diaphragms
To Exhaust
Figure 7.3: Schematic of diaphragm forming process of thermoplastic composite sheets [42].
PLATEN
Mold
Heaters Clamping
Ring
Laminate
Insulation
Mold
mmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmmt
Figure 7.4: Schematic of matched die forming [115].

bution, the chances of failure are much higher than with diaphragm forming. Hence most
match die forming has been practiced on simple shapes with a single degree of curvature
such as channel sections and bends.
The processing issues become more involved as one has to predict the nonuniformity of
pressure due to the nonuniformity of the boundary conditions.
7.2.3 Stretch and Roll Forming

Stretch forming only can be performed with materials that can locally stretch. Continuous
fiber thermoplastics cannot do this but LDF materials can. Hence one can take formed I-
beams or C-channels and stretch them by locally applying heat and pressure with a curved
tool to stretch and then consolidate them as shown in Figure 7.5. Thus, one would have
to characterize the rheology of such materials and examine its microscopic behavior and
macroscopic transverse squeeze flow to model the flow of such materials.
Heating Oven
t t t t t t
Figure 7.5: Consolidation of prepregs.
Roll forming uses a series of rotating rollers to deform a composite sheet into a curvilinear
shape as shown in Figure 7.6. This forming process is different from the others as the
deformation is completed in a series of steps using a series of rollers. Again one must
develop a model to describe the deformation of materials between two rollers to be able to
predict the deformation.
For more details on stretch and roll forming, refer to [9].
(D O
Figure 7.6: Roll forming process of fiber-reinforced materials [9].

7.2.4 Deformation Mechanisms
Deformation in shaping operations can be studied by isolating some of the mechanisms
that occur. When consolidating the various sheets of the composite into a laminate, the
dominant mechanism is consolidation in which the resin redistributes such that resin moves
from resin-rich areas to resin-starved areas on the microscale as shown in the schematic in
Figure 7.7.
Resin Rich Areas
Fibers Resin Starved Areas
Figure 7.7: Schematic of flow of resin from resin-rich areas to resin-starved regions.
In processes such as matched die, there is also transverse flow in which the fibers and
resin move as a unit together when squeezed as shown in Figure 7.8. One can characterize
p
1111 p
O
0 0 0 5°°0°5go?>
O
11 1111
°Jo°uu
0°0°oO°°°'
Q o o oo %°°d- o° o uoobû odo o oo o"
Figure 7.8: Transverse squeeze flow [277].
the rheology of squeezing flow of such materials as a single entity of a viscous material
in order to model their behavior. When forming single curvature parts, in addition to
transverse flow and resin redistribution, one also needs the individual plies to slip over
one another in the laminate to form the part as the stretching mode along the fibers is
unavailable due to the inextensibility of the fibers. Figures 7.9 and 7.10 show the phenomena
of interply slip. Here, one would like to know the force required to pull a ply out from a
stack of plies that have been consolidated. Rheological studies to characterize interply slip
are usually conducted by flexural testing of heated laminates or by ply pull out experiments
at elevated temperatures. Finally, if one is interested in forming double curvature parts, in

addition to resin flow, transverse flow and interply slip, intraply slip and interply rotation
must also occur.
Figure 7.9: Interply shearing [277].
Figure 7.10: Interply deformation: (a) buckling of inner fibers and (b) interply slip [277].
Thus at the microscopic level within each sheet of the thermoplastic material with
unidirectional fibers, the fibers have to move past one another to accommodate a complex
curvature. The fibers can shear past one another. As each fiber is covered with a layer of
resin, one can estimate the force needed for this activity. In addition, the fibers can also
move in the transverse direction. These mechanisms are demonstrated in Figures 7.11(a)
and (b).
Example 7.1: Stretching of Unidirectional Composites [281, 278]

A composite laminate bar is extended in the x direction as shown in Figure 7.12.
The rate of extension of the length can be expressed as
(7.1)
dt

Figure 7.11: Shearing modes: (a) axial intraply, and (b) transverse intraply [277].
Figure 7.12: Elongation of a composite element.
The strain rate in the x-direction may be written as

dL_
• _ dt (7.2)
L '
If at t = 0, the length is L0,
(a) Find the rate at which one should extend L, such that e = constant.
(b) If one extends the length at a constant rate of V = constant, how will e change with
time?
Solution
(a) Integrating Equation (7.2) and using the fact that L — L0 at t = 0 gives
L(t) = L0e«. (7.3)

Hence one has to extend L in an exponential manner to maintain the strain rate constant,
(b) If V = constant, then
= L0 + Vt. (7.4)

Thus dL/dt — V, and one can use Equation (7.2) to obtain
(7.5)
Thus e will reduce as time increases. The elongational viscosity is expressed as
(7.6)
7
In this case, it will be given by

(7.7)
and the stress term is equal to

Force applied in x direction
(7.8)
Cross-sectional area in x direction
7.3 Pultrusion
Pultrusion is a continuous composites manufacturing process. The goal in pultrusion is
to produce a consolidated profile with a constant cross section by pulling impregnated
reinforced material through a heated forming die. The schematic for the process is shown
in Figure 7.13.
Fiber Preimpregnated Cut-off Saw

Pulling *
Tapes or Rovings Mechanism v
Die
Preheater | Assembly
/
Figure 7.13: The schematic of the thermoplastic pultrusion process.
In this process, unidirectional preimpregnated tows, tapes or fiber rovings are guided
through a preheater where their temperature is raised to the melting temperature of the
polymer. Next, the heated polymer and fibers enter a die assembly. A die assembly consists
of a series of dies which consolidate, form and cool the material. Usually, a significant taper
is used in the entrance die to help consolidate the polymer with the fibers. Downstream,
the cooling dies cool the formed product and influences the properties such as crystallinity.
Also, faster cooling can allow one to locate the pulling mechanism closer to the die assembly.
The pulling speeds can vary from a few millimeters per minute to a few meters per minute.

A good design of the dies and heating and cooling mechanism can yield the maximum
achievable speed.
The two important issues to model in pultrusion are the pressure profile in the tapered
section of the die and the pulling force required to pull a profile through the die assembly.
Hence one needs to be able to model flow as well as heat transfer through the die assembly
to predict these important process parameters.
7.3.1 Thermoset Versus Thermoplastics Pultrusion

Physically, thermoset pultrusion involves an addition station of a resin bath between fiber
rovings and the preheater as shown in Figure 2.17 of Chapter 2. Despite this additional
step, the thermoset and thermoplastic pultrusion processes are physically quite similar.
They both pull fibers and resin through a converging die to form continuous composite
sections. However, from an analysis viewpoint, the flow in thermoplastic pultrusion is
modeled differently than in thermoset pultrusion. In thermosets, one uses Darcy's law to
model resin impregnation and the heat transfer involves cure kinetics, whereas in thermo-
plastic pultrusion due to the high viscosity of the material, Darcy's law is not the correct
model to calculate the relationship between flow rate and pressure drop . Also, due to the
shear thinning nature of thermoplastics, one would expect the viscosity to vary inside the
die. The heat transfer models do not usually involve cure but sometimes will consider the
crystallization of the thermoplastic as it passes through the cooloing die.
In this section, the focus will be on development of a model that can describe the flow
dynamics for a thermoplastic matrix as the material passes through the tapering die. The
goal will be to calculate the pressure drop as a function of the pulling speed and material
parameters such as viscosity and fiber volume fraction.
7.3.2 Cell Model [4]

To determine the pressure drop, one must consider the tapered section of the die as shown
in Figure 7.14.
If one assumes that most of the flow is parallel to the fibers, one can divide the tapered
section of the die into self similar cells as shown in Figure 7.14. A cell model is formulated by
considering a single tapered annulus of liquid resin surrounding each fiber. This assumption
allows one to simplify the problem to a one-dimensional problem in the direction of the fiber
movement. Also, due to the cylindrical nature of the fiber, we will assume that the annulus
of the resin is also circular; thus one can choose the cylindrical coordinate system to pose
the problem.
If one ignores gravity and inertia as these materials are very viscous and assumes sym-
metry in the 9 direction, one can simplify the equation of motion in the axial direction
to
u— — ,-,— +i --—
0— (rr'rzl} +—-(T
<-, V }
i ,-, \'zzl- (79}
\'- )y
dz r dr dz
Now as the cell dimensions in the radial direction are of the order of a few microns, whereas
in the axial direction they could be 3 to 6 orders of magnitude larger, one can assume that
drzz/dz «C drrz/dr and hence eliminate the last term in Equation (7.9). This assumption
simplifies it to
^dz = r- or
£ (-„). (7-10)
Now one needs an equation to describe the stress-strain relationship before one can proceed
further. We will assume a constitutive equation which encompasses Newtonian as well as

a unit cell
Fiber
Resin
v
Figure 7.14: Concept of unit cell in pultrusion [4].
shear thinning fluid models:

dur duz
(7.11)
dz dr
where rj can be a function of the shear rate.
As R -C L and u r <C w 2 , dur/dz ~ 0 thus substituting Equation (7.11) into Equation
(7.10), for Newtonian fluids we obtain
dP r\ d duz
(7.12)
r dr dr
The pulling mechanism of the fibers in the axial direction induces a drag flow in that
direction. However due to the tapering geometry, the material experiences a pressure build-
up. This makes the resin pressure higher near the exit of the die as compared to the
entrance. Hence a pressure gradient is established in the opposing direction to drag flow,
which may give rise to back flow. The boundary conditions for Equation (7.12) are
at r = Rf (7.13)
duz
=0 at r = R. (7.14)
dr
Here R is the outer radius of the annulus and is a function of z due to the taper in the z
direction, and U is the pulling speed with which the fibers are moving through the die. Rf
is the radius of the fiber. The diameter of the resin annuli at the entrance and exit of the
taper are defined by the fiber volume fractions VQ at the entrance and v± at the exit. The
zero velocity gradient at the cell interface imposes the symmetry boundary condition of no
flow in and out of each cell. At the end of the taper as shown in Figure 7.14, the velocity
is uniform and no pressure gradient exists.

The flow pattern that satisfies all these boundary conditions is schematically shown in
Figure 7.15 for two adjacent cells.
R(z)
Figure 7.15: Flow profile in two adjacent cells [4].
Notice that so far we have not utilized the continuity equation. We know that the flow
rate of the resin has to be constant throughout the taper in order to satisfy the continuity
equation. The flow rate at the end of the taper and in the uniform section of the die, where
the velocity is uniform can be expressed as
(7.15)
where Re is the radius of the annulus at the end of the taper. One should expect that at
any axial position along z, the flow rate should be the same. Note that, v\ = irR^f/itR^,
and the radius of the annulus at the inlet, Ri is related to initial fiber volume fraction of
irR2,
V
° = ^R*-
At any cross section along z, the flow rate Q is the sum of plug flow induced by fiber
drag and backflow generated due to the opposing pressure gradient as shown in Figure 7.16.
As the resin is Newtonian, one can superimpose these flows
Q = Qdrag + Qbackflow = Re -Rf (7.16)
The drag flow is uniform due to the slip boundary condition at the end of the annulus. This
slip boundary condition is the same as symmetry or no flow out of the cell boundary. Thus
(7.17)
and hence
Qbackflow = Q ~ Qdrag = UlT -R2(z (7.18)
at any cross section along the axial direction, z.

Figure 7.16: Velocity profile in the tapered section of the die. The velocity is considered to
be the sum of plug flow and backflow [4].
One can also find the total flow rate at any cross section by integrating Equation (7.12)
to find the velocity profile, uz, and relating it to the flow rate as shown below:
27T fR(z)
Q= o JR
uzr dr d0. (7.19)
By equating Equation (7.16) and Equation (7.19), one can find details of the flow pattern
and pressure gradient, once we have a rheological form that describes the viscosity T] of the
thermoplastic material.
Let us assume the fluid is Newtonian and that the viscosity does not vary appreciably
with temperature. One can now integrate Equation (7.12) to obtain the velocity profile
which is
f
4// dz [ \ r )\
Note here that uz varies with r which is between R and Rf. Substituting Equation (7.20)
into Equation (7.19) and integrating it results in
pressure driven flow

(7.21)
drag flow

Thus equating the pressure driven flow in Equation (7.21) to Equation (7.18), the pressure
driven flow or Qbackflow results in
Qbackflow = V
TT_dP_
8/j, dz
Inverting Equation (7.22) gives the pressure gradient along the tapered section of the die
(7.23)
£
- 4 ( £ M ~ + (S r + 41n
One can integrate equation (7.23) with respect to z to find the pressure profile along
the z direction. This pressure profile will be a function of the viscosity of the material, the
pulling speed, the taper of the die and the final fiber volume fraction desired.
Example 7.2: Producing a Pultruded Profile

You have been asked to produce a pultruded profile with a final fiber volume fraction of
50%. The die is already made and has a linear taper and a length of 20 cm. The initial
fiber volume fraction in the incoming rovings of fiber radius of 20 mm is 40%. The viscosity
of the thermoplastic can be assumed to be Newtonian and is equal to 10,000 Poise (= 1000
Pa.s). Find the maximum speed with which you can pull the rovings through the die if the
maximum gage pressure inside the die cannot exceed 1 MPa.
Solution:
Given,
V0 = 0.40
Vl = 0.50
Rf = 0.020 m
L = 0.2m
M = 1000 Pa.s
10 6 Pa
(7.24)
(7.25)
(7.26)
Substitute Equations (7.24), (7.25) and (7.26) into Equation (7.23), and integrate with
respect to z to obtain the pressure profile
- z,

Note that the maximum pressure occurs at z — L:
P(L)-P(0) = Pmax
a
= L
L dz'. (7.28)
Substituting Pmax and L into Equation 7.28 and inverting the equation, U is found. One
can use a mathematical solver program such as Maple [282] or Matlab [283] to calculate
the integral and solve for U as shown in Figure 7.17. The critical value of U is found to be
vO «=• 0.40:
vl = 0.50:
Rf = 0.020:
:L ~ 0,2:
- 1000:
Pin ax •"• 1.0E6:
Rin
8w~. 03 162277660
> Rex = sqrt(Rf A 2/vl) ;
&j;t = .02828427125
> ratio = Rf/Rex;
miio =.7071067811
= ( (Rex-RIn) /I.,) *z+Rin;
U) =......01669252675Z r .03162277660
> u = Pmax /
lot < <8*mu*pi*(R<S3[:-"-2- < R < B ) } '"'2} ) /<p.i.
*(3-4*ratio A 2+ratio A 4+4*ln{ratio) )
z-0. . L ) ;
U~. 7480135211
r>
Figure 7.17: Use of Mathematical Solver MAPLE [282] to solve for U.
0.75 m/s. If one pulls the rovings with this critical speed, then the pressure at the exit of
the die will be 1 MPa.
The pressure profile along the z axis is plotted in Figure 7.18. •
Shear Thinning Thermoplastics

Most thermoplastics exhibit shear thinning behavior. As studied in Chapter 4, there are
many different models to describe the shear thinning nature. Here we will consider only the
power-law model, although it is quite straightforward to extend the analysis to Carreau or
other detailed models for the resin.
The power-law model describes the viscosity as
= 7«7 (7.29)

xicr
ro
Q_
0.05 0.1 0.15 0.2
z[m]
Figure 7.18: Pressure profile along the axial z direction in the tapering die during the
pultrusion process. The rovings are pulled with 0.75 m/s.
where m and n are curve fitting parameters and 7 is the magnitude to the strain rate tensor.
One can recover the Newtonian fluid model by choosing m = /j, and n = 1. One can start
with Equation (7.10), and integrate with respect to r using the boundary condition that at
r — R, the shear stress is zero. This results in the shear stress profile
IdP
r— (7.30)
2~dz
For the power-law fluid model,
duz
—r- = —m (7.31)
dr dr V dr
The combination of Equations (7.30) and (7.31) results in
,1/n
duz _ R2
(7.32)
dr 2m dz
One must integrate uz with respect to r to find the velocity profile. Once the velocity profile
is known using the conservation of flow rate equation, one can obtain the expression for
dP/dz along the fiber direction.
Example 7.3: Derive the Pressure Profile for a Shear Thinning Thermoplastic
Composite Being Pultruded
Find the expression for dP/dz for a composite being pultruded through a die. The ther-
moplastic matrix in the composite exhibits shear thinning behavior which can be modeled

by using the power-law model. Consider two cases, (a) the power-law index is 1/2, and (b)
the power-law index is 1/3.
Solution (a):
Substituting n = 1/2 in Equation (7.32) and integrating with the boundary conditions listed
in Equations (7.13) and (7.14) gives
R L o RfL 1 RfL
uz = — U (7.33)
\2m dz J Rf+ R 3 R3
if X = R/Rf, then
/ 1 dP\*
= — -- (7.34)
dz
and using Equations (7.18) and (7.19)
1 dP\' 8 J_ 3A __ A 3 A^ N
= -2?r (7.35)
2m dz J ~5 + 2A + T " Y + To
Thus
One needs to invert Equation (7.36) to find dP/dz as a function of R(z).
Solution (b):
For n = 1/3,
-(——V
\2m dz J 5ji-F+i*V l+l7 - ' (7.37)
Thus
Qbackflow -
Again, one must invert Equation (7.38) to be able to integrate the pressure as a function
of z. Figure 7.19 illustrates the effect of power-law exponent on the pressure profile using
dimensionless variables. •

Figure 7.19: Effect of the power-law exponent on the pressure profile in thermoplastic
pultrusion.
7.4 Thermal Model

In the tapered die, one would expect heat generation by viscous dissipation. As one can
calculate the velocity profile by using the concept of a cell model, it is possible to estimate
the amount of heat generated due to viscous dissipation and its contribution to raising the
temperature of the thermoplastic. The viscosity of thermoplastics is also a strong function
of the temperature. For example, the viscosity of polypropylene reduces by 50% as the
temperature increases from 190°C to 240°C. Such a variation has a significant influence
on the pressure profile. Ideally, one may have to solve the equation of motion and energy
equation simultaneously due to the two-way coupling between them. That is, the viscosity
influences the temperature through viscous dissipation term in the energy equation and
the temperature influences the viscosity in the equation of motion. However, here we will
analyze and simplify the energy equation retaining the viscous dissipation term. In order
to obtain a closed form solution, we will assume that the viscosity is constant inside the
unit cell.
7.4.1 Transient Heat Transfer Equation

The complete energy equation with heat generation in an anisotropic medium in cylindrical
coordinates is given as
DT I 8 i~* dT\ I 32T o2T TI
~Dt a
r or drj^ " dz2 r dOdz
2
, dT 2
dT
q(r, 0, z, t) (7.39)
1 z v z
" drdz ' "" ' *"' rdedz
Here fc^ 's are components of the thermal conductivity tensor and q is the rate of internal
energy generation per unit volume. In this case, it represents the energy generated due to
viscous dissipation.

If one- assumes that the principle axes coincide with the fiber direction, one can reduce
the kij matrix to take on the diagonal form (i.e., fcjj = 0 when i ^ j). Also due to the
axisymmetric nature of the problem, one can eliminate 9 dependency.
With these assumptions, the energy equation simplifies to
, I d ( dT\ d / dT\ . DT ._ An.
k r k C 7 40
rr -r IT
dr (V 7T dz (\z z IT
dr J + 7T dz J)+ 9 = P P' TTT-
Dt '
Now
DT dT dT dT
+u
TTT
Dt = -aT dt r-»-
dr + ^7T-dz
Once the pultrusion has achieved a steady state within the die, one will not expect T to
change with time; hence ^ = 0 is not an unreasonable assumption. Also, ur §£• -C uz -^
which will be the case here as uz = U (the pulling speed) where as ur « 0. Thus
DT dT
U
^-Dl- = <*> W
Hence,
.
k 1 d ( dT\ d / dT\ TTdT lrj _.
rr-^~ r-s- 4-^ Uzz — )+q = pcpU—. 7.43
r dr \ dr J dz \ dz J ^ dz
Also the axial conduction term ^;(kzz fij) could be neglected as L is much longer than r
and one would expect most of the heat to be conducted radially. Thus, the final simplified
form for the energy equation is
r Qr \ • a~ I ' . ^ . r~i>~ £,„ • (7.44)

v
energy generation ,. ,., ,
conduction in due ^ yiscous convection of heat
radial direction ,. . , . in axial direction
dissipation
1 , , ,, ,,.
due to the pulling
of the fibers
through the die
We need two boundary conditions in the r direction and one in the z direction to uniquely
determine T(r, z). The boundary conditions related to the temperature field in a pultrusion
die can be modeled as
T(r, 0) = Ti (7.45a)
dT
— =0 or T(0, z) = finite (7.45b)
T(Rd,z}=Tw. (7.45c)
Here Ti is the preheater temperature, Rj is the radius of the taper. Equation (7.44) can be
solved using separation of variables.
^ ^RdJl(*nRd)
n=l
+ ——
4fc
/
'-
r6 JJQ\
n(\
A r}dr\
n')(J'l\
"vn> - ^z/u
Ae a (7
V-^460\
)
T2M D

where \nRd satisfies J$(\nRd) = 0. JQ and J\ are Bessel functions and a is the thermal
diffusivity, a — (krr}c/(pcp)c. Here (krr)c and (pcp}c are averaged composite properties
determined used rule of mixture
Vf (7.47)
k
(pcp)c = (l-V})pmcm + V f p f c f (7.48)
where the subscripts m and / represent matrix and fiber materials, respectively. The
particular solution that will satisfy boundary condition in Equation (7.45b) and (7.45c) is
Ts(r) = TW + - L - Rl - r 2 . (7.49)
The overall temperature solution can be calculated by superimposing Equations (7.49)

and (7.46).
i
7.4.2 Viscous Dissipation

In the tapered section, one can assume that internal energy generation is due to viscous
dissipation
q(r,0,z,t)=ri<t> (7.50)
where 77 is the viscosity and (j> is the dissipation function that describes the irreversible con-
version of mechanical energy into thermal energy. For this one-dimensional, axisymmetric
flow, the shearing of uz in the radial direction is the only dominant term. Hence,
One needs to find the average heat generated per unit volume of the cell to be used in the
energy equation. This is done by using average shearing of uz in the radial direction
« , „ „ , , , „ , rdrdO
(IT /I average
*-"
where R refers to the local radius of the cell model. Thus, dissipation will not be constant
along the taper and will vary as R changes along z.
(7.53)
where A = Rf/R. Thus the viscous dissipation term varies with the square of the pressure
gradient and the square of R. If one substitutes Equation (7.23) for dP/dz in Equation
(7.53), one could plot how viscous dissipation changes with R(z).
This viscous dissipation can then be included in Equation (7.44) and solved to evaluate
the impact of the q term on the temperature profile. There is no closed form solution for
this, but one could easily develop a finite difference solution for this problem.

Example 7.4: Nondimensionalization of Simplified Energy Equation in Thermo-
plastic Pultrusion
Nondimensionalize Equation (7.43).
Solution
If we use the following nondimensional variables,
ctrrz . ,
(7.54a)
f= (7 54c)
JTd '
<fc = If (7.54d)
and choose
7? TJ
Pe = Peclet number = - (7.55a)
arr
riU2
Br — Brinkman number = - . (7.55b)
we get
Usually Pe « 102 to 103; hence one can easily discard |^ -p- ^^ term. The last term on
the right-hand side of Equation (7.56) can make a significant contribution even for small
values of Br number as there are many fibers and hence many cells inside the tapering die
directly adding to the heat generation. •
7.5 On-line Consolidation of Thermoplastics

Consolidation in a composite manufacturing process is accomplished by applying pressure
and heat to the system to squeeze the air, volatiles and excess resin out of the composite
structure. It is a complex phenomenon with simultaneous transfer of mass, momentum and
energy. The main goal of consolidation is to produce a monolithic structure by inducing
intimate contact and adhesion between individual plies and minimizing void content inside
the composite.
As seen in previous chapters advanced composites are made from discrete plies. The
plies consist of a tow of usually thousands of fiber strands partially or fully impregnated with
resin. These plies are also referred to as tows or tapes. The approach in sheet forming in the
previous section was to arrange and stack the plies in the required structure configuration
and to apply heat and pressure to consolidate them to the desired geometry. Such processes

are called post layup processes. On the other hand, one can consolidate the structure
attaching one ply at a time. This process is known as in-situ or on-line consolidation.
On-line consolidation or in-situ consolidation refers to creation of a composite when
thermoplastic prepregs or tapes are fused and compacted. This is done by locally heating
and cooling the tapes as they are placed over a tool using a path trajectory to form the
geometric shape of interest as shown in Figure 7.20. This form of in-situ processing allows
one to place the reinforcing fibers in the desired directions without the constraint of following
a near-geodesic path. The method can be potentially used to include even non-axisymmetric
shapes. Two processes have emerged and been successfully used over the last ten years that
fall under this category. They are thermoplastic filament winding and thermoplastic tow
placement. The attractive features of these processes are that they easily lend themselves
to automation and residual stresses are negligible.
Prepreg spool
&
Tensioner
.«#*• Pre-heater
Consolidation roller
Direction of head travel * A \ p\ / />Nip point heater

Substrate layer
Tool
Figure 7.20: A thermoplastic fiber-reinforced tape being consolidated to the substrate layer
with heating mechanism and consolidation roller.
As shown in Figure 7.20, there are five main components in this process. They are
the preheater, tensioner, nip(contact)-point heater, consolidation roller and a tool for the
placement of the fiber tows to form the composite.
The tensioner is used to mechanically maintain constant tension within the fiber tow
from the moment it leaves the supply spool until it is wound on the tool or the previously
placed fiber tows on the tool.
The tool, which is known as a mandrel in filament winding and as a tape-laying head in
the tow placement manufacturing method respectively, is the surface on which the fiber tows
are placed and wound to create the geometric form of the composite structure. In the case
of filament winding, it is cylindrical in form, whereas in tow placement it can take various
complex forms based on the geometry of the part to be manufactured. Usually metals
such as stainless steel or aluminum are used to form the tool because of their durability
and resistance to oxidation. The tool is usually heated to avoid creation of large thermal
gradients between the heated tow and the mandrel. The large thermal mass of the tool
can act as a heat sink, lower the matrix temperature of incoming tow and limit the inter-
laminar flow of the molten polymer. Therefore, a heated tool is necessary to retain heat in

previously wound layers. This is usually accomplished by blowing hot air into the hollow
of the tool or, if higher temperatures are desired, resorting to electrically heated nitrogen
torches.
A thermocouple is usually placed on the outer surface of the tool to provide the feedback
to maintain the tool temperature to the desired value. A common problem is the removal
of the tool from the part. For example, if one is interested in making pipes, the process is to
wind the fiber tows over a mandrel and then remove the mandrel after the desired OD of the
pipes has been achieved. Usually a press or a collar fixture is used to slide the part from the
mandrel. If the composite to be wound consists of carbon fibers and a thermoplastic matrix
such as PEKK, the part can be easily removed upon cooling, as the thermal coefficient of
stainless steel is much higher than that of the composite.
The stainless steel compaction roller allows for the application of consolidation pressure
to fuse and compact the incoming fiber tow with the previously placed fiber tow. Although
the compaction roller may be preheated, it is generally not done, as due to low thermal
mass and short contact times, it does not influence the temperature field to any significant
degree. As the roller temperature is usually lower than the glass transition temperature
of the thermoplastic, the incoming tow will tack on to the laminate rather than the roller.
One can also monitor roller temperature if necessary with a sliding surface thermocouple.
Once a layer has been wound on the part being created, the thickness of the composite
part increases. This requires the compaction roller to move away from the tool while still
continuing to apply constant pressure. One way to address this issue is to attach the roller
to a sliding plate mounted vertically on the frame. The constant pressure is usually applied
with the help of a pneumatic cylinder. The compaction force can range from 0 to 100 kN
over the contact area.
The heater used in the preheating chamber must be easily controllable while supplying
sufficient energy to raise the tow temperature to the desired level. Infra red strip heaters
can do the job mounted equidistant from the tow along the top and the bottom surfaces.
The heater power will be a function of tow speed, the material properties of the tow, and
the temperature change one wants the tow to undergo.
Example 7.5: Power Requirement by a Heater
Find the heater power required to heat a tow from 30°C to 130°C. Assume that 20% of the
heater energy is lost to surroundings.
Solution
Qt = mcPt(Tp-Tr]
= PtVtwtttcPt(Tp - Tr) (7.57)
where

Pt density of the tow
vt velocity of the tow
wt width of the tow
tt thickness of the tow
c
pt specific heat capacity of the tow
Tp and Tr incoming and exit temperatures of the tow in the preheater.
Hence, due to losses, the power required is
Heater Power = - - . (7.58)

O.oO
The requirements of the nip- or contact-point heater are the same as the preheater
except the nip-point heaters are focused only at the point of contact of the incoming tow
and the previously placed tows. The nip-point heater should induce rapid heating to bring
the contact area to above the melting point of the resin instantly as the contact time is
usually very short. A variety of heaters can be used for this purpose. Some examples are
open torch, laser, hot gas, infrared and heated rollers, or hot shoes.
7.5.1 Introduction to Consolidation Model

There are several important issues during the consolidation process employed in composites
manufacturing. The key process parameters that influence the extent of consolidation are
the applied pressure, temperature, and time required for consolidation. Many phenomena
such as intimate contact between two adjacent plies, resin flow across and in between the
plies, adhesion, fiber deformation and movement, molecular interdiffusion, and diffusivity of
air and volatiles in the molten matrix occur simultaneously during the consolidation process.
There are complex interactions among all these phenomena. Thus, consolidation will be a
function of process parameters such as the rate of application of pressure and temperature
and also material parameters such as resin and fiber properties, the fiber volume fraction,
and the state of the initial plies. The interactions between mass, momentum and energy
transfer can be investigated by classifying them on macro-, micro- and molecular levels.
The macrolevel analysis will allow us to establish the process windows of temperature,
pressure, and time required to achieve complete consolidation. At the microlevel, one can
investigate the effect of temperature and pressure on the size of individual voids and thus
on the macroscopic density [284]. At the molecular level, one is concerned about intimate
contact between two adjacent plies and diffusion of polymer chains across the ply interfaces
[285, 286] The process and material parameters affect phenomena at all scales, and the
degree and mechanism of their interactions will depend on whether it is a post-consolidation
or an on-line consolidation process [287]. The objective is to identify the mass, momentum,
and energy transport mechanisms during the consolidation process so that one can establish
their relative contribution and significance in the consolidation process. In on-line processes,
the layup of plies and consolidation occur simultaneously.
7.5.2 Importance of Process Modeling

The phenomenon of consolidation during tow placement of composites may be mathemat-
ically modeled as the flow of a compressible viscous fluid. Such a model helps provide

insight into the effect of the process parameters, such as the tow speed and the compaction
force and about the variables of interest, such as the final void fraction and part thickness.
Typically, the final void fraction of a composite is used as an estimate of the part quality.
Therefore, the process inputs may be determined such that the quality requirement, for
example < 1% void fraction, is satisfied. Also, the model may be used as part of an on-line
control strategy for a tow placement process. Ideally, using a porosity sensor at the post-
consolidation stage, the part porosity may be compared to the required value. If the quality
requirement is not satisfied, the model may be used to correct the inputs appropriately to
achieve the required porosity level. The process model also enables one to optimize the
process in such a manner that the manufacturing speed is at the highest possible level given
other constraints such as the machine limitations for compaction force and the desired final
product quality. A typical situation is shown in Figure 7.21. The maximum compaction
Compaction Force
Machine Limit
Processing Speed
Required Porosity
Porosity
Maximum Speed
Figure 7.21: Obtaining the highest processing speed from a typical porosity-speed-force sur-
face, taking into account machine limits and quality requirements for on-line consolidation
force the machine is capable of providing may be used as the limiting condition. Section A
is taken at this level, and its projection on the processing speed-porosity plane is obtained.
The maximum acceptable porosity can now be used to determine the maximum processing
speed by following the line BCD. The line BC runs parallel to the processing speed axis
at the required porosity value until it intersects the projection of section A. The line CD
runs parallel to the porosity axis until it intersects the processing speed axis. The point
D represents the highest processing speed that can be used to obtain a part of acceptable

quality. A processing window may be defined based on the maximum force and processing
speed the machine is capable of operating at.
The process model (i) assists in development of the tow placement equipment, commonly
called the thermoplastic tow placement head, (ii) assists in design choices, (iii) reduces the
time to establish a working process window when the new process and equipment are used,
and (iv) assists in process control.
7.5.3 Consolidation Process Model

Thermoplastic matrices in advanced composites applications are highly viscous compared
to thermosets. Thermoset composites processing has been conventionally modeled as flow
of resin through a network of fibers, which is described well by Darcy's law. This is valid
for processes such as autoclave thermoset processing due to the low viscosity of thermosets
prior to cure initiation. However, due to the high viscosity of thermoplastics, it has been
observed that the fibers move with the resin rather than relative to the resin. Therefore,
the approach best suited for thermoplastic composite consolidation is a squeeze flow model.
The fibers, resin and any voids present in the tow are approximated as a homogeneous fluid
with specified rheological properties. The rheological properties of this continuum depend
on the temperature, the fiber volume fraction, and the void content.
7.5.4 Model Assumptions and Simplifications

The simplification of the geometry and the location of the consolidation of thermoplastic
composites during tape layup or filament winding is shown in Figure 7.22. This process
Compaction
Roller
Figure 7.22: Location of the coordinate axes for the consolidation process [284].
may be modeled as shown in Figure 7.23. A tow of a given height, hi, and width, Wi, enters
the region under the compaction roller. The coordinate system is defined such that x is
the width direction, y is the direction of tow movement and z is the thickness direction.
The tow speed, V, is specified. As the tow passes under the compaction roller, its height is
reduced to hf and its width changes to Wf. The consolidation force compresses the voids
and changes the height and width of the tow. Since the tow dimension in the y direction is
much larger than in the x and z dimensions, the y direction flow may be neglected. Due to
the high matrix resin viscosity, the flow may be treated as creeping motion and the inertial
effects can be neglected.

X \ Consolidation^^
Fiber-resin mixture
region
Section A-A (b)
(a)
(c)
Figure 7.23: Schematic of the various views of the consolidation squeeze flow model with
the input variables [284].
7.5.5 Governing Equations

The continuity and momentum equations that govern the motion of the fluid under the
compaction roller, neglecting inertia and body force terms, may be written as,
o
dp d
-7^(pvz} = 0 (7.59a)
d~t
dP __d_
^~ (7.59b)
dx dx dx dz
dP d dvx dv d dvz (7.59c)
^~
dz "H~
dx ^~
dz ~5~
dz
The density and viscosity of the continuum are given by p and /i, the pressure in the
material by P, and the velocity by v. In actual tows, the thickness (0.006") is much smaller
than the width (0.25"). Therefore, the dominant velocity gradient term in the momentum
equations is the shear strain rate through the gap, dvx/dz and its derivative with respect
to the thickness direction, z. Therefore, the momentum equations, Equations (7.59b) and
(7.59c), may be simplified as,
dP_ d_
(7.60a)
dx ~dz dz
dP
(7.60b)

Here Newtonian constitutive law is assumed. It should be straightforward to extend it to
shear thinning fluids. From Equation (7.60b), it is clear that P = P(x). The density of
the continuum is affected only by the local pressure. Therefore, the spatial variation of the
density may also be approximated as a function of x only and Equation (7.59a) may be
rewritten as,
Equation (7.61) may be integrated in the thickness direction from 0 to h, the instantaneous
thickness of the domain.
h
d + / \ir(pVx) dz+ v
p( ^=o = °- (7-62)
The velocity vz at z = 0 is 0 and at z = h is h, the closing speed between the two
bounding surfaces. Substituting these values and interchanging the order of integration
and differentiation in Equation (7.62) results in
.„ , .„ . vxdz + ph — 0. (7.63)
at ox \ Jo )
Equation (7.60a) may be integrated with respect to z to yield,
„[£]= ,£ + Cl(l) . (7 . 64 )
Laz j ax
Integrating Equation (7.64) once more with respect to z,
,~x dP fz £ _ „ , . fz I ,.
(7.65)
ax Jo fi Jo ^
where £ is a dummy variable of integration. The value for vx from Equation (7.65) may be
substituted into Equation (7.63) to eliminate velocity as a variable and maintain pressure
as the only variable to be solved
The values of C\(x) and vx(0) may be obtained from two velocity boundary conditions.
Since we have a second order equation for pressure, two pressure boundary conditions are
also needed.
Let p* be the nondimensionalized density of the continuum defined as,
p* = ^ (7.67)
Pf
where p is the density of the continuum and pf is the density of the composite with no
voids. Equation (7.66) can be rewritten as,
1^7- ( * I fh
9 \P
W,+ -z- Z t
^> JA * /~i t —\
fZ
I
1
_7A I _7 _ 1 i _*7 n /y rjo\
at ax y Jo o fJ. Jo M ' '

Equation (7.68) is the general form of the macroscopic governing equation for consolidation
in which one is squeezing the voids out of the composite. This equation can be specialized
depending on the particular problem that is to be solved (such as isothermal incompress-
ible, isothermal compressible, etc.). However, first we must have a model to describe void
mechanisms at the microscopic level.
Void Reduction Mechanisms and Models
Voids may be broadly characterized as interlaminar or intralaminar. Interlaminar voids

will not be addressed in this work. Existing models for degree of intimate contact may be
used to model them (for example see [289, 290, 291, 292, 293]). The focus here will be
on the growth/collapse and transport of intralaminar voids. The various mechanisms of
intralaminar void growth/collapse and transport are shown in Figure 7.24 schematically.
Void coalescing may occur when the voids in a tow grow or move in such a manner that
the boundaries of two or more bubbles meet; this leads to the formation of a bigger void
of a different shape. Since our aim is to model void compression under the compaction
roller, this mechanism is not of importance. The voids may migrate due to the pressure
gradient in the fluid or other mechanical motions [294, 295, 296]). The transport of the
voids along with the resin can be addressed here, but void migration relative to the resin
has been neglected because the high viscosity of the resin impedes any such motion. In the
region of interest, cooling of the tow takes place and should lead to reduction of the void
size. This contraction can be taken into account using the ideal gas law. Void compression
also takes place due to the applied compaction pressure. The effects of heat input and void
compression are taken into account using a microscopic model. The effect of void transport
is accounted for in the macroscopic flow model.
0 0
° o&00ocb°o.0d00o
Void Coalescing Void Migration
O
U O- OO o^\ Or\ r\°
O O oPOD °0 cO o
Void Bubbling Void Compression

Figure 7.24: Different void mechanisms for intralaminar growth/collapse and transport.

Microscopic Model
A typical void at any location is approximated by a sphere of radius R, as shown in Fig-

ure 7.25. The void is assumed to be surrounded by a concentric spherical resin shell of outer
radius S. The ratio of R and S is determined by the void fraction at the location under
consideration. Void growth or collapse is governed by a balance between the pressure inside
and outside the void, the surface tension and the resin viscosity [294].
r>3
-1 - - (7.69)
The initial radii of the void and the resin shell are R0 and S0, respectively. Pg and Pf are
the gas and resin pressure inside and outside the shell, respectively. The resin is assumed
to be incompressible; therefore
= Jr-3 n3
0 - ri0. (7.70)
Also, from the ideal gas law,

Pg0Rl _ PgR3
(7.71)
^r^~^T
The radius of the void and the shell of resin may be expressed in non-dimensional form as,
(7.72)
Ro
R* = — (7.73)
RO
Equation (7.69) may now be rewritten using Equations (7.70) and (7.71) as,
dR* Pgo T
-1 =0 (7.74)
~dT T0
Void fraction distribution

Equivalent volume
of fluid
Mean void
fraction
O O
Axis of symmetry
Figure 7.25: Microscopic void compression model used to determine the bubble radius as a
function of the local pressure and temperature.

It can be shown that the rate of change of p* with respect to time can be expressed in
terms of the rate of change of the nondimensional radius of void as
dp* -3fl* 2 (S 0 * 3 -l) dR*

dt ~ (Sf-l + R*3)* dt ' {
'
Thus the rate of change of the nondimensional density with respect to time may be obtained
using Equations (7.74) and (7.75). The coupling between the microscopic model and the
macroscopic pressure distribution is obtained by substituting Equation (7.75) in (7.68) to
compute the pressure distribution in the domain. Equation (7.74) can be used to compute
the individual change in the radius of the voids at various locations in the domain.
Example 7.6: Bulk Density and Voids

Derive the expression for change in bulk density due to void compression (Equation 7.75).
Solution
Initially, the composite material occupies a hollow spherical volume between r = R0 and
r = S0. The mass of the composite material excluding the void in it, m/ is given as
( 7 - 76 )
where pf is the density of the composite material excluding the void in it. At any time, the
mass of the cell (composite material including the void) is given as
m = m/ + mvoid = p — S3 (7.77)
o
where p is the density of the composite material including the void and S is the radius of
the cell at that time. If one neglects mvojd relative to m/, then
(7.78)
which reduces to
If one takes the time derivative of both sides of Equation (7.79), the following is obtained
dp* _ 8
~dt ~ ~di
= -3^ f. (7.80)
Time derivative of Equation (7.70) allows one to express dS/dt in terms of dR/dt
CL . _.o.. CL , ™Q T-.Q -r-.Q\
dt dt
2
dS _ R dR
~dt ~ 52 dr

By substituting for ^ from Equation (7.80) into Equation (7.81), one can obtain the
following:
= 0 0 dR
6
dt S dt
dR
dt
{
"°\wj '"'u,;
(S*3-1 + R*3}2 dt ' (
'
which is Equation (7.75). •

Two velocity boundary conditions and two pressure boundary conditions are needed to
obtain the solution for the governing equations. The velocity boundary conditions will be
addressed first.
Velocity Boundary Conditions

There has been some speculation in the literature (e.g., [294]) about the type of velocity
boundary conditions that needs to be imposed at the interface between the fluid and solid
in processes such as compression molding. The problem under consideration is similar in
nature to compression molding as far as the velocity boundary conditions are concerned.
Traditionally, a no-slip boundary condition is imposed at the interface between a fluid and
a solid wall. This implies that the friction between the fluid and the wall is much greater
than the internal friction (due to the viscosity) in the fluid. However, in some cases a more
appropriate boundary condition is partial or limited slip at a fluid-solid interface. Such a
condition may be thought of as a friction factor boundary condition and expressed as,
AM ^- ) = #wall '"wall (7.83)
The ratio ETwau//i (j3 in Equation (6.45)) determines the type of boundary condition
that is imposed. If one expects the friction to be very high, i.e., Kwau//j, —> oo, it is clear
that wwaii must be zero such that the left hand side is finite. This is equivalent to a no-
slip boundary condition. On the other hand, if the friction is expected to be very low,
i.e., Kwaiif/j, —> 0, the normal derivative of the velocity goes to zero at the wall. This is
equivalent to a perfect slip boundary condition. Therefore, this friction factor boundary
condition may be used to impose all types of velocity boundary conditions ranging from
no-slip to perfect slip.

Pressure Boundary Conditions
We also need pressure boundary conditions to solve the consolidation problem uniquely. If
the tow is assumed to be unrestricted along the width, i.e., there are no tows that have been
laid adjacent to it, then the appropriate boundary condition would be to impose atmospheric
pressure at the free surfaces. However, if the tow being considered has neighboring tows on
one or both sides, then the boundary condition on the constrained edge needs to be modified.
We do not expect any flow to take place out of the constrained edges and therefore need to
impose a zero pressure gradient condition at these edges. The pressure boundary conditions
may be summarized as follows:
unconstrained edge atmospheric
\ Ox / constrained edge = °
(TT)
While considering the tow that is being laid down, we apply the free surface bound-
ary condition because the unconsolidated tow width is smaller than the consolidated tow
width. However, for a tow that was placed previously, one applies the constrained boundary
condition because it has tows along both edges of the width.
7.5.7 Rheology of the Composite

An important input to the consolidation process models described above is the viscosity of
the composite. The composite consists of fibers, resins and voids. This combination may
be treated as a continuum on length scales that are much greater than their individual
dimensions. The viscosity of this continuum needs to be determined experimentally.
Previously, the viscosity of heterogeneous media has been measured using capillary
rheometers, cone and plate rheometers and dynamic mechanical analysis. However, for
application in a consolidation process model, the squeeze flow (transverse shear) viscosity
of the composite is required. This is not obtainable using any of the above mentioned
equipment. Therefore, the resistance of a composite laminate to squeezing should be used
to estimate the transverse shear viscosity.
Example 7.7: Characterization of the Viscosity of AS4 Fibers with PEKK Resin
A constant load with a heating unit attached is used to characterize the viscosity of AS4
fibers with PEKK resin. The specimen, which is a ten layered consolidated AS4/PEKK
laminate, was placed inside an oven using a dead weight as the source of the constant load.
The composite and the dead weight were held at the desired temperature for 20 minutes.
The dead weight was then placed on the specimen for a predetermined duration of time.
The dimensions of the specimen before and after the dead weight being placed on it were
measured to estimate the viscosity of the composite at different temperatures. Table 7.1
shows the results from these experiments. Find the temperature dependence of the viscosity
of this system.
Solution
The change in dimensions of the laminate can be related to its viscosity assuming that the
composite behaves as an isothermal incompressible Newtonian fluid. Thus,

Table 7.1: Viscosity of AS4/PEKK Composite at Various Temperatures
Sample Li Wi hi Temp Wf-™< Viscosity Average

Li hi
ID. (m) (m) (m) (°C) xlOO% xlOO% x 100% MPa.s Viscosity
MPa.s
A7 0.0508 0.0064 0.0014 350 0.96 32.39 15.06 12.21
A8 0.0573 0.0051 0.0017 0.42 15.19 10.61 48.77
A10 0.0510 0.0033 0.0015 0.15 54.16 22.84 44.92 50.46
All 0.0509 0.0035 0.0014 0.30 27.51 10.53 95.94
Bl 0.0482 0.0065 0.0014 360 0.84 14.52 6.36 38.18
B2 0.0487 0.0065 0.0014 0.81 17.05 13.93 13.62
B3 0.0489 0.0064 0.0013 1.53 23.48 9.75 20.36 21.32
B4 0.0490 0.0065 0.0014 1.32 42.13 13.79 13.14
Dl 0.0494 0.0064 0.0013 380 1.26 23.45 8.88 22.30
D2 0.0494 0.0065 0.0014 0.31 24.16 7.34 30.76
D3 0.0494 0.0065 0.0014 1.47 29.78 12.52 15.36 18.76
D4 0.0495 0.0065 0.0014 0.92 48.65 20.66 6.64
El 0.0495 0.0064 0.0013 390 2.80 47.90 22.43 5.30
E2 0.0495 0.0064 0.0013 2.62 41.79 20.12 6.32
E3 0.0495 0.0064 0.0013 2.23 41.29 19.66 6.90 7.25
E4 0.0488 0.0065 0.0014 1.67 39.51 15.81 10.50
(An average force of 266.72 N was applied for 60 seconds.)
5 Ft
(7.86)
8 LiW? tf -
Hence, at each temperature, one can find /j>.
It is clear that the average viscosity of the composite decreases with an increase in
temperature. The viscosity of AS4/PEKK can be approximated by the following functional
form (see Chapter 4 for details):
Pa.s (7.87)
where T is the temperature in K. By plotting viscosity values at 4 different temperatures, a
best-fit line was found. Note that viscosity is plotted on a log scale due to the exponential
nature of Equation 7.87. The values of A and B that best-fit the experimental data were
1.28E-4 and 16548.6. The best fit line and the experimental data are shown in Figure 7.26.
7.5.8 Model Solutions

In this section, sample solutions of the consolidation model described earlier will be pre-
sented. It is seen from Figure (7.23b) that the linear tow velocity with respect to the roller
along with the geometric parameters, hi, hf and the roller radius, Rr, determine the closing
speed h completely as a function of the instantaneous height.

100
Best fit
Experimental
to
Q.
10
620 625 630 635 640 645 650 655 660 665
Temperature (K)
Figure 7.26: Viscosity of AS4/PEKK composite as a function of temperature
From geometric considerations, the contact length Lc may be expressed as,
Lc = [Rl - (Rr -hi + hf)2]V2 (7.88)

The instantaneous height h may be expressed in terms of the position y as
r a on 1/2
h = Rr + hf-[R2r- (Lc - y) 2 ] (7.89)
Differentiating both sides with respect to time and equating dy/dt to the tow speed V", we
obtain
1/2
dh
l^, - _ - _____ I/
(7.90)
~ dt ~ (Rr-h
Equation (7.90) is used to express the imposed closing speed as a function of the instanta-
neous height in all the computations.
The first solution we will present is for the simplest case of an isothermal incompressible
fluid.
Isothermal Incompressible
Consider an isothermal incompressible Newtonian fluid with the following boundary condi-
tions. The friction factors at z = 0 and z — h are denoted by Kb and Kt in Equation 7.83.
The susbcripts b and t characterize the bottom and top, respectively. The pressure at x — w
is zero and the pressure gradient dP/dx = 0 at x = 0. Equation (7.65) can be used to solve
for the velocity profile.

dP_
(7.91)
dx
where K* and K£ are Kt and Kb nondimensionalized with (j,/h and z* is z nondimension-
alized with respect to h. Figure 7.27 shows the velocity profile for various values of K%
u.oo
0.5 Kb= 1000 -
0.45
,,,<..,---•••••'"""""'"
c 0.4
o
ts
2 0.35 .,-•''".--•'''"
X
0.3 /('•••''' K t =1000
(D
±=
^C 0.25 /.••• 0.1
/•••' 0.001
0.2
8 /••'
<D
->
0 15 // _.— -.,
0.1 " / ^^^ "~~~~^^\"""""---
0.05
n
/^^ ^X;
0.2 0.4 0.6 0.8
Non-dimensional height through the gap
Figure 7.27: The velocity profile changes from a symmetric parabolic to an asymmetric
parabolic shape as the top surface friction factor goes to zero with the bottom surface surface
friction factor maintained constant at a high value (which models the no-slip boundary
condition).
for a given value of K£. It can be seen that the velocity profile changes from a symmetric
parabolic profile for the case of no-slip at both walls to an asymmetric profile when no-slip
is imposed on one wall and perfect slip is allowed at the other wall. Equation (7.68) can
now be used to determine the pressure distribution in the domain.
-i
p— (7.92)
7?
Figure (7.28) shows the pressure distribution in the domain for various friction factors. The
pressure distribution is seen to be parabolic in nature independent of the type of velocity
boundary condition that is applied. However, the pressure drop from the mid-plane to the
outer edge is the lowest when a perfect slip condition is imposed on the top surface and
the highest when a no-slip condition is imposed on the top surface, given that the bottom
surface has a no-slip condition prescribed.
The change in width or the movement of the free surface may be tracked as a through-
thickness average based on the velocity in the x direction at the free surface.

2
k t =1000 —
1.8 t 10 ____.
0.1
1.6 0.001
1.4 Kb=1000
1.2
E 0.8
73
C
O
0.6
0.4
0.2
0
0.2 0.4 0.6 0.8
Non-dimensional width
Figure 7.28: The pressure profiles maintain a parabolic shape. The pressure drop from the
middle of the tow to the outer edge decreases with decreasing top surface friction factor.
dw 1
(7.93)
dt ~ h
Substituting for vx from Equation (7.91), it can be shown that,
dw h
—— = — w — (7.94)
dt h
In other words,
w h = constant (7.95)
This result is not surprising because we are dealing with an incompressible fluid and expect
the total volume to be conserved. This result is, in fact, a verification that we conserve
volume in this formulation.
Example 7.8: Compaction Force

Find the compaction force required to compress the tow as a function of the final hf shown
in Figure 7.23.
Solution
The force required for compaction, Fc, for this incompressible material may be obtained by
integrating the pressure distribution across the width and along the contact length.

Fc = P(x,y)dxdy (7.96)
Substituting for h and the pressure solution from Equations (7.90) and (7.92) respectively
and carrying out the integrations we obtain
(7.97)
wf
The compaction ratio hf/hi is governed by a single nondimensional parameter, Yin, given
by the right-hand side of Equation (7.97).
.. -—
n-M
1J _15 A *L
„ o
1 r (7.98)
+
2,
Therefore, Equation (7.97) may be rewritten as
-^"1/5 (7.99)
11^ varies between zero and oo depending on the parameters of the problem. For example,
for high compaction forces, low tow speeds or low material viscosity, the magnitude of H^ is
large and thus hf/hi is a small number. Figure 7.29 shows the variation of the compaction
ratio with the nondimensional parameter HJJ. •
DC
to
Q.
o
O
0.001 1 10 100 1000 10000
Figure 7.29: Variation of compaction ratio with II;,

Isothermal Compressible
In this section, we relax the assumption that the fluid is incompressible and solve the flow,
pressure, and density field in the domain of interest. Physically it implies that there are
small voids in the material that can be squeezed out.
The formulation follows along the same lines as the incompressible case, but the terms
with density gradients need to be retained in the solution. The governing equation for the
pressure in the fluid field is given by
dP
- - (7.100)
at 2 ) (I + K: + K?/K?} e
The velocity field is still given by Equation (7.91). Equation (7.100) needs to be solved
numerically due to the dependence of the density on both time and position, x.
The solution methodology is shown in Figure 7.30. The initial density in the domain is
Macroscopic Microscopic
Figure 7.30: Solution methodology,
assumed to be uniform. Equation (7.100) is solved with the pressure boundary conditions
- 0 (7.101)
' x=0
P(x = w(t)) = 0 (7.102)
using a central difference scheme for the spatial derivative of P. The velocity in the x
direction is calculated from Equation (7.91). Based on the average velocity of the material
in the x direction, the free surface and the other nodes are advanced to the new positions.
The microscopic void compression equation, Equation (7.74), is solved using a Runge-Kutta
algorithm at each node in the domain to obtain the updated void radii at all locations. The
densities at these locations are updated, and the Equation (7.100) is solved again. This
procedure is repeated at every time step during the solution.
The model solution is illustrated for the case of a no-slip condition at the bottom surface,
z = 0, and a perfect slip condition at the top surface, z = h, in order to limit the number
of results to be presented. The initial void fraction is maintained at 0.05 (5%), and a tow
speed of 0.05 m s"1 was used. The final void fraction distribution was calculated for the
compaction ratio, /i///i;, of 0.99 to 0.95. A constant viscosity of 105 Pa.s was used for
the medium. The initial pressure inside the voids was assumed to be atmospheric and the
initial void radius was assumed to be 10 /im. The final void fraction distribution for these
cases is shown in Figure 7.31. The final void fraction is seen to be highest at the outer
edge of the tow because the pressure is the lowest at that point. As the compaction ratio
decreases, i.e., the amount of compaction increases, the final void fraction decreases, which
is consistent with our intuition.

0.05
hx /h.. = 0.99
0.049 I
0.98
0.97
0.048 0.96
0.95
0.047
o
0.046
0.045
"§
CO 0.044
0.043
0.042
0.041
0.04
0.2 0.4 0.6 0.8 1 1.2 1.4
Non-dimensional position along the width
Figure 7.31: Final void fraction distribution in an isothermal compressible medium under-
going consolidation.
Nonisothermal Compressible
The most general case considers the continuum to be compressible and the domain to be
nonisothermal. The viscosity of a continuum is a function of the temperature and therefore
varies throughout the domain.
The values of ^(O) and C\(x] in Equation (7.65) may be evaluated from the velocity
boundary conditions and the equation may be rewritten as
dP
(7.103)
where FI (£) and F^ (£) are denned by
(7.104)
F 2 (0= f-dz. (7.105)

Jo fJ>
The pressure solution is given by Equation (7.68). The solution procedure is similar to
the previous case. However, the difference is that the temperature field needs to be known

in this case to evaluate the viscosity of the material at various points in the domain. One
could use Equation (7.87) for the temperature dependence of viscosity [284].
7.5.9 Inverse Problem of Force Control

The natural input to the problem being solved is the displacement rate given by h. How-
ever, in practice, tow placement machines are run under a specified force rather than a
displacement. Therefore, the results obtained using any of the above models except the
isothermal incompressible model need to be inverted, and the force required for a certain
compaction ratio is computed and expressed as the compaction ratio obtained for a given
roller force.
7.5.10 Extended Consolidation Model

All the models that have been discussed have had free surfaces on the tow edge for the
resin-fiber-void continuum to flow. This is appropriate for the topmost tow. However, tows
beneath the top layer that are still at elevated temperatures (> Tg) also feel the effect of
the compaction roller. These tows are constrained from the sides, and material cannot flow
out in the width direction. Therefore, an appropriate boundary condition for them would
be a no out-flow condition. This is depicted in Figure 7.32. The domain is divided into
-o 0 o o o o— Region 1
o o o o o o \
\
o o o o o o \
'v2 \ Region II
0 0 o o o o \
Figure 7.32: Extended consolidation model
regions I and II. Region I denotes the topmost tow that is being placed. The void fraction
in this tow reduces from the incoming value, <f>vi to an intermediate value, </)V2. Region II
denotes the layers beneath the topmost layer that are still at a temperature > Tg. The void
fraction in this region reduces from 4>V2 to the final void fraction ^3.
The pressure in region II is uniform and the continuity equation simplifies to
ph = constant. (7.106)
The combined solution of the change in height of regions I and II needs to be carried
out iteratively. The rates of change of the height of regions I and II are denoted by hi and
hn respectively. These are related to the total change in height, h by
h = hj + hn (7.107)
h is known from the geometric parameters and the tow speed. An initial guess is used for hj
and (j)v2 and the pressure distribution in region I is computed and averaged over the width
of the tow. This average pressure is used as the driving pressure for the void compaction
in region II. Based on the void compression model the change in density of region II and
the associated change in height may be computed. The sum of the changes in height is
compared to the known total change and the guess for hj modified appropriately. This

procedure is repeated until h is equal to the sum of hj and /i//. Figure 7.33 shows a typical
result for void fraction changes in regions I and II.
g
ra
'o
0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9

Dimensionless position along the tow direction
Figure 7.33: Variation in the void fraction in regions I and II as a function of the non-
dimensional tow position under the compaction roller for a tow speed of 0.005 m/s.
Summary
A model for consolidation and void reduction during thermoplastic composites processing
was discussed. This work is based on the assumption that the composite can be modeled as
a compressible continuum. Thus the problem is solved as the squeeze flow of a compressible
viscous fluid. After deriving a general formulation, three specific cases — isothermal in-
compressible, isothermal compressible and nonisothermal compressible — were solved. The
final one is the most applicable model for the fiber tow placement manufacturing process.
However, for an extended model of the consolidation process, the domain can be split into
two regions, the topmost tow and the other tows beneath it that are at a temperature
greater than Tg. Given the total thickness change in both regions, an iterative scheme can
be used to estimate the individual changes in thickness in the two regions. Simultaneously
the changes in their void fraction and the required compaction pressure to achieve the given
thickness change can be computed.
This analysis demonstrates how one can start with a simple model and refine the model
by relaxing the assumptions to move towards accurately describing the physics. Comparison
with experiments can usually help determine if these refinements are necessary. Revisions
and refinements are usually more time consuming in terms of model development and solu-
tion.

7.6 Exercises
7.6.1 Questions
1. Name at least three advanced thermoplastics composites manufacturing processes.
2. What are the microscopic phenomena that influence the constitutive equations at the
macrolevel?
3. What are collimated fibers?
4. Why do the reinforcing fibers buckle and distort more when a thermoplastic resin
impregnates than a thermoset resin?
5. What are the four key factors that cause internal stresses and hence can lead to
microcracking in the composite part?
6. Describe the sheet forming process by using all of the following terms: deform, stretch,
inextensibility, curvilinear shape, thermoplastic polymer, stacked fabrics, and pre-
impregnated laminate.
7. What is the advantage of using long discontinuous fiber (LDF) material in the sheet
forming process?
8. Name the four main composite sheet forming processes.
9. What are consolidation, interply slip, intraply slip and interply rotation?
10. What are the differences in the deformation mechanism of consolidation of fabric
sheets between (i) single curved and (ii) double curved parts?
11. How can one calculate the force required to pull a ply out from a stack of plies that
will be consolidated?
12. In the pultrusion process, (i) what types of reinforcing material are guided through a
preheater where their temperature is raised to the melting temperature of the poly-
mer? (ii) After the heater zone, which assembly do the heated polymer and fibers
enter? What are the functions of this zone? (iii) What is the last zone?
13. Why is the cooling speed important in the pultrusion process?
14. What is a typical pulling speed range in the pultrusion process?
15. What are the two important issues to model in pultrusion?
16. What are the similarities and differences in the thermoset pultrusion and thermoplas-
tic pultrusion processes?
17. Describe viscous dissipation in the pultrusion process.
18. What do the Peclet (Pe) and Brinkman (Br) numbers represent in the pultrusion
process physically?
19. What are the key process parameters that influence the extent of consolidation?

20. What is the in-situ or on-line consolidation process? How does it differ from the
regular consolidation process?
21. Give some examples of different types of heaters that are commonly used in the on-line
consolidation process.
22. In the tow placement process, what properties of the composite part are used to
estimate part quality?
23. How does a process model help engineers in the tow placement process?
24. How does void coalescing occur?
25. Why should there be a concern about the execution time of the numerical solution of
a model for the tow placement process with on-line control?

1. Reinforced material can have different levels of crystallinity. The rate at which the
material is to below the temperature, governs the crystallization
in the matrix. Presence of fibers also provides sites and can cause sec-
ondary crystallization. rates can influence the material solidification only
for composites in which the outer layers will be and the inner
core is crystalline but a short cycle crystallizes the surface layer.
2. Usually as the composite is cooled, the resin tries to which is resisted by
the stiff inextensible This places the fibers in and the resin in
3. The composite is cooled from the outside to the center. This would shrink and so-
lidify the first, and then the is constrained during its solidifica-
tion. This puts the outside under and the interior under Hence
controlled cooling is an important process parameter during manufacturing of such
materials.
4. In the diaphragm forming process, a laminate of the composite material is sandwiched
and heated between two sheets of and a is used to form the
composite. The edges of the material are not as the inextensibility of the
material can cause fiber
5. In the matched die forming process, the composite laminate or sheet is held and
between two metal tools surfaces as is accomplished in sheet metal forming.
The process takes very time. Most match die forming has been practiced
on shapes due to nonuniform and distributions.
6. The stretch forming process can be used only with materials that can
stretch. fiber thermoplastics cannot do this but materials can.
7. The roll forming process uses a series of rotating to deform a composite
into a shape.
8. When forming single curvature parts, individual plies over one another in
the laminate. The stretching mode along the fibers is unavailable due to the
of the fibers.

9. Pultrusion is a continuous composites manufacturing process. The goal in pultrusion
is to produce a cured and profile with a constant by pulling
reinforced material through a forming die.
10. Compared to thermoplastic pultrusion, thermoset pultrusion involves an additional

station of a between and
11. In thermoset pultrusion, one uses law to model resin impregnation, whereas
in thermoplastic pultrusion, due to the high of the material, this law is not
the correct model.
12. The heat transfer model in thermoset pultrusion involves On the other
hand, the heat transfer model in thermoplastic pultrusion focuses on
13. In pultrusion, if one assumes that most of the flow is parallel to the , one
can divide the section of the die into self similar cells. A cell model is
formulated by considering a single tapered annulus of liquid surrounding
each This assumption allows one to simplify the problem to
problem in the direction of the fiber movement. Also, due to the cylindrical nature
of the fiber, one can assume that the annulus of the resin is also ; thus one
can choose the coordinate system to pose the problem.
14. In pultrusion, the mechanism of the fibers in the axial direction induces
a flow in that direction. However due to the geometry, the
material experiences a pressure build-up. This makes the resin pressure higher near
the of the die as compared to the Hence, a pressure gradient is
established in the direction to drag flow, which may give rise to
flow.
15. In pultrusion, at any cross section along the axial direction of a tapered die, the flow
rate Q is the sum of flow induced by the fiber , and
generated due to the opposing
16. In the tapered die of the pultrusion process, one would expect heat generation by
17. The viscosity of polypropylene (a thermoplastic resin) reduces by about %

as the temperature increases from 190°C to 240°C. Such a variation has significant
influence on the pressure profile in the pultrusion process. Ideally, one may have to
solve the equation of and equation simultaneously due to the
two-way between them. That is, the influences the
through viscous term in the energy equation, and the influences
the in the equation of motion.
18. There are five main components in on-line consolidation process. They are the
, , , , and a for
the placement of the fiber tows to form the composite.
19. The is used to mechanically maintain constant tension within the fiber tow
from the moment it leaves the until it is wound on the tool or the previously
placed fiber tows on the tool.

20. The tool, which is known as in filament winding and
in the tow placement manufacturing method respectively, is the surface on which the
fiber tows are placed and to create the geometric form of the composite
structure. In the case of filament winding, it is in form, whereas in tow
placement method it can take various complex forms based on the geometry of the
part to be manufactured.
21. The stainless steel allows for application of consolidation
to fuse and compact the incoming with the previously placed
22. The heater used in the preheating chamber must be easily controllable while supplying
sufficient energy to raise the temperature to the desired level. The heater
power will be a function of the tow , the material properties of the ,
and the change one wants the tow to undergo.
23. In the consolidation process, the interactions between mass, momentum and en-
ergy transfer can be investigated by classifying them on , and
levels. The level analysis will allow us to establish the process
windows of , , and required in order to achieve com-
plete consolidation. At the level, one can investigate the effect of temper-
ature and pressure on the size of individual and thus on the macroscopic
At the level, one is concerned about intimate between
two adjacent and of polymer chains across the ply interfaces.
24. In the consolidation process model, , and any present
in the tow are approximated as a homogeneous fluid with specified rheological prop-
erties. The rheological properties of this continuum depend on the , the
, and the content.
25. In the thermoplastic consolidation process model, due to the matrix resin
viscosity, the flow may be treated as motion. In other words, the
effects are neglected.
26. In the consolidation process, voids may migrate, along with resin, due to a pressure
On the other hand, void migration relative to the resin is usually
because of high of the thermoplastic resin.
27. In the consolidation process, cooling of the tow leads to of the void size.
Void compression takes place due to the applied pressure. The effects of
heat input and void compression are taken into account using a model. The
effect of void transport is taken into account in the flow model.
28. In the microscopic void model of the consolidation process, a typical void is approx-
imated by a surrounded by a concentric resin shell. The ratio
of of these two is determined by the fraction at that
location.
29. Void growth or collapse is governed by a balance between the inside and
outside the void, the , and the resin
30. A mathematical model for consolidation and void reduction during thermoplastic
composites processing can be developed based on the assumption that the composite
can be modeled as a Thus, the problem is solved as the
flow of a and fluid.

7.6.3 Problems
1. Derive Equation (7.86).
2. If you are interested in obtaining a composite laminate of thickness 2 mm and you start
with an initial thickness of 3 mm containing no voids, what will be the compaction
force you will need for AS4/PEKK material at a temperature of 350°C? The initial
width of the tow is 2 cm. Assume no-slip boundary condition and velocity of 1 cm/s.
3. Write a finite difference program to solve for compressible isothermal consolidation
case as explained in the isothermal compressible section.

Chapter 8
Processing Advanced Thermoset

Fiber Composites
8.1 Introduction
Thermoset resins are very conducive to processing, as their viscosity is reasonably low to
allow easy impregnation of the empty spaces between the fiber preforms. The earliest
composites manufacturing concentrated on processes such as wet hand layup, which is an
open mold process. This process employed a one-sided male or female mold, in which a
layer of resin called the gel coat is applied on the mold surface. The gel coat is usually
about 0.5 mm in thickness, has good environmental resistance and produces a smooth and
pigmented surface that covers the fiber preform. To manufacture a composite, a measured
amount of the thermoset resin is poured over the gel-coated surface. The fiber preform is
placed on top of the liquid resin and pressed by a hand held roller. The resin percolates
through the fibrous network due to the application of the pressure as shown in Figure 8.1.
Laminate
Dry reinforcement \ Gel coat
Figure 8.1: Schematic of the wet hand layup process.
After one layer of the fiber preform is satisfactorily impregnated and compacted, another
layer is placed on top and the procedure is repeated until the desired lamination of the
composite is complete. Although this process was one of the first techniques to be used in
manufacturing composites, it is still widely used by the boat manufacturing industry due
to its versatility and low capital investment. However, as the resin that is widely used in
this open molding process contains styrene (which is emitted to the environment), there is
a push to replace it with closed mold processes due to environmental concerns.
All the processes we will discuss in this chapter evolved from this process in which the

goal was either to automate the process to reduce labor costs, to improve surface treatment,
eliminate or reduce emissions of styrene to the environment, improve dimensional tolerances
and/or increase the fiber volume content in the composite. The three processes we will
scientifically analyze in this chapter are the autoclave molding process, liquid composites
molding and filament winding.
8.2 Autoclave Molding

Autoclave processing is one of the oldest composites processing technologies. In this process,
plies or prepregs or tapes (fibers that are preimpregnated with the resin) are stacked on the
surface of the tool. They are then subjected to high pressure and temperature to allow the
stacks to become a single coherent structure by forcing out air pockets and excess resin.
The process is carried out in an autoclave, which is a large pressure vessel with an integral-
heating element. One can think of an autoclave as an oven that can be pressurized. Not
unlike a pressure vessel, it is usually constructed as a cylindrical tube with a door at one
end. Its main function is to provide the heat and pressure necessary to consolidate and cure
composite structures. A schematic is shown in Figure 8.2.
Autoclave Insulated Shell Heating Elements

Door
[ Recirculating Air
VoJifc,. (Forced Convection)
D
in i n t
.'
i i
."
I
."
I /
/
/ '
i\ ; . •, . , •: „ o, _j
/ i
v i \ / y
\ /
Bagged Composite Parts
Figure 8.2: Schematic of an autoclave (redrawn from [51]).
Autoclave processing is carried out under high pressure and temperature. The tempera-
ture and pressure requirements are set by the material systems used. For example, for high
temperature thermoset resins such as polyamides and PMR-15, the temperatures required
could be in the range of 300-400° C and pressure requirements may exceed 1 MPa. For such
cases, one may need special autoclaves. Thermoplastic composites can also be processed
in these autoclaves as most advanced thermoplastic resins such as PEKK and PEI melt at
high temperatures and require higher pressures for consolidation.
Autoclave consolidation has been the champion of the aerospace industry for years.
For aerospace applications, the parts can be very large, such as the case would be with
an airplane wing; consequently, the autoclaves need to be even larger. The autoclave
dimensions for some aerospace applications can be as large as 30 meters in diameter, and
over 50 meters in length. This is equivalent to a multi-floor building. The largest existing
autoclave in the U.S. is at the Boeing commercial aircraft plant in Seattle, WA — large
enough to fit an entire length of a commercial airplane wing. The autoclaves are usually
made of welded steel as they are subjected to high pressures and temperatures. Hence they
are expensive pieces of equipment [51]. This is the main reason for reluctance to use this
process in other industries besides aerospace, such as automotive and sporting.

However, in other industries where parts are small and not complex, the autoclave
process can be cost effective. High volume production can be achieved by reducing cycle
time by choosing materials that cure faster. Multiple parts could be cured simultaneously.
One can address small curvatures and minor geometric complexities by placing the wet
composite on a tool surface. As the resin heats up, the plies become less stiff and will
adhere to the shape of the tool lying beneath it.
The advantages of the use of autoclaves include the ability to process a wide variety
of materials and be able to obtain a very high fiber volume fraction in the composite due
to its ability to apply high pressures. Hence, the autoclave has traditionally been used to
process composite structures for the aerospace industry. The main disadvantages of the use
of the autoclave are the high initial capital investment and the inability to use the pressure
and temperature control effectively to produce void free composite structures. In addition,
one cannot make complicated near net shaped structures as the mold is usually one sided.
Also most of the cure cycles developed for aerospace structures are slow and can take hours
before one can remove the part from the autoclave rendering it unsuitable for high volume
production.
8.2.1 Part Preparation

The autoclave has been successfully used for many years to make composite parts which
have no or negligible geometric complexity. Hence, the tool is usually a flat plate with
very few curvatures and inserts. The tool material may be aluminum, steel, nickel, invar
or even a composite depending on the application and the cost. A release film or a coating
of release gel is usually applied on the tool surface for easy removal. The composite layup,
consisting of prepregs or tapes, is placed on the tool surface sandwiched between release
plies or fabrics. Cork or solid spacer plates are placed around the perimeter of the stacked
plies, and they act as dams and limit resin flow in the lateral direction. The release film and
release fabric are necessary for easy separation of the composite part from the tool surface
and the vacuum bag. Bleeders are used to absorb excess resin in the thickness direction.
The release fabric, in addition to assisting in releasing the composite from the tool, allows
resin to flow into the bleeders. Peel plies provide surface texture and protect the part
surface during handling. The breather material allows for uniform distribution of vacuum
over the surface of the part. An inner vacuum bag is placed on top to seal the assembly
along the tool surface and the perimeter dams. A caul plate covers the whole assembly. The
role of the caul plate is to improve the surface finish of the part and improve dimensional
tolerance by applying uniform pressure and minimizing ply movement. The caul plate may
be semi-rigid and is made of thin metal, composite or rubber material or may be rigid
for critical dimensional tolerance. The vacuum bag and breather material creates vacuum
pressure inside the assembly. The driving force for consolidation is the difference between
the autoclave pressure on the outside and the vacuum pressure inside the vacuum bag. A
typical stacking order of layers is shown in Figure 8.3.
8.2.2 Material and Process Parameters

The goal of consolidation is to force air pockets (or voids) and excess resin out of the
structure. By squeezing these flaws out of the composite part, a single coherent structure
can be made by inducing intimate contact between the individual plies. The final structure
will be thinner than the original material placed into the autoclave, but the fiber volume
fraction, Vf, will increase making it a stronger part. Moreover, due to consolidation, the
interlaminar shear strength will also increase.

Vacuum Bag
Caul Plate
Breather Material
Release Film, Perforated
Bleeder Material
Release Fabric
Peel Plies
Composite Lay-Up
Release Fabric
Release Film
/ Tool
Vacuum Bag Dam Vacuum Bag
Sealant Tape
Figure 8.3: Schematic of stacking order in autoclave processing (redrawn from [297].
Typically, thermosets have been used in autoclave processing. For most thermoset
resins, the heat of the autoclave is actually necessary to initiate the cure reaction. The
typical temperature range for autoclave processing of thermosets is around 100-200°C, with
pressures in the 600-700 kPa range. Thermoplastics can also be used, but as is typical with
thermoplastics, the temperature and pressure requirements are much higher than those for
thermosets. For example, thermoplastic matrix materials such as PEI or PEKK require
processing temperatures in the 300-400° C range with pressures of the order of 1 MPa.
The typical inputs to the autoclave process are the raw material quality, attributes of
part preparation and handling, and most importantly from the process modeling viewpoint,
the pressure and temperature cycle imposed on the autoclave for composite manufacturing.
The quality of the part manufactured is measured in terms of final thickness or dimensions,
degree of cure or cross-linking (for thermosets) and void or porosity content. The prepregs
used in the composite layup can be either impregnated (either partially or fully) tapes with
smooth surfaces, or fully impregnated tapes with rough surfaces. It was found that fully
impregnated tapes with smooth surfaces do not provide a path for the volatiles and air to
escape from the part and can lead to a lower quality part. The material preparation can
influence the part quality if the procedure of layup is not executed in a repeatable fashion.
However, as a process modeler, the most effective way to influence the part quality is by
controlling the pressure and the temperature cycle during the curing and consolidation of
the composite part.
An example of a pressure and cure cycle is shown in Figure 8.4. There are typically
three stages of autoclave processing. Stage I is the heating stage. At the same time, the
pressure is ramped up inside the autoclave during this stage. The first pressure ramp
and hold in stage I is for the viscosity to go down and for excess resin to flow vertically
into the bleeder material. The second ramp and hold is for polymerization of the resin to
initiate during which time the viscosity rises dramatically. Stage I ends when the selected
processing pressure and temperature are reached. Stage II is essentially a "hold" stage. The
autoclave is maintained at the processing pressure and temperature to allow consolidation
and curing to occur during this stage. As the cure reaction proceeds and generates heat
due to polymerization, in stage III, the temperature is lowered to allow the excess heat
from the reaction to diffuse through the part but the pressure is maintained to prevent
voids from growing. When the cure reaction is complete and the temperature of the part is
lowered, the pressure is released and the part is removed from the autoclave. The vacuum is
discontinued to allow for out-gassing of volatiles. Although the autoclave pressure is high,

Temperature *
and
Pressure
_ _"[emp_erature
r~_ *\ Pressure
1 bar I , Stage I Stage I Stage ill

Room temperature \
Time
Figure 8.4: Typical autoclave temperature and pressure cycles during the three stages of
autoclave processing.
most of that pressure is borne by the fiber network.

Figure 8.5 schematically shows how the autoclave pressure redistributes between the
fibers and the resin during the consolidation phase. Thus, at the end of consolidation,
the resin pressure is low, the temperature is high and the volatile vapor pressure is high
creating ideal conditions for void formation and growth. As resin pressure Pr tends to zero,
no further resin will bleed but it will be easy for volatiles to vaporize and form voids. Hence,
it is important to maintain some pressure in the resin to arrest formation and growth of
voids.
Example 8.1: Void Growth

Show that as the pressure in the resin reduces, the void growth rate of the nucleated voids
increases.
Solution
Consider the sketch shown in Figure 8.6 of a nucleated void of radius R. To relate, dR/dt,
the rate of growth of this void, to the resin pressure, one can balance the stress at the
interface between the resin outside the void and the air inside the void. One can write the
following equation that equates the normal stress on either side of the interface location
= R:
2a
— i-oaid = ~Pr (8.1)
~R
-=R
where Pvoid is the void pressure, Pr is the resin pressure, R is the radius of the void, a is
the surface tension of the resin, and rrr is the normal stress experienced by the resin. For a
Newtonian fluid, low Reynolds flow and considering spherical symmetry, the normal stress

B, = 100 psi Resin bleeds
Resin bleeds
uum i B, = 100 psi
muu = 100 psi
UIUU
Fiber, f
Resin, r-
P = 100 psi P = 50 psi P = 0 psi
F' = 0 psi P = 50 psi P = 100 psi
(a) (b) (C)
Figure 8.5: Redistribution of resin and fiber pressure as the network is compressed [61]. In
(a), the fiber network is carrying no load. In (b), as the network is compressed partially,
more and more load is being taken by the fibers, and in (c), all load is taken by the fibers.
Figure 8.6: Schematic of force balance during void growth in autoclave processing.

is equal to ~4fj,R/R where R = dR/dt. Equation (8.1) can be rewritten as
(8.2)
.n, -it
Prom Equation (8.2), one can easily conclude that, as Pr decreases, R increases. Hence,
it is important to have (Pvo;d ~~ -Pr) < 2a/R in order to suppress the void growth. •
Thus as resin pressure goes down, the rate of bubble growth could potentially increase.
It is crucial to understand and predict the resin pressure inside the part during consolidation
as it plays a dominant role in formation and suppression of voids. If resin pressure drops
to zero, voids will form freely inside the composite since there is no back pressure to resist
the void growth. Intuitively, one may want to increase the autoclave pressure to prevent
this. However, as seen from Figure 8.4 applying too much pressure can cause consolidation
to occur too quickly (in which case the pressure will be all borne by the fiber network), or
cause regions to lose too much resin. If this happens too quickly, then resin pressure will
be lost before the part has had a chance to fully cure initiating void growth. Also complete
wet-out of the fibers may not occur which is detrimental to its mechanical properties. Hence
it is important to control the resin pressure to allow slow enough consolidation to allow total
wet-out, while maintaining sufficient resin pressure until the part solidifies.
There are many combinations of pressure and temperature one could apply with time
to change the cycle shown in Figure 8.4 to produce the part. However one is limited by
how fast one can change the pressure and temperature in the autoclave. At a given power,
to find the time it takes to increase the temperature by 1°C, one would have to consider
the mass and heat capacity of the autoclave. In general the MCp term for the autoclave
and the tooling can be much larger than that of the part where M and Cp are the mass
and specific heat, respectively. Hence, large autoclaves are not well suited for rapid rates
in heating or cooling of the autoclave due to their large thermal inertia.
Example 8.2: Heating Rate in Autoclave Made of Welded Steel

Consider an autoclave that is made of welded steel of thickness 25 mm. The autoclave is a
cylindrical tube of diameter 2 meters and length of 5 meters. The tooling and part thermal
inertia can be considered negligible as compared to the autoclave inertia. The heater power
supplied to the autoclave can vary from 10 to 50 kW. If one wants to heat the autoclave by
1°C, how long will it approximately take to do so at the power supply of 10 kW through
50 kW? Plot the effect of heater power on the time to heat the autoclave by 1°C. Also plot
the heating rate as a function of the input power.
Solution
The schematic of the autoclave is shown in Figure 8.7. One can write the heat transfer
to the autoclave as Q = QAt = MCpAT. Here Q is the heater power, At is the time
to increase the temperature of the autoclave by AT = 1°C, Cp is the specific heat of the
autoclave material, and M is the mass of the autoclave which can be calculated as
M = Mtube + 2Mendplate
= P (Kube + 2T4ndplate)

•I-OC21T
_ Jt_——~~~
— — ~ ~ ~ ~ ~ " ""*"
i'
f<V ~-~ ~~
'/ - - - ~ "".I I—"—"'"""
Figure 8.7: Dimensions of the autoclave for Example 8.2.
= 7, 800 [vr(2)(5)(0.025) + 27r(l) 2 (0.025)]

= 7,351kg. (8.c
Taking Cp = 460 J/(kg °C) for steel, one can find the time to heat the autoclave by 1°C
At =
3 4 106
= - *: j
seconds .0 ^
(8.4)
Q
where Q is in Watts. Note that one Joule is equal to 1 Watt second. Figure 8.8 shows how
long it takes to heat the autoclave of these dimensions by 1°C at various power inputs. For
example, it takes 5 minutes and 40 seconds if the heater has a power of 10 kW, and only
1 minute and 8 seconds if the input power is 50 kW. The rate at which one can increase
the autoclave temperature is plotted as a function of the power input in Figure 8.9. This is
obtained by rewriting Equation 8.4 such that ^ is on the left-hand side:
^ °C/seconds (8.5)
At Mcp 3.4* 106
Thus, the heating rate is directly proportional to power input. •
For industrial autoclaves, which are generally heated by natural gas burners, it is not
uncommon to have heating rates of about 2 to 3°C per minute.
The most widely used method of pressurizing the autoclave is to use nitrogen gas. Air is
unsuitable at high temperatures due to the risk of auto-ignition. However as the approach to
increase the pressure is to use a compressible medium and as the volume to be compressed is
large, one can only expect sluggish rates of increase in pressure. However, there is sufficient
flexibility in application of the pressure to the part. Usually the parts are placed on one side
of the tool and wrapped in a plastic bagging material. Pressure is then applied to the part,

500
10000 20000 30000 40000 50000
Heater Power [Watts]
Figure 8.8: Time to heat the autoclave by 1°C at various power inputs.
10000 20000 30000 40000 50000

Heater Power [Watts]
Figure 8.9: Heating rate (temperature rise) AT/At at various power inputs.

which presses it against the tool. Pulling a vacuum in the bag can intensify the pressure on
the part. This way one can locally control the pressure more effectively.
The most important process parameters that influence the part quality manufactured by
autoclave processing are pressure, temperature and time. The goal in autoclave processing
has been to employ the science base of composite processing to develop the "most optimal
pressure and temperature cycle" to manufacture void free composite parts. In this section
we will delineate the approach to model issues pertinent to autoclave processing using the
scientific base. This is a necessary step before one can develop the optimal pressure and
temperature cycle.
8.2.3 Processing Steps

There are three important steps involved in manufacturing of a composite part by autoclave
processing. They are (i) material preparation, (ii) resin flow, consolidation and cure, and
(iii) inspection and post-cure.
In the material preparation step, the precursor materials, which are usually in the form
of plies of fabric or unidirectional prepregs, are cut and stacked to occupy the tool. Lay
up may be accomplished either manually or by an automated procedure such as automated
tow placement or automated drape forming. The composite lay up is placed on the tool
surface along with the bagging and other ancillary materials. The arrangement of the tool,
composite and ancillary material may vary slightly, but the general lay up configuration is
Vacuum bag / Breather
Barrier
Sealing tape
Separator/release film
- Prepreg stack
Release agent/film
Dam Mold
Figure 8.10: Typical vacuum bagging assembly.
The next step involves heat, resin flow, consolidation and cross-linking of the composite
layup. In this step, the process parameters of pressure, temperature and time play an
important role in the quality of the part that will be made, as this process is irreversible for
thermosets. Insufficient pressurization can result in excess resin in the part. On the other
hand, high pressures can lead to resin starved regions. The spatial curing distribution and
the degree of cure is determined by the temperature cycle with time. Usually the focus is to
understand the flow and heat transfer dynamics in this step to effectively model this step of
autoclave processing. The final step of post processing usually will initiate with inspection
and based on the findings may require either rework including further heat treatment to
increase the degree of cure, trimming, machining or assembly.

In this process there is ample room for error due to the number of manual procedures
involved which then lead to flaws in the part and a very high rejection rate. Some of the
errors involved in the material preparation step are [51]

• Failure to clean tool surface or apply release film which will cause imperfections on the
composite surface or will make it difficult to separate the part from the tool surface.
• Failure to completely debulk (remove large air pockets in between the plies by adhering
the layers to each other) the composite layup which can lead to void formation.
• Incorrect ply orientation or inaccurate placement which can lead to reduction in me-
chanical properties.
• Failure to place ancillary material correctly such as bleeder or breather material which
can lead to resin build up and low fiber volume fraction in the part.
• Inproper sealing of the vacuum bag which can lead to loss of vacuum during cure and
can result in void formation.
During the consolidation and curing step, an incorrect pressure and temperature.profile
can cause uneven cure, warpage, low fiber volume fraction, voids, resin degradation and
insufficient consolidation.
The important issues for composites made by autoclave processing that are influenced
by the cure and consolidation step are the thickness variation, void formation and growth
and warpage. The thickness variation is linked to the degree of consolidation of the plies
during the process. The void formation and growth can be related to the moisture absorbed
by the prepregs during manufacturing and storage. The warpage issue is linked to the
residual stresses developed in the part and the differences in the coefficient of thermal
expansion of the composite both along the fibers and in the transverse direction. The
residual stresses are mainly caused by temperature gradients across the thickness of the
part, which are influenced by the temperature control during processing. Process models
can help the manufacturing engineer understand the influence of pressure and temperature
on the quality of the composite manufactured. In the table below, critical issues involved
in autoclave processing, and the reasons for modeling them are summarized.
Table 8.1: Critical Issues in Autoclave Processing and Benefits of Modeling

Issue Possible Benefit of Modeling
Resin Pressure Minimize void growth
Resin Flow Ensure completely wetted fibers and lamination of plies
Fiber Deformation/ Consolidation Consolidation of fiber network to maximize fiber volume fraction
Temperature Avoid resin degradation and reduce temperature gradients
Cure Kinetics Improve cycle time and reduce residual stresses
8.2.5 Flow Model for Autoclave Processing

The resin flow and resin pressure predictive model can be very complex as there is mass,
momentum and energy transfer taking place simultaneously during the process. Below we
will list assumptions that will simplify the model while retaining the important physics.
Assumptions
• The fibers in the composite can be considered as nonlinear elastic porous media.
• The composite consists of incompressible resin and fibers (pr and pf are constant).

• The composite is void free; that is, the volume of the resin and the volume of the
fibers is equal to the volume of the composite (i.e. Vr + Vf = 1).
• The applied pressure is distributed between the resin and the fiber network.
• Darcy's Law can describe the resin flow into the fibers.
• Fibers act as a bending beam between multiple contact points and the load borne by
the fibers depends on the fiber volume fraction.
• The permeability of the porous medium changes with the fiber volume fraction, Vf.
• The fiber volume fraction changes with only the transverse z direction, i.e. Vf = Vf(z).
• The resin viscosity changes with temperature and cure but is expressed as a function
of /j, — n(t) only.
The composite domain is usually compressed in the z direction only. Hence, the fiber
volume will change in that direction and so will the thickness as the part consolidates.
Gutowski [298] as shown in Figure 8.11 introduced a new variable, £ = w + z, where w
is the local displacement to account for the local deformation of the fiber network and
thus convert a moving boundary problem to a fixed domain problem. Figure 8.11 shows the
local deformation coordinate system. For a mo_re detailed discussion of the local deformation
network, please see Chapter 4 and Appendix 4A of [298].
dx
Figure 8.11: Schematic showing the geometry and the deforming coordinate system of a
control volume.
Flow and Consolidation Model

First, we should ensure fiber and resin continuity. The fiber continuity allows one to relate
the new coordinate to the z direction as follows:
(8.6)
Vf dz
Here V0 is the initial fiber volume fraction and Vf is the fiber volume fraction during the
consolidation stage. One can now use the control volume shown in Figure 8.11 and establish

continuity of mass for the resin in the porous medium using the mass balance principle
introduced in Chapter 3. This will result in
Replacing d^/dz with V0/Vf from Equation (8.6) results in
V
v\
V}] °] n
- V}\ = °
Using Darcy's law instead of the momentum equations, one can introduce the velocity and
pressure gradient relationship through the permeability of the preform in the x, y, and z
direction
^x — ,-, i '-'y — o i ^2 — ,-,
H ox p, ay n oz
where Kxx, Kyy, Kzz are the permeabilities in the x, y, and z directions. It is assumed
that x, y, and z are the principal axes of the permeability tensor. Substitution of velocities
in terms of pressure gradients in the continuity equation and assuming that Vf does not
change with x or y direction results in
KXX d*pr + Km d*pr , i d („ „ dPr\ d - -

ir o 19 ~i rT 1
o~9~ TF> "n~ ^z~^.— — TTT
Vf dx Vf dy V* dz V 9z J dt \—77
Vf
Pr refers to the resin pressure and JJL is the viscosity of the resin. From the force balance, one
can relate the resin pressure and the fiber stress to the applied pressure, which is usually
the autoclave pressure PT, as follows:
PT = Pr + azz. (8.11)
Gutowski [299] developed a constitutive equation to describe the relationship between
the stress taken on by the fibers as a function of fiber volume fraction. They used a
conceptual model called the Fiber in a Box model (see Equation (4.116) and the related
text in Chapter 4 for detail). The relationship is very nonlinear and can be expressed as
3.12)
In this relationship, A3 is a material or "spring" constant that will be a function of the

elastic properties of the fibers and the fiber diameter. Va is the maximum attainable fiber
volume fraction, and V0 is the initial fiber volume fraction at which the stress taken on by
the fibers is zero.
We also know that as the fiber bed compresses under the applied autoclave pressure,
the transverse permeability, Kzz, will also reduce as the fiber volume increases and the
pore space between the fiber network reduces. Hence, one would need another constitutive
equation to describe the relationship between the fiber volume fraction and the transverse

permeability. Many such expressions have been developed. The best known and developed
for isotropic porous media is known as the Kozeny-Carman equation [23] (Equation (8.13)).
Other expressions that more specifically focus on fibrous porous media are the Gebart
transverse permeability expression [215] (Equation (8.14)), the Bruschke-Advani model [216]
(Equation (8.15)), and the modified Kozeny-Carman relation (Equation (8.16)). In these
expressions, Vf is the fiber volume fraction, and Va is the maximum attainable fiber volume
fraction. One only needs to know how the transverse permeability in the z direction for
these models changes with the fiber volume fraction. As we assume that the fiber volume
fraction does not change in the plane of the composite, we do not expect the permeability
to change in that direction. All the permeability relations are given below.
7-2 i _ v3
(8.14)
Kzs l ( l - L ) 2 / 3 L t a n - g T . £2 . , , _2 4V
- -- —f (8.15)
Notice that all of these equations require an empirical constant such as pzz or kc except
for the Bruschke-Advani model, which is based on flow across solid cylinders for a certain
packing geometry and fiber volume fraction, r or r/ in these equations refers to the radius
of the fiber.
Substitution of any of the permeability relationship with the fiber volume fraction in
Equation (8.10) results in a partial differential equation for resin pressure in which Vf is
also unknown. However, using Equations (8.10), (8.11) and (8.12) one can solve for Vf
and Pr if the applied autoclave pressure is known. Another important quantity is the final
fiber volume fraction after the compaction since this will give an idea of the mechanical
properties of the panel, as well as the final consolidated thickness. These are related via
nAw
hh = —— fsi7\
(8.17)
where h is the consolidated thickness in [m] in SI units, AW is the weight of the fabric per
unit area in [N/m2], n is the number of layers, and p is the weight density of the fibers in
[N/m3].
Usually in autoclave processing, one strives to eliminate the flow in the in plane direction
(x and y direction) and focuses on bleeding the excess resin through the z direction into the
bleeder cloth. Thus one can easily show by dimensional analysis that if h <C a and 6, one
would expect the pressure gradient and the resin flow to be primarily in the z direction.
This allows one to reduce the Equation (8.10) to
V0 dV

Example 8.3: Find Vf as a Function of Time
Delineate the approach to obtain Vf as a function of time for a composite subjected to a
constant autoclave pressure.
Solution
To solve Equation (8.18) to obtain Vf as a function of time, first assume \i, to be constant
and also the autoclave pressure, PT to be constant. The approach is to define a new variable
e as follows:
I — Vf resin volume fraction
Vf fiber volume fraction '
Hence, Vf = 1/(1 + e) and dVf = —de/(l + e) 2 , and Equation (8.18) can be rewritten in
terms of e as follows:
and simplification results in
1 6 f Kzz dPr\ de (821)

dz \j,l + e dz ) dt
Now as PT = Pr + &zz, and PT = constant, differentiation results in 0 = dPr + dazz, or

rearranging, we have dPr = —dazz. Then, one can write Qjg- = —^r ff, and Equation
(8.21) can be rewritten as
d ( K*. dazz de\ de

dz \ l +e de dzj dt
where V0 =
One can solve the above equation for e, along with the equations for permeability and
fiber stress constitutive equations. The initial condition is that the fiber volume fraction is
V0 at t = 0 and two boundary conditions are necessary along the z direction. At z = h,
the boundary condition would be that as Pr = 0; therefore, azz will be equal to PT. Hence,
one can find the fiber volume fraction using Equation (8.12) at z=h, which will allow one
to calculate e at z = h. The second boundary condition is at the tool surface, that is at
z = 0, there is no flow of the resin out of the tool surface. Mathematically, this can be
expressed as dPr/dz = 0 at z — 0. One can take the derivative of Equation (8.11) at z — 0,
which gives dP^/dz = dPr/dz + do~zz/dz. This implies that dazz/dz = 0 at z = 0 as the
other two terms are zero as well. dazz/dz will be zero only if dVf/dz = 0 at z = 0. One
can express gradient of Vf in terms of de/dz. A typical solution of how the resin pressure
and the fiber volume fraction change with time due to known applied pressure gradient
are shown in Figures 8.12 and 8.13, respectively. Note the significant variation in the fiber
volume fraction as a function of thickness at early times, but as one approaches a steady
state, the Vf becomes more uniform. •

0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
Figure 8.12: Resin pressure versus dimensionless thickness [298].
0.75
0.70
0.65
0.60
0.55
0.50
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
Figure 8.13: Fiber volume fraction versus dimensionless thickness [298].

Heat Transfer and Cure
The hot autoclave walls and the heated air inside the autoclave transfers heat to the com-
posite surfaces by radiation and convection respectively as shown in Figure 8.14. This heat
is transferred to the interior of the composite by conduction and raises the internal energy
of the composite and hence the temperature of the resin present in the composite. The
raised temperature will initiate the curing of the resin which is an exothermic chemical
reaction that cross-links the resin molecules and releases the heat. The heat released can
be modeled as an energy generation term that further raises the temperature of the com-
posite and needs to be conducted out of the interior of the composite as the curing reaction
approaches completion. Thus, one needs to first increase the temperature of the autoclave
and later reduce it to extract the heat of the reaction and cool the composite part.
Figure 8.14: Curing of a composite in an autoclave.
To simplify the analysis, one can assume that the resin bleeding is complete and can use
the energy conservation principle to write the governing equation to predict the temperature
field inside the composite as a function of time. This temperature field will be a function of
the thermophysical properties of the composite, the cure kinetics of the resin, the geometry
of the part and the temperature of the autoclave. One could control the temperature
history of the composite by changing the temperature of the autoclave. Mathematically,
this translates into boundary conditions on the composite surface that may be of the first,
second or third type as discussed in Chapter 3.
One can obtain the following governing equations for conservation of energy and resin
cure state with temperature as a primary variable for a composite that is undergoing curing
without any resin flow:
.dT d // £. &T\I J d /, dT\1 _| d (/ 1I. dT\I _l_ (.1
„ dC* ,,
T\fr\rt
d- 1
n f-.,
dt
—
— r-. I ^x ^ I ^ f-i
[ L
dx \ dx J dy \ dy JJ ~*~ dz
I ^V r-i o I ^2 r-i
\ dz JI "TV-*-
dt,. •
f7
VflPrflr
(8.23)
Here p is the density, Cp is the heat capacity and V/ is the fiber volume fraction. The
subscript r is for the resin and / is for the fibers. kx, ky and kz are conductivities of the
composite in the x, y and z directions, respectively. dC*/dt is the degree of cure expressed

by constitutive equation for that particular resin. Some examples are given by Equations
(4.77) and (4.78). For example,
rlC1*
^— = k0exp(-E/RT)(C*)m(l-C*)n. (8.24)
By selecting the cooordinate directions to coincide with the principal directions of the fiber
preforms, one can write the governing equation as cast in the form of Equation 8.23. The
composite is usually much longer in the in-plane directions (a; and y directions) as compared
to the thickness direction and hence one can usually eliminate the first and second terms
on the right hand side in the analysis (see Example 5.3 in Chapter 5 for details). The
constitutive form of the cure kinetics equation is usually a function of the temperature
and the current cure state (Equations (4.23) through (4.31)). One can solve Equations
(8.23) and (8.24) simultaneously to obtain the temperature and cure history as a function
of the imposed boundary and initial conditions. The initial condition for the composite
temperature is usually room temperature, and for cure it is zero cure. The boundary
conditions are related to the temperature of the autoclave. The simplest approximation is
that the temperature of the two surfaces at z = 0 and at z — h is equal to the autoclave
temperature Tw(t), and one can solve the coupled system of equations to obtain temperature
and cure simultaneously. See reference [300, 301, 302] for details.
8.3 Liquid Composite Molding

Liquid composite molding (LCM) is a class of composite manufacturing processes in which
a mold cavity containing a reinforcing preform is injected with liquid thermoset resin to fill
the empty spaces in the mold. After the resin cures partially or completely, the composite
part is demolded. LCM is used in almost all industries that benefit by switching from metals
to composite parts. They include the aerospace, automotive, marine, and civil industries.
The reinforcing fabric preform is usually made of continous glass or carbon fiber mats, and
it can be dry or preimpregnated when it is placed into the mold cavity. The objective of the
process is to manufacture composite parts by completely wetting the fabric preform with
resin at the macro and micro scales with no regions that are resin starved. The following
are the most commonly used LCM processes:
• Resin Transfer Molding (RTM)

• Vacuum Assisted Resin Transfer Molding (VARTM)
• Seeman's Composites Resin Infusion Molding Process (SCRIMP)
• Injection Compression Molding
• Reinforced Reaction Injection Molding (RRIM)
• Structural Reaction Injection Molding (SRIM)
8.3.1 Similarities and Differences Between Various LCM Processes

LCM processes can be broadly classified into two groups: matched mold processes and
single-sided mold processes.

Matched Mold Processes
Matched mold LCM processes include RTM and Injection compression molding. As the
name implies, the molds have at least two rigid parts. If the composite part to be manufac-
tured does not have a very intricate or complicated shape, then the mold usually consists
of a two-part cavity for the preform. As the complexity of the shape or the size of the
part increases, then the male and female halves might be constructed from smaller pieces
in order to ease the demolding as shown in Figure 8.15.
Figure 8.15: Various mold sections to manufacture the composite part depicted on the
bottom right.
Under compressive clamping force, the mold parts completely enclose the fiber preform
that is placed inside. By conforming the preform to the desired dimensions of the final
part, a near-net-shaped part can be manufactured by this type of LCM process. However,
process and design engineers should be careful in selecting the mold material. If the thermal
expansion coefficients of the mold and composite materials are dissimiliar they will expand
or contract at different rates during the heating/cooling stages of cure. This will usually
lead to significant warpage or cracks in the composite part. Usually exact match of the
thermal coefficients is not achievable, and design engineers have to adjust the mold cavity
dimensions to compensate for the different expansion and contraction rates of the two
materials. However, the key advantage is that this type of process allows one to obtain very
tight tolerances which is rarely possible with one-sided molds.
RTM, the most widely used of the closed mold processes, was first introduced in the
1940s. A schematic of the RTM process is shown in Figure 8.16. One can describe the RTM
process in five steps: (i) manufacturing of reinforcing preform, (ii) draping of preform over
a tool surface, (iii) compaction of preform by closing and clamping of the mold, (iv) filling
the empty spaces between the fibers of preform with resin and cross-linking of the resin,
and (v) demolding.

Part removal
1. Preform Manufacturing
5. Demolding and Final Processing
Resin
2. Lay-up and Draping 4. Resin Injection and Cure
3. Mold Closure
Figure 8.16: Schematic of the process steps in RTM.
The reinforcing fabric preform is usually manufactured by stacking individual fabric

layers. During the draping stage, the fabric tows (bundles of fibers) undergo structural
deformation if the mold has a doubly curved cavity, corners and ribs [303]. A tackifier
adhesive (binder) is added to hold the individual fabric layers together in order to ease the
handling and placement of fabrics, especially if the mold cavity is complicated or a large
number of layers are stacked. During the compaction stage, the fibers mostly compact in
the thickness direction. The draping and compaction can change the permeability of the
reinforcing fabric very significantly and nonuniformly and influence the resin injection stage
[304, 305].
The RTM process is widely used due to its many advantages, including the following:
• Near-net-shaped composite parts with a good surface finish and close dimensional
tolerances.
• Large parts with complicated shapes.
• Achievement of good mechanical properties by tailoring (i) the structure and the
stacking order of reinforcing fabric, and (ii) the resin system.
• Use of metal inserts in order to attach the part to the main structure.
• Use of internal wood or foam cores to reduce cost and increase the stiffness of the
part.
• Consistency in reproducibility of parts compared to wet hand layup.
• Fast production cycles compared to wet hand layup.
• Low mold clamping pressure compared to processes such as injection compression
molding.
• Much less exposure to volatile chemical vapor than wet hand layup.

• More automated (less labor skill needed) than wet hand layup.
Although the items listed above make the RTM process very promising for the manufac-
turing of composite parts, there are some disadvantages that need to be overcome, including
the following:
• Inconsistency in reproducibility: inherent variations in preforming due to inconsis-
tent fabric rolls from vendors, and inconsistencies in fabric cutting, stacking, pre-
impregnating, and placement into the mold cavity.
• Sensitivity to mold design, since improper gating and venting can cause incomplete
filling of the empty spaces and result in macroscale dry spots (resin-starved regions)
in the composite.
• Long production cycles compared with parts made from aluminum or steel in auto-
motive industry.
• Higher clamping pressures than vacuum bagged VARTM and SCRIMP.
• Movement of preform (wash out) due to loose compaction and/or high resin pressure.
A variation of RTM involves drawing a vacuum in the cavity before the resin injection
is initiated. By removing almost all of the air from the mold cavity, the chances of void
formation are significantly reduced. It also reduces the required injection pressure or/and
the time to fill the mold. However, vacuuming inside the mold sometimes can cause the
resin to bubble if its vapor pressure is low.
A relatively new modification in matched mold processes is called injection compression
molding. In this process, the mold is closed to nearly but not exactly its final thickness
creating an empty space between the mold and the preform, after the preform is placed into
the mold cavity. The amount of resin needed to fill the closed mold is injected into this
empty space between the mold wall and the preform. Because the resistance to flow in the
preform is orders of magnitude higher than the resistance offered by the space between the
mold and the preform, the resin fills this space first. After the calculated resin is injected,
the mold is gradually closed (compressed) to the desired dimensions pressuring the resin
and squeezing it into the preform in the thickness direction. Injection compression molding
allows one to reduce the injection pressure and fill time as compared to RTM but requires
a press that can control the compression process [306].
Single-Sided Molding Processes

"Vacuum bagged" vacuum-assisted resin transfer molding (VARTM) and SCRIMP are
single-sided LCM molding processes. As the name implies, these processes have only one
rigid side of the mold. In "vacuum bagged" VARTM, after the preform is placed into the
cavity of the rigid female mold part, a vacuum exit tube and resin inlet tubes are placed
around the preform. Then, a plastic film layer is placed on top of the preform and tubes,
and sealed using "tacky" tape. The air inside is removed through the vacuum exit tube
by using a vacuum pump drawing air through the vacuum exit tubes and clamping the
resin inlet tubes. Once sufficient vacuum is created the resin inlet tube is inserted into a
resin pot, and the clamp is removed. Pressure differential of one atmosphere between the
resin container and the interior of the mold pulls the resin into the mold. After the mold is
saturated with resin and reaches the vent, the resin injection is discontinued.by clamping
the tubes. Once the resin cures, the part is demolded, and the tubes and plastic film are
discarded. Figure 8.17(a) shows a schematic of this process.

Vacuum
Resin Injection
Bagging
t Vacuum
Tube
Figure 8.17: (a) "Vacuum bagged" VARTM and (b) SCRIMP [307, 58].
FASTRAC layer
graphite or
inner vacuum bag fiberglass
L
primary (inner)
vacuum line x>
secondary (FASTRAC )-
vacuum line
Figure 8.18: Schematic of the FASTRAC process [308].
The major advantages of the single-sided LCM processes are (i) a very simple injection
system, (ii) a simple mold, (iii) visual control of filling stage on the surface through the
transparent plastic film (iv) capability to manufacture parts of the order of a few meters
such as train and bus compartment sides that can be upto 15 meters long, and (v) low
capital investment.
However, there are many disadvantages, including (i) long fill time due to low injection
pressure of 1 bar, (ii) low fiber volume fraction due to low compaction pressure of 1 bar,
(iii) low quality surface finish and low dimensional tolerance, (iv) requirement for skilled
labor during the bagging stage, (v) labor intensive as in Autoclave processing, (vi) material
wastage is much higher than other processes, and (vii) for thick parts, formation of voids
through the thickness, as one can visualize only the resin close to the top layer adjacent to
the plastic film.
In order to overcome the long fill time disadvatage of VARTM, The Seeman Corpo-
ration resin infusion molding process (SCRIMP) was developed and patented under their
company's name. A very porous fabric, known as the distribution medium, is placed on top
of the preform. Since it has very low resistance to resin flow, resin saturates this porous
layer quickly and then flows into the reinforcing preform in the thickness direction. Other

Figure 8.19: Resin flow in three early frames of FASTRAC [308, 309].
similar processes such as FASTRAC have been developed to improve the delivery approach
to get the resin from the container to the surface of the preform quickly. In such approaches,
channels are formed along one of the faces of the mold to distribute the resin along one
of the faces as shown in Figure 8.18 [308]. The quick distribution of the resin is shown in
Figure 8.19 [308, 309].
8.3.2 Important Components of LCM Processes

The major ingredients of LCM processes are the fiber preform, resin system, mold and
injection equipment. We will discuss them briefly here. Details can be found in many
books written about this process [53, 214, 310, 311].
Fiber Reinforcements and Inserts

The most commonly used reinforcement fabric materials are fiberglass, carbon, and aramid
(Kevlar). Proper fabric material and structure type (woven, stitched, knitted, braided,
random, etc.) must be selected considering mechanical properties, surface finish, and cost
criteria. Strength and stiffness of composite parts depend on the reinforcing fabric. Resin
acts as a matrix that holds the fibers together, and plays an important role against wear
and corrosion of fibers.
Resin is expected to fill the empty spaces between fiber bundles and also the interior
of each fiber bundle. Fiber volume fraction is the ratio of the fiber volume to the total
volume of fabric. The fiber volume fraction of a preform in a closed mold depends locally
on the mold gap thickness, number of fabric layers and in-plane compaction around corners
and ribs if they are present. Permeability of a reinforcing preform, which is a measure
of resistance to resin flow, is dependent on fabric structure and fiber volume fraction. An
ideal fabric should have high wash resistance and wettability, and sizing on its fiber surfaces.
Wash is the movement of fabric under high resin pressure. Wettability is a measure of how
easily an interior of a fiber bundle is wetted as resin moves around the bundle. Sizing is a
coating on the fiber surface in order to increase the wettability property and also to increase
the bond between the fibers and the resin as it cures. Different sizings are used on the fiber
surfaces to make them compatible with the selected resins.
The structure of the fabric reinforcement can be tailored in order to achieve the de-
sired mechanical properties such as tensile strength and stiffness. However, the structure
affects how resin flows through it. Hence, while designing new fabric structures, not only
mechanical properties, but also permeability and wettability properties must be considered
simultaneously. A fabric structure with a high resistance to resin flow (low permeability)
will require higher injection pressure or filling time. In some industries such as aerospace,

this might be acceptable as the mechanical properties are more important but may not be
viable for other high-volume production industries.
In order to ease the handling and placement of preform into the mold, a veil, or a
tackifier adhesive (also called binder) is used by spot-glueing the adjacent fabric layers of
preform to each other. Tackifiers are made by dissolving the resin in a solvent. A tackified
preform allows one to place the preform into the mold easily and reduces the possibility of
creating unplanned empty channels between the preform and the mold wall, where resin can
flow easily due to low resistance to flow. This racetracking phenomenon can dramatically
change the flow patterns as the resin impregnates the preform and can lead to unpredictable
fill patterns. However, the disadvantage of using tackifier is that the permeability of the
preform can reduce locally at the glued spots.
Between the reinforcing fabric and the resin, a strong bond should be created by treating
the surface of fibers. This process is called sizing. The reasons why sizing should be applied
are as follows:
• The major part of load on composite part will be directly transferred to the reinforcing
fabric through the matrix without damaging the matrix due to the strong interface
bond.
• The fibers will be lubricated against potential abrasive damage during handling and
preforming operations such as weaving.
• Static electricity between the fibers will be minimized.
Cores such as foams and balsa wood are included inside large and thick parts. Cores are
used to lower the cost, increase the moment of inertia, and reduce the weight of the part as
cores have lower density than the rest of the composite part. If a runner network is machined
into the cores, resin moves more rapidly in the mold through the core runners. Besides the
advantages of cores, there are some disadvantages that design engineers must be cautious
about. Cores might shrink or even collapse during the resin filling and curing stages. Resin
pressure must be kept below the compressive strength of the cores. Also, during the heating
and exothermic curing stages, the temperature of cores should not exceed a critical value
which may otherwise deform the part.
As an alternative to cores, internal inflatable bladders might be used in thick parts such
as tennis racquets and rotor blades [312]. The bladder is initially under inflated. After the
preform is placed and the mold is closed, the bladder is inflated further.
Metal inserts, which are usually steel, can be placed inside the mold which allows the
composite part to be attached to other parts of the structure. The surface of inserts must be
processed to enable a good bond between the insert and the surrounding matrix. The ther-
mal expansion coefficient of insert material should not be much different from the composite
material. The insert material must also be resistant to corrosion.
Textile type preforms are manufactured by weaving, stitching or braiding fiber tows
(fiber bundles). The elliptical tow cross section has dimensions of the order of millimeters.
High strength composite parts such as the ones used in aerospace are made of very dense
fiber tows with up to 48,000 fibers in each tow. "Chopped" and "continuous strand" random
fabrics are manufactured from inexpensive and short E-glass fiber tows which contain about
100 fibers.
In hand preforming, also known as cut-and-place preforming, dry fabric layers are cut
from rolls and placed into the mold cavity. Fabric stacking might consist of different types
of fabric and/or varying orientation. This method eliminates preforming instrumentation,
but requires many manual hours. Consequently, reproducibility of parts is not consistent.
Stamping of fabrics with a thermoformable binder is a versatile and automated preform-
ing process. A small amount of thermoformable binder is added to nonwoven glass fabric

layers that are cut larger than the mold cavity surface area. Fabrics are heated around
150°C to soften the thermoformable binder in it. Fabric layers are then stamped in the
mold cavity at lower temperatures as thermoformable binder stiffens and holds the shape.
The excess fabric outside the mold cavity is then trimmed. This process has the advantage
of preparing preforms with accurate dimensions which eliminates the tedious labor and
skill required to cut and place preforms stacked by hand, and also eliminates the potential
racetracking channels created between the preform and mold walls. Another advantage is
that the preform has higher resistance against resin wash as it is stiffer. A drawback of this
method is that some fabrics, such as directional and carbon fabrics, cannot take advantage
of this method as they don't stretch during the stamping stage. Another disadvantage is
that the fibers might buckle during the stamping stage.
Resin System
Resin forms the matrix of the composite part after it polymerizes. A resin system may
consist of some or all of these ingredients: promoters, fillers, mold release agents, pigments
and catalysts. Some of the most commonly used resins in LCM are polyester, epoxy, vinyl
ester, urethane, and nylon. Fillers such as clay, aluminum trihydrate and calcium carbonate
are used to reduce costs. A good resin system should have the following properties:
• Low viscosity to ease injection.
• Effective wetting properties to wet the fabric.
• Uniform and consistent cure kinetics.
• Rapid cure after gelation.
• High transition temperature.
• High tensile strength to support the reinforcing fabric under load.
Low resin viscosity is desirable as it will require low injection pressure under constant
flow rate injection, or short filling time under constant pressure injection. If the resin
viscosity exceeds a typical upper bound of 500 centipoise (typically, one centipoise is the
viscosity of the water), it will not only require high injection pressure equipment, but might
also "wash-out" the fabric by forcing it to move from its originally placed configuration.
At the other extreme, injecting a resin with too low viscosity (typically lower than 50
centipoise) is much easier, but it may fail to "wet-out" the interior of each individual fiber
tow (fiber bundle) even if the resin impregnates the empty spaces between the fiber tows.
A thermosetting resin system can be injected either as a single component system or
a multiple component system. In multiple component systems, the resin is premixed with
the cataylst in a single container in the desired ratio and injected into the mold. This is
a simple and reliable system but one must use up the resin before it gels or have to clean
the container before the next injection. The other option, the single component system
requires separate containers for the resin and the catalyst or the accelerator, which are
mixed "on the fly" as they enter the mold. This allows the flexibility of changing the mix
ratio to accelerate or decelerate the cure. However this could introduce variability in the
part quality due to uneven mix or cure.
Table 8.2 shows a comparison of the most commonly used LCM thermosetting resins
from the viewpoint of performance, processing and cost [9].
Resin cures due to the chemical reactions to create a matrix around the reinforcing
fabric. Usually, the chemical reaction is a step- and/or chain-growth polymerization. The

Table 8.2: Thermoset Resins Commonly Used in LCM Processes [9]
Resin type Performance Processing Cost Aerospace industry Automotive industry
Polyester Low Ease Low v7 V
Vinyl Ester V7 V
Urethane v V
Epoxy V y
Cyanata Ester y
Bismaleimide v7
Phenolic V V
Polyimide High Difficult High V
length of the cure cycle depends on the type of resin system and temperature of the heating
system. During the cure cycle, the viscosity increases and then eventually gellation starts
at Tgei. The cure kinetics of resin systems, especially the length of the cure cycle, can be
adjusted by changing the amount of catalyst and accelerator that are added to the resin
system. Some resin systems are designed for room temperature cure.
The strength of the matrix starts to build up after Tgei. The part is demolded when the
matrix reaches a "green strength" such that the part will not deform or warp after being
taken out of the mold. Wedges, mallets or hydraulic ejection system can be used to demold
the part.
Demolding the part before it reaches the maximum strength has advantages and disad-
vantages. The main advantage is that the production cycle is shortened by enabling early
injection of the next part. Another advantage is that the damage due to exothermic resin
cure reaction on the mold surface is reduced. The disadvantage is that the demolded part
might warp or develop scratches on its surface. Hence, demolding should be done neither
too early nor too late. Some trimming might be needed to remove excess matrix along the
edges of the part.
Although most RTM applications use thermoset resin systems, research is underway to
use thermoplastic resin for RTM due to the added attraction of recyclibility. The research
is focused on reducing the viscosity of cyclic thermoplastic resins to the order of thermoset
resins to promote impregnation.
Mold (Tool)
Mold material must be selected considering the production volume, the temperature bounds
of the heating/cooling system, tolerances in part dimensions, and the quality of surface
finish required. Steel, aluminum and copper are the most commonly used metals. Steel
is preferred for high volume production because of its high resistance to wear and hence
can last longer. Aluminum and copper are easier to cut during tool making. For low
production volumes (less than several thousand parts), nonmetallic materials such as wood
and reinforced polyesters or epoxy composites are preferred because of easy and rapid tool
manufacturing and low cost.
Temperature fatigue, solvents, mold release agents and accidental scratches made on
the manufacturing floor cause wear of the mold surfaces. A nickel shell on the mold cavity
surface delays the wear of the surface and is usually applied to molds that need to produce
large number of parts.

Release agent is sprayed on the mold cavity surface in order to ease separation of the
composite part from the mold surface. An inflatable bladder mold half made of silicone
rubber might be used, instead of a rigid mold half, to ease demolding of large parts with
complicated shapes.
The locations of gates (resin inlet ports) and vents (air and resin exit ports) must be
properly designed such that the reinforcing fabric is completely wetted when resin reaches
the last vent. Resin is injected into the mold cavity through the gates, and the air in
the mold cavity is pushed out by the propogating resin through the vents. Mold design
engineers use either their experience along with some trial and error mold fillings or mold
filling simulations in order to properly place the gates and vents. Once the gate locations
are decided, vents are placed at the last points of filling in order not to entrap air inside the
mold. After the resin bleeds out from the last vent, a little extra time is allowed for complete
wetting of the fibers. Then, all of the gates and vents are closed. At this time, resin might
continue to percolate to wet the interior of the fiber tows. Unconventional techniques such
as vibrating the mold or the inlet flow rate in order to wet the spaces between the fibers in
a tow are used to eliminate micro voids [313].
Although the resin pressure in RTM is usually less than 20-30 bars, this pressure can
cause resin leakage through the edges of the mold if the mold is not properly sealed. In
order to prevent leakage, temperature and solvent resistant O-ring silicone rubbers are used
along the perimeter of the mold.
Some resin systems require elevated temperatures to cure. Once the resin cures, the part
is demolded much more easily if the mold is cooled down. In order to heat and then cool
the mold, heating/cooling channels are machined inside the mold as shown in the computer
model in Figure 8.20. Or, alternatively, the mold is placed into an oven for the heating
stage.
Upper half
of mold
Composite Part
Lower half
of mold
Figure 8.20: A finite element model of a complex RTM mold with heating and cooling
channels and the composite part.
Runner systems (a network of resin-carrying tubes for the inlet gates) are sometimes
used to reduce the filling time or reduce injection pressure by having multiple resin carrying
tubes, T or multiple connectors, and valves between the injection machine and the mold,
instead of having a single tube and and a single gate. For large parts, runner systems are
required in order to inject the resin within a limited time (of the order of minutes), before

resin starts gelation. However, while attempting to improve the process, the outcome could
become worse. Design engineers must be vigilant about where the flow fronts of resin
propogating from different gates meet because it could lead to entrapped air if the flow
fronts do not merge in the vicinity of vents.
By using a vacuum pump and a good mold seal, most of the air inside the mold cavity
can be removed. This will reduce the resin injection pressure or filling time and also the
content of voids (dry spots) in the part. However, this additional instrumentation adds to
the cost, and some resin systems may bubble under vacuum.
Injection System
Simple injection equipment can be used for single component resins, or batch mixed multi-
ple component resin systems. However, expensive injection equipment with the capability
of mixing the resin components is preferred for high production volumes of composite parts
with multiple component resin systems. Ideal injection equipment should allow the man-
ufacturing engineer (i) to change injection pressure or flow rate, (ii) to open and close
gates for sequential gating by opening/closing gates, and (iii) to monitor the temperature,
pressure, flow rate and cumulative amount of resin injected.
Most of the injection equipment is designed for either pressure controlled or flow rate
controlled injections. Flow rate controlled injection equipment should allow the user to set
an upper critical injection pressure to protect the mold from damage and bending. Once
the critical pressure value is reached, either the flow rate may be reduced, or the injection
may be continued at the critical pressure value.
Radius Engineering Inc. [314] and Liquid Control Corp. [315] are some injection equip-
ment manufacturers for LCM. Plastec and Liquid Control allow for single component sys-
tems, where one has separate containers for the resin and the catalyst and one can pre-select
the mix ratio before the injection. Figure 8.21 shows an injection machine with simple con-
trols from Radius Engineering Inc. [314].
Figure 8.21: Radius injection machine [314].

8.3.3 Modeling the Process Issues in LCM
Once the mold is closed, even in one-sided mold processes, one cannot know or see if the
resin has completely saturated the preform or if there are regions inside the composite with
only "dry" fibers (uncovered by the resin). Sometimes even very small regions without resin
can cause catastrophic failures of the composite part. Modeling of the flow will allow one
to investigate the resin impregnation process and strategically design gates and vents and
injection schemes to optimally fill the composite part without any dry spots. Almost all
of the issues that influence flow impregnation are related to the permeability in the mold.
Higher permeability along the walls and corners of the mold due to unintentional gaps
between the preform and the mold wall causes racetracking and changes the flow pattern
dramatically. Draping the fabric over the tool surface can make the permeability change
in magnitude and direction over doubly curved surfaces and introduce changes in the flow
pattern of the impregnating resin. If the permeability of the fiber tows is distinctly less
than the permeability between the fiber tows, it gives rise to a dual scale porous medium
flow in which the fiber tows may fill at a much slower rate than the flow in between the
tows. In addition, if the flow slows down dramatically, surface tension effects of the resin
can influence the microscopic flow pattern. These issues are schematically shown in Figure
8.22.
Thus, during the mold filling stage these flow issues can influence the final quality of
the manufactured part and the decision as to whether one can adopt the LCM process to
manufacture a selected net-shape part. The flow issues arise due to significant changes in
the flow pattern as a result of minor changes in the material or process parameters. Below,
we discuss the most crucial ones that could be modeled and incorporated into simulations
to understand and resolve such issues.
Racetracking
When the fiber preforms are placed in a mold, one may inadvertently create a small gap
between the mold wall and the preform. The flow always uses the path of least resistance
and will race along this edge. This phenomenon has been termed racetracking [54, 316, 317,
318, 319, 320, 321, 322]. Figure 8.23 shows experimental snapshots of racetracking along an
edge of a mold, and Figure 8.24 depicts the changes in the flow pattern due to racetracking
around edges and a corner in a simulated mold filling example.
This racetracking is manifested not only along the mold wall edges and corners but also
around ribs, T-joints and inserts which are usually present in complex net shaped structures.
Tackified preforms could provide a good solution to reduce the possibility of racetracking
channels or at least make such disturbances tractable. A predictable model of resin flow
with racetracking along the edge can allow the process engineer to take advantage of such
channels to impregnate the part. Hence modeling of such channels will be very useful.
Example 8.4: Permeability of a Racetracking Channel

Consider a racetracking channel as shown in Figure 8.25. The bulk permeability of the pre-
form in the flow direction is Kbuik = 1 * 10~10 m 2 . The thickness of the mold is 1 millimeter
and the channel width is, on an average, one millimeter. Estimate the permeability of the
channel.

Racetracking
Transverse Flow
Macro Void Formation
Unsaturated Effects
Preform Deformation &

Micro Void
Compaction Formation
Figure 8.22: Flow issues in LCM filling process: (i) race-tracking, (ii) macrovoid formation,
(iii) transverse flow, (iv) preform deformation due to draping and compaction, (v) microvoid
formation, and (vi) unsaturation effects [54].
Figure 8.23: Experimental snapshots of racetracking along the left edge of a rectangular
mold cavity [316, 319]. Resin enters the mold cavity from the upper edge by creating a line
injection. Horizontal flow fronts would be developed if there was no racetracking.

(a) Mold gap
zoom
zoom
zoom
(b) No racetracking (c) Racetracking channels

Air
I I
Flow fronts
Figure 8.24: Simulated racetracking along the edges of a mold: (a) mold gap with possible
regions for racetracking, (b) no low resistance areas; hence, simulation shows uniform filling
pattern, and (c) racetracking along the edges changes the flow pattern significantly and can
cause dry spots during manufacturing.
.V"
' * &•**'
ic sli at !«• iiji

.*"
•-•-•-
^ V
ftPHJI flO«JV ' "*
Figure 8.25: A schematic to estimate the permeability in a racetracking channel.

Solution
One can solve for fully developed flow through a rectangular channel to find the flow rate
pressure drop relationship. For viscous resins and low Reynold's number flows, fully devel-
oped flow assumption is valid. By integrating the velocity profile through the thickness,
one can find the average velocity. By comparing this equation with Darcy's law for one di-
mensional flows, one can estimate the permeability of the channel. Two other assumptions
are (i) the flow is in a channel with all solid boundaries (although in our case there is one
porous boundary and one would expect slight loss of fluid in that direction) and (ii) most
of the flow takes place in the flow direction, which is a reasonable assumption.
Consider a channel of height h and width w as shown in Figure 8.25. First, a simple and
approximate answer will be attempted by assuming that the flow in the channel direction
(which is the x direction) is a function of z only; that is, ux = ux(z}. This is a good
assumption if w S> h. Poiseuille flow will be induced under applied an external pressure
gradient, as shown in Chapter 3. From Equations (3.70) and (3.71), the velocity and flow
rate are written as follows:
Ux\Z) -— T ~ \z rizj (jj.ZiOj
L\X £fji
and
fh
Ul(z)dz = -^^-. (8.26)
One can also write the flow rate using Darcy's law:
AP
= Ui(wh) = ,^^^. (8.27)
The permeability of the racetracking channel, Krstce can be obtained by equating the two
flow rates, Qp0iseuille = QDarcy
^race = ~- (8.28)
For a gap of h = 0.001 m, Equation (8.28) results in Krace = 8.3 * 10~8 m 2 .

To obtain a more accurate result, one can relax the assumption that w ^> h as in most
cases w will be less than or of the order of h. Now, as w = O(h), and ux = ux(y,z), one
must solve the exact Stokes flow by applying no-slip boundary conditions on all four edges of
the channel (still retaining the assumption that there is no porous wall) [323, 54, 324, 102].
The corresponding flow rate is then calculated as [102, 319, 325]
r rw h/i2 192ft ^ tanh (iirw/2h)

= / / ux(y,z}dydz = -—
Jo Jo 12 7T°U> . ^ I5 Ax
4=1,3,5,...
The permeability of the channel Krace is obtained by equating Q in Equation (8.29) to

one-dimensional Darcian flow rate, Q = whux = — (•w;/i.Krace/M)(AP/Ax)
192/1 ^ tanh (iirw/2h}

i =— y = (8.30)
TT^W 4=1,3,5,...
, /rl i°
For channel dimensions of h = w = 0.001m, it is calculated that Kiace = 3.51 * 10 8 m 2 ,

which is 42% of the value found by assuming w S> h, which resulted in KTace = ^. Krace

is tabulated in Table 8.3 for different h and w values. The last column clearly shows that
as the width of the channel, w increases by two or more orders of magnitude of the height
of the channel, h, the permeability found using the exact Stokes equation approaches the
simple one dimensional channel flow solution which is independent of w.
Table 8.3: Permeability Krace of a Rectangular Racetracking Channel with a Height of h

and a Width of w. All Four Walls of the Channel are Assumed to be Nonporous.
•""•race
h [m] w [m] ^race [m2] h2
12
0.001 0.0001 7.81E-10 0.01
0.0005 1.43E-08 0.17
0.001 3.51E-08 0.42
0.005 7.28E-08 0.87
0.01 7.81E-08 0.94
0.1 8.28E-08 0.99
0.002 0.0002 3.12E-09 0.01
0.001 5.72E-08 0.17
0.002 1.41E-07 0.42
0.01 2.91E-07 0.87
0.02 3.12E-07 0.94
0.2 3.31E-07 0.99
Note that substitution of the values for h and w = O(l)mm gives an estimate for Krat
channel which is about two to three orders of magnitude larger than the .Kbulk = 1*10~10 m
Macrovoid Formation
Macrovoids are formed when the air being displaced by the resin gets entrapped or when
there is not sufficient resin pressure to overcome the resistance offered by the fiber preform
and/or the viscosity of the resin. Figure 8.26 shows snapshots of a mold filling situation
at different times in which the resin is impregnating the preform. The experiment clearly
shows the formation of the dry spot or the macrovoid.
These dry spots (voids) might significantly reduce the strength of the composite part
depending on the location and the size of them. The size and location can usually be
detected by nondestructive evaluation (NDE) methods such as ultrasound. Entrapment of
dry spots is a critical issue as it will cause a high rejection rate. Flow modeling can definitely
help in eliminating or reducing the size of the dryspot by identifying the last regions to fill,
once the injection gate locations are specified. This will allow the mold designer to place the
vent locations in the last regions to fill. The current trial and error methods allow the resin
to bleed out of the vent for sufficient time in the hope that the void will get transported
towards the vent and eliminated. This technique may be successful, if the void is within
the proximity of the vent. Morevover, flushing of the resin causes wastage and increases the
cycle time.

Figure 8.26: Snapshots of resin impregnation from two injection gates at different times in
a mold containing fiber preforms with low and high fiber volume fraction Vf. Macrovoid or
dry spot formation results due to incomplete filling [326].
Transverse Flow
As most composite structures are thin, one can ignore the flow in the thickness direction
and assume an average value for it. This is a good assumption when the in-plane permeabil-
ities of the preform do not change by orders of magnitude through the thickness. However,
transverse flow can be significant if the transverse permeability component of a fabric pre-
form is much smaller than the in-plane components (see Example 5.8 in Chapter 5). Also,
for processes such as SCRIMP and FASTRAC, the main goal in the process is to speed up
the flow or reduce the pressure requirements by flooding the preform face with the resin
by introducing a very high in-plane permeability material. This will introduce flow across
the thickness of the composite which will be very nonuniform and may trap macrovoids
as shown in Figure 8.27. In VARTM, the transverse flow is significant if L\ ^> LI where
LI and 1/2 represent the distances between the injection gate and the flow fronts in the
distribution medium and bulk preform, respectively, as shown in Figure 8.28.
To address this issue, one must address the flow in the transverse direction. Either
analytic models [327, 328] can be developed or fully three dimensional simulations need to
be implemented [329, 330, 331, 332]. One would also need to characterize the transverse
permeability of the preform which is usually much more difficult to measure [333, 334, 335].
Dual Scale Preforms and Microvoids

Many fabrics consist of fiber tows (bundles of fibers) that are either woven or stitched. This
usually will create two scales of permeabilities. The resistance to flow between the fiber

Dry preform
Transverse flow Resin

:
s Mold wall
Trapped macrovoids
t=t
:f Mold wall
Figure 8.27: Transverse flow traps macrovoids in the part.
Distribution Media
A.
• ^ l : transverse flow negligible
•:» i : transverse flow significant
Figure 8.28: Transverse flow in VARTM/SCRIMP.

tows may be different than the resistance within the tows. Thus, if the resin flows faster
within the tows, it is likely to create microvoids between fiber tows when it gets wicked due
to capillary action across a stitch as shown in Figure 8.29 [336].
Inter-Bundle
Voids
1
Intra-Bundle
Voids
Figure 8.29: Microvoids are created because the permeability inside a fiber tow region is very
different than the permeability of the region between the fiber tows in woven and stitched
fabrics, (a) Interbundle voids are created as resin races along the tows and encircles itself
along a stitch, (b) Resin flow is faster in between the tows which traps voids in between
the fiber bundles [336].
However, if the flow is faster in between the fiber tows, the resin will encircle itself along
a stitch and entrap a microvoid within a fiber tow as shown in Figure 8.29. This issue is
usually addressed on the manufacturing floor by slowing the flow down, allowing sufficient
time for the regions within the tow to impregnate as in most instances, the fiber tow regions
are about two to three orders of magnitude less permeable than the regions in between the
fiber tows. Modeling can help understand the important parameters that influence this flow
in between and within the tows which should prove useful in eliminating the microvoids.
Hence, it may be important to include this phenomenon in flow modeling.
Heat Transfer and Cure

For LCM processes one usually aims to saturate the mold and fiber preforms with the resin
before the curing reaction immobilizes the resin. Hence it is important to fill the mold before
resin cure reaches the threshold value where the viscosity starts to increase dramatically.
(See Equations (4.23) through (4.31) in Chapter 4.) Secondly, it is important to know the
time to demold the part which is equal to the time the part takes to reach its green strength
(sufficient strength to retain its shape). A very important issue is also the development of
temperature gradients and cure across the thickness of the part. For thin parts of thickness
less than 3 millimeters, this is less critical as one can remove the heat quickly by conduction
through the surface of the part. For thicker parts, the conductive resistance increases and
one can develop significant temperature gradients which will lead to build up of residual
stresses and eventually cause warpage and shrinkage.

Example 8.5: Relationship Between Cooling Rate and Temperature Gradient
Through the Thickness of a Composite
Thermal design criteria require you to keep the temperature differential between the center
and the surface of the composite to less than 10°C. You know that a cooling rate of 10
Watts/sec for a 3 mm thick composite was able to do so for an epoxy resin. Design and
scaling requires you to quadruple the thickness of the composite. What is the maximum
cooling rate you can impose if the thermal design criteria must also be met?
Solution
Under steady-state conditions, one can show that
gi = ^ (Tw - Tc] (8.31)
where qi is the cooling rate of the thin composite of thickness h\ and kt is the transverse
conductivity of the composite. (Tw — Tc) is the temperature difference between the wall
and the center. Thus if the thickness is quadrupled, the cooling rate should be reduced to
one-fourth to continue to maintain the thermal design criteria. Hence the cooling rate for
the thicker composite should not exceed 2.5 Watts/sec. •
The above example was a very crude estimate as we assumed steady state. Polymers
and glass generally have a low thermal diffusivity and hence it takes them much longer to
reach steady state as compared to the processing time. To obtain more accurate predictions
it is useful to solve the governing equations with numerical methods to obtain more accurate
predictors. Example 5.5 shows how one could solve for the transient problem to obtain a
better prediction of the temperature field.
In the last two decades, numerical simulation codes have been developed that incorpo-
rate the process physics of mold filling and cure and thus allow composite process design
engineers to understand the physics and use the simulation as a design tool for prototype
development instead of using trial and error manufacturing approaches. The engineers can
change the process parameters in the simulation and evaluate the influence of the para-
meters on the simulation results in order to search for the optimal material and process
parameters such as locations of the injection gates and vents, injection pressure or flow
rate, cooling rate, resin system, fabric type and fiber volume fraction.
The focus of the next section is to model the impregnation of resin into the fabric
preform, which is usually called the filling stage of LCM, and also develop the non-isothermal
formulation with cure kinetics. The filling stage occurs in all LCM processes with slight
variations. However, in most cases the resin propagates through a stationary fabric preform
which is modeled as a porous medium. The filling model is based on Darcy's law which was
introduced in Chapter 4.

The objective of all LCM processes is to manufacture a composite part with no regions
that contain voids or dry spots. Most applications, in addition, require a short production
cycle and low manufacturing costs in order to be competitive with other manufacturing
techniques and materials. To achieve these goals, the fabric, the resin system, the tool and
the injection system design should be selected such that the filling and the curing stages
require short cycle times with low rejection rate due to dry spots.

Flow and cure modeling will allow one to control the process parameters and design
the tool accordingly in order to achieve these goals. The process parameters that can be
easily controlled and influence the process are location of the injection gate and vents and
the flow rates or injection pressures to be applied at these locations. For nonisothermal
injections, initial resin temperature and mold temperature will also play an important role.
The curing process, as in an autoclave, is decided by the mold wall temperatures and the
reaction kinetics.
Permeability of the fabric and reaction kinetics will be important constitutive equations
for realistic modeling and simulation of the process and must be characterized as outlined
in Chapter 4.
Since the late 1980s, mathematical models for resin flow through reinforcing porous
preforms and for the resin cure along with simulation codes based on the solution to these
models have been developed. These models have been useful to manufacturing engineers in
coupling tool design and process parameters for efficient manufacturing. In the next two
subsections, we will formulate the flow and the heat transfer and cure models. Many book
chapters have also delineated the details [214, 311, 330, 53].
8.3.5 Resin Flow

As discussed in Chapter 4, Darcy studied liquid flow through a sand column, and put
forth what is now known as the Darcy's law. Darcy's law adequately models most LCM
applications in which the Reynolds number is small. This allows us to ignore the inertial
forces and assume a quasi steady state process. The reinforcing fabric preform within the
mold cavity is considered as porous medium, and the relationship between the resin pressure
and its average velocity is given as follows [337, 338]:
u = -— - V P (8.32)
V
where u is the volume averaged Darcy velocity, /J, is the viscosity of the fluid, VP is the
pressure gradient, and K is the permeability tensor of the preform. In expanded form,
Darcy's law can be rewritten as
ux\ f Kxx Kxy Kxz \ f dP/dx

= — I Kyx Kyy Kyz dP/dy | , (8.33)
Kzx Kzy Kzz ) \ dP/dz
where uxi uy and uz are the resin velocity components and Ktj are the permeability tensor
components. The details on measurement and prediction of the permeability components
were discussed in Chapters 4 and 5. Variations of RTM process such as SCRIMP involve
three-dimensional resin flow, as the high permeability distribution medium placed on top
of the preform creates a large transverse gradient flow through the thickness as shown in
Figure 8.28. However, resin flow in most LCM applications can be approximated by two-
dimensional flow because the transverse flow in the thickness direction is only of the order
of a few thicknesses as seen from the example in Chapter 5 and the in-plane dimensions
are usually two to three orders of magnitude larger than the thickness. Approximation
of three dimensional geometry with two dimensional flow brings about significant savings
in computational time and reduces the number of material parameters one must measure
or calculate. By ignoring the flow in the thickness direction, the two-dimensional form of

Equation (8.33) can be re-written as
UT. \ L I KTX Kxy ] I 0^/dX

(
dP/dy J ' '
where ux and uy are Darcy velocities averaged through the preform thickness. This assump-
tion is a very good one as long as in-plane permeabilities of the preforms that are stacked in
the thickness direction are about the same order of magnitude. Note that in SCRIMP, the
permeability of the distribution medium may be two to three orders of magnitude larger
than the preform permeability in the inplane direction; therefore, the two-dimensional as-
sumption is not suitable. Thus, for this process one has to be ready to accept a larger error
in the calculations or resort to a fully three-dimensional flow model. The computational
time for the three-dimensional model would increase by an order of magnitude and one
would require data regarding the transverse permeability of the preform.
In most LCM processes there is insignificant transverse flow; hence, they lend themselves
to two dimensional flow in the plane of the preform. Hence we will restrict ourselves to
discussing the solution of the mathematical model that will be based on a two-dimensional
case for simplicity. The extension to three dimensions is straightforward and does not
involve any conceptual problem.
The equation of mass conservation is obtained by the divergence of velocity as
TT- (ux] + -^- (uy) = 0. (8.35)
We also assume here that the tows impregnate at the same rate as the space in between the
tows. Substitution of the velocity terms from Equation (8.34) in terms of resin pressure P
yields the following second order partial differential equation for the resin flow:
d (Kxx dP\ d (Kxy dP\ d (Kyx dP\ d (Kyy dP\
=U
"~~
fj, ~3~~
ox / + «~ «~~ ) + a~
ox \ ^ ay ] ay \ fj, ~a~
ox)) + ay
a~
\ p, ~x~
ay) ' (8.35J
This governing equation is solved to calculate the resin pressure in the resin domain that
has a moving free surface. The solution domain changes continuously. However because
of the "quasi-steady state" assumption, one solves for the pressure in the resin occupied
domain at that instant in time. For open mold processes such as VARTM and SCRIMP,
there is a dynamic distribution of pressure between the preform and the resin which may
change the fiber volume fraction and the permeability due to the presence of the resin just
as depicted conceptually in Figure 8.5 for autoclave processing. More details on this can be
found in [339, 340, 341, 342].
With known material parameters of viscosity and permeability, which may vary with
position, this governing differential equation with boundary conditions along the boundary
of the resin domain has a unique solution. The boundary conditions are written for three
segments of the boundary: (i) at injection gate(s), (ii) on the free surface (flow front), and
(iii) along the mold wall. Usually, the injection system will inject the resin into the mold
under constant pressure or constant flow rate:
P = -Rnj (8.37a)
or
A(-— -VPV n = - Q i n j (8.37b)

where P;nj and Q-mj are the injection pressure and flow rate, respectively, and A is the
injection surface area with an outward normal vector n. Some injection equipment allows
the users to vary the value of P;nj or Q;nj during the same injection. This translates into the
boundary conditions as replacing Pjnj by Pmj(*) and Q-mj by Q-m](t}. This does not influence
the solution technique as one solves the steady state problem for the pressure at each time
interval. The free resin front may be at the ambient pressure, which is atmospheric or
vacuum pressure depending on whether it is the RTM or VARTM process:
PS = or, Pe = 0 (8.38)
where Pg and Pvent are the flow front pressure and vent pressure, respectively. Along the
in-plane mold wall boundary, the normal velocity component of velocity should be zero if
there is no resin leakage:
^ dP „ dP
un = — Knn— + Knt— = 0, (8.39)
an at
where n and t denote the directions normal and tangential to the mold wall, respectively.
These three types of boundary conditions are illustrated in Figure 8.30.
u.n=o
Gate
P-P
or _ I")
(u.n)A=-Q
inj
Vent
Impermeable mold edge
Fluid flow front
Figure 8.30: Boundary conditions for resin flow in a mold.
It is possible that due to the presence of inserts or multiple gates, multiple resin fronts
may result. When these fronts meet and are not linked to any vent, the air that they
displace gets entrapped in the regions encompassed by the resin flow fronts. For such cases,
the boundary condition given in Equation (8.38) can be modified to include the increase in
the flow front pressure due to the increase in the void pressure. The entrapped air may be
assumed to behave as an ideal gas satisfying
•'void ' void
= constant (8.40)
'void
where Pvoidi ^void and Vvoid are the pressure, temperature and volume of the air enclosed
[343]. However, this would require one to keep track of the void created by merging flow
fronts and calculate its volume at each instant of filling. In reality some of this air will

dissolve in the resin, reducing the void pressure. To model this phenomenon, one may have
to include a mass diffusion equation at the interface of the resin and the air and characterize
the diffusion coefficient. As this is usually not a significant factor in changing the flow front
pattern, most modelers ignore this issue and assume that all air will dissolve in the resin
and use Equation (8.38).
For preforms in which the fiber bundles impregnate at a slower rate than the flow in
between the preforms as shown in Figure 8.31, one can model this effect by introducing a
sink term in the governing equation.
Unsaturated fiber bundle

Resin
Figure 8.31: Fiber tows or bundles are impregnated much more slowly than the regions in
between the fiber tows.
In order to model this phenomenon, a sink term is added to the mass conservation
equation (see Equation (3.10) in Chapter 3): V - U = — s. Or in expanded form, Equation
(8.36) is replaced with the following:
_ KxxdP\ | d K^dp_\ K*-yx
VX8P\ . 8 (K _
= S. (8.41)
— )+ —
dx î dx J dx dy J dy dy)
Here, s is the rate at which the fluid is impregnating inside the fiber tows, and should .be
proportional to the permeability of the fiber tows. For typical LCM fabrics, individual tow
permeability is usually much lower than the overall fabric permeability. Besides the tow
permeability, the value of s is also dependent on pressure outside the tows, the geometry
of the tows and the density of these tows. For a circular tow, s can be derived as follows
[344, 345, 346, 347]:
s = (8.42)
-1 'la
where
dra Kit(P0 + Pc-
(8.43)
dt • O ln
Here, PQ, Pc, and Pvac are the free surface, capillary and vacuum pressures, respectively, €j
is the porosity of the inner region (intratow), r/a is the microfront radius inside the tow,
7*i0 and r-2a are the tow and the cell (the circular computational domain with the tow and
surrounding air channel) radii, Kit is the fiber tow permeability (see Figure 8.32).

\
Fiber Tow
Figure 8.32: Parameters to model the sink effect during impregnation with resin of fiber
tows of permeability, KH.
Thus one would have to solve Equation 8.36 and 8.41 simultaneously to solve for the
macro flow front and the saturation of each tow as the mold filling proceeds. This usually
will modify the pressure profile under constant injection conditions [348, 349].
Example 8.6: Influence of Constant Sink on Injection Profile in One-Dimensional

Flow
Consider one dimensional flow in a preform.
(a)When one injects resin under a constant flow rate, one would expect to measure a
linear rise in the pressure with time at the injection location. This is in accordance with
Darcy's law and the assumption that the preform region that consists of spaces in between
the fiber tows and the fiber tows saturate instantly and at the same time (single scale
preforms). Find the permeability of this single scale preform in the flow direction using the
information of the injection pressure that one can gather with time.
(b) Now, assume that the preform is a dual scale preform, in which the spaces between
the fiber tows saturate instantly but the fiber tows continue to absorb resin at a constant
rate even after the flow front has gone past it. How would you expect the pressure curve to
behave if the resin is injected under constant flow rate conditions?
Solution
(a) In Chapter 4, the relation between the permeability of a single scale preform and the
injection pressure was derived in detail under the conditions when resin is injected at con-
stant flow rate in one-dimensional flow. We will rewrite the final equations for completeness
of this problem:
t. (8.44)
Thus,
pM SQ\2
Kxx = d p (—) • (8.45)

Here Q is the flow rate, w and h are the preform width and thickness, <p (= 1 — Vj) is the
porosity of the preform, —^- is time derivative of the injection pressure which is evaluated
by using experimental data. If the fiber tows are saturated at the same time as the space
in between the tows, then the injection pressure P;nj will increase linearly with time in
one-dimensional flow (assuming line injection and no racetracking). Hence, experimentally
measured ^nj will be constant and Equation (8.45) will allow one to find Kxx.
(b) If the resin flow is in a fabric that exhibits dual scale, one-dimensional conservation
of mass equation, ^j^- = 0 is replaced with
dux
— —s. (8.46)
dx
Here s corresponds to the sink term due to delayed saturation of fiber bundles coinpared
to the empty spaces between the surrounding fiber tows. If s is a constant as stated in the
problem, one can integrate both sides of Equation (8.46) with respect to x, and apply the
boundary condition at the injection gate, ux(x = 0) = Q/(wh), which then results in the
following expression for the resin velocity as a function of x\
ux = -sx+~. (8.47)
One-dimensional Darcy's law relates the resin velocity also to the pressure gradient through
the resin viscosity and the preform permeability in the flow direction, Kxx
KT.xdP_
ux = -- (8.48)
dx
Equating the two ux's in Equations (8.47) and (8.48) yields dP/dx = -£—(sx — ^). One
can obtain P(x, t) by integrating both sides of this equation with respect to x, and applying
the boundary condition at the injection gate, P(x = 0,t) = Pinj(t)
v (8.49)
' ' Kxx | 2 wh
The boundary condition at the moving resin flow front, x = x/, yields the following:
A4 sxj Qxf
P(x = x f , t ) =0 = (8.50)
~2 wh
assuming that P(x — xj, i) = PVent = 0. One can rewrite Equation (8.50) in order to obtain
a relation between Kxx and other process parameters and variables
QXf(t)
(8.51)
Pinj(t) [ 2 wh
One needs to write x/(t) explicitly in order to use Equation (8.51). This is shown below
*/(*) =

o
= - ! \-sxf(t') + -VI dt' from Equation (8.47)

9 Jo L w/ij
Xf(t'}dt'. (8.52)
0
Xf(t) appears on both hand sides of Equation (8.52). In order to write Xf(i) explicitly, the
Laplace transform of Equation (8.52) will be taken as follows:
-Xf(p] = - (8.53)
where A = Q/(wh(/)) and B — s/<j) were used for the sake of simplicity. In Equation (8.53),
Xf(p) is the Laplace transform of x/(t), and p is the Laplace variable. Rearranging Equation
(8.53) by using partial functions, one can obtain the following:
(8 54)
'
One can now take the inverse Laplace transform of Equation (8.53) which results in the
following:
B
Q (8.55)
swh
Finally, one can substitute this expression into Equation (8.51)
_ MV /-, -st/4\ 1 /-, ep-st/c/A" (O rp\

J^-xx — 9,9n 77^ I J- — Z I T; \ L ~ \ • (0.00)
Preform permeability Kxx along the flow direction is calculated by substituting injection
pressure at any time (except at t = 0) into Equation (8.56). At t = 0, that expression
is 0/0 and singular. As a good engineering practice, Kxx should be evaluated at several
time values, and an average should be taken due to minor variabilities in s, Kxx, Q, and
racetracking effects. Figure 8.33 illustrates some typical plots of Xf(t) and Pinj(t) with and
without the effect of dual scale flow. In reality, s is not a constant but is coupled to the
flow outside the tows because of the variation in resin pressure. The resulting equations are
nonlinear and require numerical methods to solve them. •

There are many resins such as vinylester that cure at room temperature. Hence it may not
be necessary to model nonisothermal mold filling for such resins. However, these are usually
single component resins in which the second component to initiate the reaction is added.
Hence the cure will initiate with time. The goal in such cases is to fill the mold before the

Figure 8.33: Flow front Xf(t) and injection pressure Pinj(i) as a function of time for three
different values of sink term, s = 0, 0.001, 0.002 and 0.004 s"1. Preform width w = 0.1 m,
thickness h = 0.01 m, porosity <j> = 0.5, permeability Kxx = l*10~ 9 m 2 , resin viscosity
fj, = 0.1 Pa.s, and flow rate Q = 5*10~6 m3 were used in the calculations. As s —> 0, both
Xf(i) and Pj n j(t) become linear with time as one would expect for single scale porous media.

resin cure reaches a value where the viscosity of the resin starts to increase dramatically.
However, as the resin continues to cure from the initiation of the process as demonstrated
by Figure 8.34, the resin entering the mold will be at different degrees of cure; thus, the
viscosities will be different and will be functions of time. Usually, this effect is ignored as the
degree of cure during mold filling is minimal, and the increase in viscosity is usually of the
order of the noise in the system and assumptions made in the model. Hence unless we have
a strong reason to believe that this is a primary influence, one can safely ignore the cure
during the filling and focus on isothermal filling. The cure can then be separately handled
in a similar form to autoclave cure except the boundary conditions may be different.
a contour levels
Figure 8.34: Schematic of resin cure during the mold filling stage, a is the degree of cure
[330].
For resins that need to be heated to initiate cure, usually warm or cold resin is injected
into a hot mold containing heated preforms. In such cases the heat is transfered from the
mold and the preforms to the resin as the resin flows into the mold. As the resin temperature
increases, the resin viscosity decreases. However, higher temperature of the resin will initiate
and accelerate its cure and as the degree of cure increases, the resin viscosity will increase.
Usually the viscosity due to the cure can increase by orders of magnitude whereas the drop
in viscosity due to increase in temperature for thermosets is only a few percent. To model
the change in the viscosity due to temperature and cure kinetics in the flow equation, one
must also characterize the viscosity dependence on these functions as discussed in Chapter
4.
The temperature and degree of cure will be nonuniform in the mold, as the heat dis-
tribution is nonuniform due to convection of the resin and also due to conduction of the
heat through the mold walls and the preform. Also, if one uses a multi-component injection
system then the initial concentration of the cataylst may be different for different regions in
the resin, initiating different rates of cure. The important processing step here is to design
heating systems to prevent early gelation of resin and hence incomplete filling stage. For
such situations, one would find the nonisothermal resin flow model along with the energy

equation and cure kinetics equation very useful. The coupling between energy, flow and
cure kinetics equations is through the cure and temperature dependent viscosity model.
One could model heat transfer through porous media using different approaches and
models [350]. One could either use a two-phase model in which one solves for the energy
equation for fibers and resin separately and uses constitutive equations to express the energy
transfer between the two phases or one could use the simpler local equilibrium model. In
this model, one focuses on the average temperature of a control volume that has the resin
and the fibers in them and assumes that the resin instantly equilibrates to the average tem-
perature as soon as it covers the resin [351]. This model is commonly used as experimental
results support the assumption especially for low Reynolds number flows. Thus, the local
equilibrium model will be discussed here.
The energy equation for this model is given below [352]
[(1 - Vf)prcPr + Vfpfcp}] ^ +PrcPru • VT = V • [(ke + KD) • VT] + (1 - Vf}s + /m - K'1 • u

(8.57)
where T is the average temperature of resin and fabric preform, t is the time, p and cp are
the density and heat capacity. The subscripts r and / denote the resin and fabric preform,
respectively. Vf is the fiber volume fraction, s is the source term due to curing, ke is effective
conductivity which is expressed in terms of fiber and resin thermal conductivities Kr and
Kf [350]. K£> is called the heat dispersion coefficient and quantifies the differences in heat
dispersion not accounted for by the convection of heat. In accordance with Darcy's Law,
it is assumed that the average velocity is in the flow direction and this is sufficent to find
the pressure distribution. Figure 8.35 shows that the local velocity vector is in different
directions, and convects the heat in other directions in addition to the flow direction. This
influence is lumped in the second term on the right-hand side of the above equation, in
which the dispersion is expressed as a conductive effect by K£> • VT.
Figure 8.35: Schematic of heat dispersion effect; the figure on the left (a) depicts the resin
impregnation directions across the fibers. The figure on the right (b) due to the assumption
of Darcy's law can account for convection only in the flow direction. The difference in heat
convection effect is expressed by a dispersion term.
A dimensional analysis shows that, for mold filling applications with a small Brinkman
number, viscous dissipation is negligible. Further, for thin shell-like domains, heat con-

duction in the in-plane directions and heat convection in the transverse direction are also
negligible [352]. However, heat dispersion may be significant [353, 354]. It is difficult to
evaluate the heat dispersion term K£> [355, 356], and it is usually neglected in the models
[357]. K£> is found to be proportional to the Peclet number. Hence the higher the velocity
of the flow, the larger will be the effect [354, 355].
The first term on the left hand side of Equation (8.57) is the change in the internal
energy of the resin and the preform; the second term is due to fluid convection due to
volume-averaged Darcy's velocity. Even if flow was considered two-dimensional, due to the
presence of the first term on the right-hand side of Equation (8.57), the energy equation is
three-dimensional. One can ignore the through thickness flow, but the dominant conduction
mode is through the thickness direction; hence, one may ignore the heat conduction in the
plane but must retain the conduction through the thickness.
Equation (8.57) is a second order elliptic partial differential equation in spatial coordi-
nates and first order in time. In order to solve it, boundary conditions on the entire spatial
domain and an initial condition for temperature are needed. In some applications, the mold
temperature is assumed to stay constant during the filling. However, this is not a very
realistic assumption. Instead, a quasi-steady state approach yields the following boundary
condition in the thickness direction [241, 330]:
dT
- + Cbc(T - =0 (8.58)
where n is the normal in the outward direction to the mold wall, and the boundary condition
constant C&c is written as follows:
l
3.59)
kt l/hh + l/hri
where hh and hm are the heat transfer coefficients between the heating fluid and the pipe,
and between the mold and resin, respectively, km is the thermal conductivity of mold
material, kt is the conductivity of the composite in the transverse direction, a is the distance
between the mold wall and the heating pipe, and T^ is the temperature of the heating fluid
as shown schematically in Figure 8.36.
heating
pipe
top mold a z
platen at
Resin o o OAP 0*0 o
flow ~~* o o o o o
Figure 8.36: Boundary condition at the mold wall across the thickness of a composite [54].
The other boundary condition is usually at the injection gate where the temperature of
the resin is usually prescribed. At the flow front, an energy balance allows one to account
for the convection into the unsaturated region as shown in Figure 8.37.

flow front,at time t + At
flow front at time t
T0, unsaturated
preform
temperature
fArea^:!™"1"""""""1
m's IB m
î^ mi»
^^
fluid filled preform
Figure 8.37: Energy balance at the flow front [353].
The s term in the energy equation models the heat released by the exothermic reaction
when the resin molecules are cross-linking as the resin cures. Hence one needs a constitutive
equation that can characterize cure and also provide the rate at which it generates energy.
Example 8.7: Cold Resin Injected into a Hot Mold [355]

Consider flow of a resin in the x direction. If cold resin continues to be injected into the
hot mold even after the preform is saturated and allowed to exit at one or more vents,
the temperature distribution in the mold cavity will reach a steady state. Even if one
does not flush the mold in this way, most of the resin near the gate will reach the steady
state. Assuming the steady state, find approximately the temperature distribution for slow,
intermediate and fast resin injections. What dimensionless number governs this flow?
Solution
The energy equation, Equation (8.57), for steady state reduces to
d(T)
= k, (8.60)
dx
with boundary conditions
(T) = Tin at x = 0 (8.61)

(T) = T0 at z = ±h. (8.62)
Here (pcpjr is the heat capacity of the resin, (u) is the Darcy's velocity in the flow
direction (x direction) and (T) is the average temperature at a given location. Here kzz is
the conductivity of the medium in the thickness direction. Also as thickness is much less
than the length, one can ignore the conduction in the x direction.
When the filling speed is slow, the conduction across the thickness will dominate. At
steady state, the mold wall temperature will diffuse through the thickness, and resin and
preform will reach the mold wall temperature. The only exception will be the injection gate
region of width h, where the temperature changes from T{n (from inlet resin temperature
to T0) as sketched in Figure 8.38 [355, 358].

Figure 8.38: Schematic of steady-state temperature distribution at low injection speeds
(Gz « 1). At steady state, T = T0 in the shaded region. In the central white region, T
changes between Tin and T0.
The dimensionless number that governs the ratio of the convection in the inflow direction
and conduction through the thickness direction is the Graetz number, Gz:
(u i "-ZZ
Gz = where azz = 3.63)
azzL
This can be obtained by nondimensionalization of Equation 8.60 by using the following
nondimensional variables:
(T) - Tin X
XT' - z'-Z (8.64)
T0-Tin ' ~L' h
(pcp}r (u) <90 _ kzz <929

(8.65)
Z d^7 ~~~
h2 (u) (99 _ d2Q
(8.66)
azzL a^7 ~ ~
Z d& _
~ (8.67)
Thus when Gz « 1, conduction dominates as shown in Figure 8.38. One can easily
solve Equation (8.66), by introducing a new variable
(8.68)
where z is the distance from the wall towards the center in the thickness direction. This
allows us to convert a partial differential equation into an ordinary differential equation by
similarity method and the solution can be easily obtained:
(T) - Ti
= l-erf(0 (8.69)

Figure 8.39: Schematic of steady-state temperature distribution at high injection speeds
(Gz » 1). At steady state, T — Tin in the white unshaded region and changes from T0 to
Tin hi the shaded boundary layer.
for Gz » 1. Here erf represents the Gaussian error funtion. Thus for Gz » 1 (large
filling speeds), the thermal boundary layer increases with distance from the entrance as
shown in Figure 8.39. The thickness of this boundary layer grows with the square root of
the distance from the mold entrance and is given by
(8.70)
Thus at high Gz » I , 6 « h. At intermediate speeds when Gz ~ 1, 5 ~ h when x — L.
Resin Cure Models

There are many empirical models for resin cure as discussed in Chapter 4. Models for
various resins are also presented in [241, 351, 359, 360]. One can assume that the heat
generation due to the cure reaction, s is proportional to the rate of the reaction Ra
s—
where Ea is the heat of reaction. Ra is assumed to be a function of temperature T, and

degree of cure a. For example
Ra = (fc1 + /c 2 a m )(l-tt) n (8.72)
where
(8.73a)
(8.73b)
where R is the universal gas constant. The resin material constants m, n, AI, A%, E\ and
E-2 are measured experimentally, as discussed to some extent in Chapter 4.
The cure convects with the resin as it flows to occupy the mold; hence one can express
the conservation of cure in mathematical form as follows:

„ da da da ,„ „,.
Ra = -zr + ux — + uyy—. 8.74
dt dx dy
The right-hand side of Equation 8.74 represents the substantial derivative of the degree
of cure and must be solved along with the flow model, the energy equation and the cure
kinetics model. This system of equations is coupled through the viscosity dependence on
the cure kinetics and temperature of the resin.
Temperature and Cure Dependent Viscosity

There are many empirical models available for viscosity. For thermoset resins that are
undergoing nonisothermal process and cure, chemorheological models best describe the
change in viscosity both as a function of the temperature and degree of cure [214, 330]
(8.75)
iwhere the activation energy E^ and the constant A^ are given as follows:
E^ = a + ba (8.76a)
(8.76b)
where the constants a, 6, ao and bo are determined experimentally.

The temperature changes in the thickness direction as well as the in-plane directions.
Hence, temperature dependent viscosity will change in all three directions. However as the
flow is modeled as two-dimensional, one must average the viscosity through the thickness
as follows:
1 1 rh I
4 = ± / -dz (8.77)
p h JQ n
where h is the mold cavity thickness and ft is the local in-plane viscosity.
The isothermal flow model of LCM processes can be solved analytically for simple one
dimensional flows with constant viscosity, permeability, fiber volume fraction and thick-
ness. However, most practical situations where prediction will be useful involve complicated
geometry with inserts and nonuniform thickness of the part, varying permeability across the
region and multiple injection locations. Therefore, one has to resort to numerical solutions
to address the mold filling process in LCM. In the next section, we briefly introduce the
approach usually followed to accomplish this.
8.3.7 Numerical Simulation of Resin Flow in LCM Processes

A numerical simulation of the mold filling process can be developed by discretizing the
governing partial differential equation with numerical methods such as finite difference,
finite element or boundary elements. The advantage of numerical simulation is that it
will help the process or manufacturing engineer to understand the flow behavior inside the
mold, especially when the geometry of the part being manufactured is complex and has
permeability and fiber volume fraction variations. This understanding can improve the tool
design and placement of gates and vents in locations that help saturate the preform without
any dry spots.
As the process engineer needs to run simulations on complex models multiple times with
different choices for gates, it is important that the simulation is computationally efficient.

One way to make moving boundary problems computationally efficient is to use a simplifi-
cation of the resin flow model to in-plane two dimensions from three dimensions and use a
finite element/control volume (FE/CV) approach. The (FE/CV) approach does not require
remeshing at each time step. It is based on the marker and cell method [361, 258, 362].
First, the part geometry is discretized as a thin shell by using triangular and/or quadri-
lateral elements. This allows one to model geometries in three-dimensional space as shown
in Figure 8.40.
Figure 8.40: Two-dimensional mold geometry discretized in three-dimensional space with

two-dimensional finite elements.
Material properties (permeability, fiber volume fraction and part thickness) can be as-
signed for each element individually, allowing for nonuniform material properties and vari-
able thickness of the part. A linear pressure profile is assumed between the nodes of an
element
Pe = îNiPi (8.78)
t=i
where n is the number of nodes of the element e, Pe is the pressure within the element e,
Pi is the unknown nodal pressure and Ni is the interpolation function. The Galerkin finite
element method can be used to convert the partial differential equation into a system of
algebraic equations that minimize the error at the nodes and can be expressed as a linear
system of equations as follows:
[[«"]] [P] = I/I (8-79)
where the components of the element stiffness matrix are given by
Kxx dN, dNt Kyy ONj dN, Kxy dNj dNt Kxy dNs 8N, \
o Q 1 Q Q 1 Q Q 1 O O
M ox ox fj, ay ay n ox ay ^ ay ox J «"• (O.OUJ
This set of governing equations can be solved at any instant during the filling process. The
zth component of [[<5e]][P] vector is the amount of mass generated per unit time at the

ith node. Hence, the forcing vector [/] on the right-hand side of Equation (8.79) has all
zeros except at rows corresponding to the injection nodes. The value of the forcing vector
at that row is related to the flow rate or pressure boundary condition specified. After
pressures at the nodes are calculated by solving the set of algebraic equations described by
Equation (8.79), the next step is to advance the flow front. The control volume approach
to accomplish this is as follows: first, the mold geometry is divided into control volumes, by
associating one with every node. The control volume is bounded by the element centroids
and the element mid-sides. Next, the flow rate between the control volumes is calculated
by multiplying the average velocity with the area connecting the two control volumes. For
example, the equation for the flow rate from the control volume associated with node i to
the control volume associated with node j, qij is
qij = n • K ds 3.81)
where Sij is the boundary between the two control volumes, h is the mold gap thickness at
the boundary, and n is the normal vector to the boundary lying in the plane of the preform.
Nodal fill factors are used to track the moving flow front. The fill factor for each node is
defined as the fraction of its control volume occupied by the fluid as shown in Figure 8.41
[337, 214, 330].
Finite element mesh

Control volumes!,,, .
Fil I ed area of th §1
Figure 8.41: Nodal fill factors in FE/CV approach to mold filling.

Pressures are calculated at full nodes only and empty nodes are ignored. Partially filled
nodes are assumed to lie close to the flow front and the flow front boundary condition is
applied there. The flow front is advanced at each time step by updating the fill factors
of control volumes, using the flow rates between the connecting nodes, thus rigorously
accounting for mass balance. With this technique, one can fill thin cavities with highly
complex geometries in three-dimensional space and also account for the variation in the gap
height of the part.
Each control volume used for the pressure analysis is rediscretized in the transverse z
direction to generate a three-dimensional mesh for temperature and cure analysis. Equations
(8.57) and (8.74) are solved by a method [363, 330] which is explicit in time t and the x-y
plane but implicit in the z direction. The method does not require an excessive amount of
memory considering the number of nodes in the third dimension, but the downside of the

method is that it is only conditionally stable. If the time step is not choosen to be small
enough, the numerical solutions will not converge. Since the source term in the energy
equation is a nonlinear function of temperature, an iterative solution method is applied to
evaluate the temperature distribution. The calculated temperature is then used to estimate
the degree of cure. After the temperature and degree of cure are known within the three-
dimensional resin domain, the averaged (or effective) resin viscosity can be calculated using
Equations (8.75) and (8.77).
There are two disadvantages in conducting numerical simulations nonisothermally. First,
the computational efficiency and speed go down drastically as one has to solve energy and
flow equations simultaneously and due to an increase in the number of nodes. Research in
simplifying the nonisothermal analysis has reduced the time but still requires over two to
three orders of magnitude of CPU time than solving the isothermal problem [330]. Secondly,
more material parameters such as the dispersion coefficient, thermal conductivities, and
resin cure kinetics are needed to obtain the results. There have not been many studies that
have conducted rigorous experimental verification of nonisothermal simulations; hence, the
sensitivity and accuracy of these models is untested. Further research in this area is essential
if one expects to cure the resins during mold filling in an attempt to reduce cycle times.
For high-temperature resins, a good compromise would be to fill the mold under isother-
mal conditions and then invoke the cure kinetics. Numerically, it is very efficient as one
does not have to deal with convective-diffusion problems which are notoriously difficult in
converging and giving the correct result.
8.4 Filament Winding of Thermosetting Matrix Composites

8.4.1 Introduction
In thermoplastic filament winding, more commonly known as thermoplastic tape layup,
a tape of continuous fibers is preimpregnated with thermoplastic resin. In this process, a
relatively thin tape is consolidated on a substrate under the application of heat and pressure
(Figure 8.42).
Consolidation
Composite Substrate
Figure 8.42: In-situ thermoplastic tape layup process.

In most cases, the feed tape, the heater (gas, induction, laser, etc.) and the consolidation
rollers/shoes are traversed over the substrate at a predefined path and velocity.
Thermoset filament winding is a process of winding strands of reinforcement fibers em-
bedded in a thermoset resin matrix onto a tool (mandrel), then curing the resin and remov-
ing the mandrel. In simple terms, a continuous strand (rope-like) reinforcement which may

be a glass or a carbon strand is saturated in a resin bath, then wound over the mandrel like
a thread over a spool by going across from one end to another and back. This winding is
repeated until the desired thickness is achieved. Figure 8.43 illustrates the process.
Figure 8.43: Thermoset filament winding process [59].

One can precisely place the fibers on the mandrel as it is a machine controlled process
and hence can be accomplished at high speed. The major development costs are the filament
winding machine and the mandrel. However as the process is automated, the labor cost
is low and repeatibility is high. High-speed, precise positioning of fibers in predescribed
patterns and automation are the attractive features of the filament winding method for
manufacturing composites. The fiber strands are either in the form of continuous resin-
impregnated rovings or tows that are wound over a rotating male mandrel. The mandrel
may be cylindrical, spherical, rectangular, or any shape that does not have a concave
curvature. The reinforcement fiber may be wound either in adjacent bands or in repeating
bands, which eventually may cover the entire mandrel surface. The winding tension, fiber
angle, resin content and fiber material are important process and material variables that can
be varied in each layer of reinforcement until the desired wall thickness is obtained. A good
filament winding process model can enable the designer to custom engineer components by
placing the exact, mechanical characteristics where needed within the part and allow the
design to be optimized for weight, stress concentrations and fatigue.
The thermoset filament winding process is primarily used for the manufacture of cylin-
drical and hollow composite parts. Figure 8.44 shows the mandrel and the composite part
being wound. The tension in the filament can usually provide the consolidation pressure
for fiber motion and for the saturated fiber band to percolate the resin through it. The
composite along with the mandrel may be cured in an autoclave if the curing needs to
initiate at a higher temperature.
Some of the key benefits of the process include machine controlled fiber placement,
ease of automation, and the potential for high fiber volumes. Accurate, repeatable fiber
placement from layer to layer and from part to part are other attractive features from
the viewpoint of manufacturing. The capability to use continuous fibers over the length
of a component area (no joints or splices) and ability to easily orient fibers in the load
direction are other useful properties of filament winding that can influence the use of this
process in applications that require it. Complex shapes can first be wound as a preform
and then molded to near net shape using filament winding. Filament winding also allows

ompos to
F-.ber Band
Fiber)
Figure 8.44: Schematic of filament winding process [59].
for customization of properties such as torsional stiffness, axial stiffness, tensile strength,
proportional elastic limit, hardness, abrasion and wear resistance.
During this process, the following physical phenomena occur:
• Thermochemical reaction and heat transfer: The resin cures due to the cross-linking
exothermic reactions of the thermoset matrix, and the heat generated is conducted to
the ambient.
• Resin Slippage: Since there is uncured resin between the fibers, the fibers slip from
their original position under tension.
• Void Formation: Voids are formed due to the air trapped between the bands of fibers.
• Thermal expansion effects and the development of stresses and strains: The mandrel
and the composite expand due to the changes in temperature which creates thermal
stresses and strains due to mismatch in thermal expansion. This adds to the stresses
developed due to the fiber tension.

For filament winding of thermosets, process models have been developed to (i) calculate
fiber motion and tension in the fiber filaments during winding, (ii) predict temperatures and
cure during winding and in the autoclave, (iii) estimate void growth and final fiber volume
fraction, and (iv) evaluate residual stresses. Springer and co-workers [364, 365, 366, 367]
have developed extensive formulations that include thermochemical, fiber motion, stress,
and void submodels. Their models have been experimentally validated for prepreg thermoset
composite materials.
The thermochemical submodel provides temperature, viscosity and degree of cure during
winding and when the part is cured in the autoclave. The inputs needed for this model are
thermophysical properties, constitutive equations that describe the cure behavior and the
viscosity change with temperature and cure along with the boundary and initial conditions.
The fiber motion or fiber seepage submodel predicts the fiber position and the fiber volume
fraction within the cylinder along with fiber tension during the winding process.

The stress submodel calculates the stresses and strains experienced by the composite.
Fiber tension, thermal expansion or contraction and chemical changes cause the stress and
strain development. Usually, the stresses and strains due to each of the causes is calculated
separately and then added to predict the total strain and stress in the composite. The
details on this submodel may be found in [364, 365, 366, 367].
Voids may form during winding when the resin percolates through the fibers. The voids
may also be introduced in the prepreg that is wound over the cylinder and modest amount
of flow during the winding may not be able to flush it out. Void nucleation is not modeled,
only changes in void size is considered by Springer et al. [364, 365, 366, 367]. All voids
are considered to be spherical and contain a vapor of known composition (usually initial
concentration of water and air). The volume of the void is considered to change because
vapor is transported in and out of the void across the void composite interface and pressure
differential between the resin pressure outside and the vapor pressure inside the void. Figure
8.45 shows the interrelationships of the various filament winding submodels. They have been
reproduced from reference [368].
Geometry Material Properties Processing Conditions

I
Thermochemical Stress-Strain Submodel:

MODEL INPUTS
Submodel Winding and Thermal
GEOMETRY
cylinder dimensions (H, T, a) Loads
(a, E, r)
tow dimensions
layup
MATERIAL TS Wind OUTPUTS
chemical kinetics Fiber Motion (functions of position and time)
viscosity Submodel H resin viscosity
mandrel mechanical properties T composite temperature
(F, u.)
mandrel thermal properties a degree of cure
composite mechanical properties F fiber tension
composite thermal properties u fiber position
a stresses within cylinder
PROCESSING
surface temperatures Void Submodel E strains within cylinder
hold time between layers d d void diameter
tow tension r composite radius
time to wind a layer v fiber volume fraction
Figure 8.45: Interrelationship of submodels for filament winding with thermosetting matrix
materials
In this section, we will consider only the thermochemical reaction and the fiber motion
or the resin seepage submodel. These two models are coupled via the resin viscosity, which
is temperature and cure dependent. It is assumed that the winding of the mandrel is in-
stantaneous. The modeling approach will be described with the use of a simple example.
Significant work in the modeling of the filament winding process for thermosetting matrix
composites has been undertaken by [368], and the models have been verified with experi-
ments. The following process submodels are adopted from their work. The goal here is to
introduce modeling and improve the understanding of the modeling process and not solve
comprehensively for all the details.

Thermochemical Model
In this process, heat transfer and cure kinetics play an important role, whereas resin flow
is considered to be negligible. Hence, one can focus on the energy transport and ignore
resin motion. Prom the energy balance equation introduced in chapter 3, we can simplify
the equation by neglecting the convective terms and ignoring the variations in the azimuth
direction due to cylindrical symmetry. So, terms that are retained are an increase in the
internal energy of the composite due to the increase in the temperature on the left-hand
side which is a result of the energy generated by the curing of the resin (last term on the
right-hand side of the equation). Part of the heat is lost to the ambient by conduction in
the radial as well as axial directions (first and second terms on the right-hand side)
3T 1 d dT d dT
- 7T
•(8.82)
r <9r
where krr and kzz are the composite conductivities in the radial and axial directions, re-
spectively, p and C are the density and heat capacities of the composite. One could use
simple rule of mixtures to find these values knowing the density and the heat capacities for
the resin and the fibers and the fiber volume fraction. Hu is the heat of reaction for the
resin, da/dt is the rate of cure, where a is the degree of cure. One would need an equation
that can describe the cure-kinetic reaction. The cure-kinetic reaction is usually a function
of temperature. Hence the cure kinetics are coupled with the energy equation and one must
solve them simultaneously
— = rEV(a, HP +\
1 , t). fQ Q'3\
(a.od)
Hence our independent variables are t, r and z and our dependent variables are a and T.
The initial conditions for cure and temperature need to be specified (usually a is zero at
t = 0). As the temperature equation is a partial differential equation, boundary conditions
are required to solve for the temperature. Temperature, heat flux or a convective boundary
condition is usually specified on the composite outside diameter and on the mandrel inner
diameter. In Figure 8.46, constant temperature boundary conditions are applied in the
radial and axial directions. Here hm and h are the thickness of the mandrel and the
composite respectively.
R
mo R
mil
z=0 z=L
Figure 8.46: Thermal boundary conditions of constant temperature.

Fiber Motion or Resin Seepage Submodel
Darcy's law as applied to the fiber governs the movement of fiber through the resin. In liquid
molding processes, we considered the fiber network stationary and the resin moves relative
to the fiber network because of the pressure gradient created. In autoclave processing, the
resin was made to bleed across a network of fibers that was being compressed. In this
process, the fibers or the porous network formed by the fibers are forced through the resin
due to the applied tension as seen in Figure 8.47.
Fiber
Sheet
Resin
Figure 8.47: Schematic of fiber motion through the resin due to the applied tension.
Flow of the resin, expansion of the mandrel and expansion of the composite affect the
fiber position. However, in the fiber motion model we will consider fiber movement only
due to the flow of the resin. As seen in Figure 8.47, each composite layer is idealized as a
fiber sheet surrounded by thermoset resin. The motion of the fibers can be denoted by Xf.
Then, Darcy's law gives the rate at which the fibers move relative to the resin
dxs KrrdP
= (8 84)
-dT -—^' '
This model assumes that the resin flows transverse to the fibers in the radial direction.
Another critical assumption is that the resin carries the entire load and none is carried by
the fibers, unlike in autoclave processing. The consolidation pressure is provided by the
component of the tension in the filament over the distance r/, as recast below:
*^sin'*00.. (8.85)
dt [i rf
Here dxf/dt is the rate of radial movement of the fibers, <jf is the tension in the fiber,
Krr is the permeability of the fibrous network in the radial direction, since the fibers are
moving through and relative to the resin of viscosity, fj,. 3>0 is the angle at which the
fiber is wound onto the mandrel and r/ is the radius of the fiber layer. The fiber motion
submodel is coupled with the thermochemical submodel through the resin viscosity, fj,, which
is temperature dependent
). (8.86)
The radius of the fiber layer, r / , is given by the following relation:
rf = r°f + xf (8.87)

where r9 is the initial radius and Xf is the displacement of the fiber layer. Under this
displacement, the fiber deforms and the fiber tension changes. The equation governing the
rate at which the tension, <jf, is changing and is given by:
duf/ EfKrrs'm43>0 ,„ „„,

~di ~ ~ M r} "' ^ '
where Ef is the elongational modulus of the fiber material. Hence we have a set of coupled
nonlinear equations for the fiber displacement and the fiber tension, which have to be
integrated to obtain the displacement for every layer. The initial conditions for the above
equations are
xf = 0 (8.89)
af = ^ (8.90)
rj = r°f (8.91)
at t = 0. Here F0 is the winding tension and r°, is the initial radius of the fiber layer. We
will conclude this section by demonstrating the approach to calculate the temperature, cure
kinetic and fiber motion by coupling the thermochemical and the fiber seepage submodels.
Example 8.8: A Cylindrical Composite Part Wound on an Aluminum Mandrel

A sample problem based on the work of Callus et al. [365] is used here for the purposes
of demonstrating the approach to carry out the analysis. A cylindrical composite part is
wound on an aluminum mandrel that is 1/4" thick, 6" outside diameter by using 18 layers
of Fiberite T300/976 (Thornel T-300 fibers/Fiberite 976) prepreg at an angle of 40 degrees,
giving it a thickness of 5/32". Each band of prepreg was wound with tension of 6 Ibf and
has a width of 0.125". After winding, the cylinder is cured in an autoclave and subjected
to a cure cycle that lasts 6 hours. This cure cycle has a ramp section of one hour to 350°F
(177°C) from room temperature, followed by a dwell time of 4 hrs and then a cooling period
of an hour, back to room temperature. The geometry and the cure cycle are illustrated in
Figure 8.48. Describe the approach to solve for fiber tension with time during the curing
process. •
Thermochemical Model Solution

By using the following nondimensional variables,
I — / • •, -y
m* -*- -Mint * ^ *
T
-*• air,max _ 71
• • '
-Mmt 7" '
-^ A/ i _u<~ '-*^composite
^"mandrel A* A / '
^-**'tot
(8.92)
the equations governing the heat transfer and curing reaction in the composite and the
mandrel were nondimensionalized as follows:
ktc l d prVrHu da
dt* pCpbtlfi I r* Or* \ dr*) \ L ) 0(z*}2 frp Tf,—r -^- (8-93)
-

MatersaSs Alum.niu-n {Mandrel) ' 15 24 en
Fee'ite
Bi»B»Siaa»K»™»^«KU^^ VWHUJM Ita.
^" " ^ " ... -">* ' - - - ™*,-«.^. |r<
T * -4OT!*- ,'
177 C ' . ' •;
:
= Cure C^cle
1hr 5 NTS. St«
Figure 8.48: Sample composite part and cure cycle used for the model solution [365].
Using the documented values of the thermal capacity and heat conductivity of the composite
and aluminum, it was found that the time scale of heat conduction in the composite (45
s) was much slower than the conduction time scale in the mandrel. In addition, since the
composite layer is thin, compared to the length of the part, the terms for the conduction in
the z direction can be neglected.
2
£tot „, PCp&tlt __ PrVrHu
fc
T I ^^ ' t>c —
c
7, i P — n /rri rp \) c,Al ^ <"c,composite •
L J k
(8.94)
This leads to the following simplified thermochemical equation in nondimensional form:
dT* 1 d ( *dT*\ Qda

= r - * —1— } +/3—. (8.95)
Q^* f* QT* \ c/7 * / dt*
The cure kinetics of the epoxy resin and the relation for resin viscosity can be recast as
follows:
^=(Kl + K2a1-03) (B - a1'22) (8.96)
= A W «P^*J (8.97)
-=tc~ (8.98)
dt* dt ^ '
: Moo exp f-— + /caV (8.99)
Since the conduction time scale in the mandrel is much smaller than that of the composite,
the conduction in the mandrel can be assumed to be in quasi-steady state and the transients
there can be neglected. In addition, the chief mechanism of heat transfer from the autoclave

to the composite part is the convective heating or cooling. This leads to the following
boundary conditions, where the conductive resistance of the mandrel and the convective
heat resistances between the part and the autoclave atmosphere are used to derive mixed
type of boundary conditions:
T •i r 'j. -'air J- composite, inside , ul. , .

Inside surface, composite: —-=p--- = ~^~^" at r = r-m (o.lUUj
^conv.,in ^cond., mandrel UT
m . _ T"1 . ftrr
L
f~^
, . -i £ ., -'•air -*• composite, out j *~'-
Outside surface, composite: - ----'— = k—, at r — rout/'o -i n-i \
(8.101)
i | '"in, composite \
_ I _ \ nn.mandrel / _ 1
rl
•rt-convl — ~ Ti
i i -t"cona —
-ftcond n
9 ti ' conv2 — «
^-convz i •
in mandrel^ ^^"^niandrel ^^"^"out, composite'^
(8.102)
These boundary conditions can be nondimensionalized to give the following conditions:
71* _ 71* . ., i. flrr*

T •i r -j_ air composite, inside ^ ^^ , * *
Inside surface, composite: —-=j- - — ——- -—- at r = rin
-KConv.,in -Kcond., mandrel '-^'-tot OT
(8.103)
1 1
/^ , • i c -j_
7 air
* _ Tcomposite,
* . out i. f,QT*
"- JJ
Outside surface, composite: - —--- = - —- - j. *
at* r =/o riout
nyi\
(8.104J
-flCOnv.,out Aftot C*r
The initial conditions are given by:
Initial condition: T = Troom, and a = a;nit. (8.105)
The governing PDE may be discretized using finite differences to give the following
scheme:
(1 + 2v + /J,)T?+l* = Tr + (v + fi)2£V* + vT?-i* + /5At* n

• (8-106)
Ai* At*
v =- FT, u = —r^- , V i = 1 . . . r steps and i — 0 . . . t steps v (8.107)
Ar* 2 r*[z]Ar* .
B .V^.
r~\ 1
S.
rpn+1 *
_i Q ^^
-^
^
Mconv. ,in~i~^cond.,mandrel
^ ,
/7^n+l *
J. yy = ^
H-\-Hco
^
d.,mandrel -^ -ttcoiiv.,out
(8.108)
where R — fc/(AttotAr*). The numerical scheme selected to solve this problem is fully
implicit since the explicit scheme has an inherent limitation in time-step size which can
increase the computational time substantially.

Fiber Motion Submodel: Solution
The governing ODEs for the motion of the fiber through the resin, while the resin is curing,
can be integrated using the viscosity data from the thermochemical model to obtain the
following equations for the fiber motion and fiber tension:
2
^ / - C - ^ (8.109)
rnf+1 = r°f + xnf+l (8.111)
Ftension
Initial conditions: x°f = 0, a°f = , r°f = Rf (8.112)
A
f
The discretized thermochemical model can be solved using an iterative solver for the
temperature and the cure rate. The viscosity can be determined from the calculated values
of the temperature and cure. These viscosity values can then be used to solve for the fiber
motion and tension. The fibers tend to move downwards through the resin pool, until the
resin gels and solidifies. As the fibers move down, they become slightly slack and the fiber
tension decreases. Hence fiber tension also decreases with time.
However, other phenomena — the development of stresses and strains, thermal expan-
sion of the mandrel and composite with temperature rise — have not been modeled here.
These phenomena will definitely have a significant effect on the fiber movement. Hence,
though the presented results are reflective of the process physics, a complete picture can be
obtained only by including all these effects.
8.5 Summary and Outlook

In this chapter, we introduced the modeling approach to three processes in which the resin
moves relative to the fibers. Each process has its own complexities although the general
approach is to adopt Darcy's law to describe the impregnation of the fluid into the porous
network created by the fibrous preform. The fibrous network is represented by permeability.
Accurate modeling and characterization of this quantity is the key to success in modeling
of the process. However, in autoclave, VARTM and filament winding there is a dynamic
change in the permeability due to the rearrangement of the fibrous media as the load on
the fiber network changes during the impregnation process.
Hence the challenges in this modeling efforts remain are description of the compacting
effect and its influence on the preform permeability and also more accurate methods to
characterize the preform permeability such that one can design the preform to ease the
processing needs. Use of these process simulations in an effective manner in optimization
and control of the process is currently being pursued and with the use of sensors, one can
see the manufacturing of composites moving into the era of intelligent processing which will
allow for statistical variation of material properties and also for human error. This would
naturally lead one into the realm of automation of the process, which should be the final
goal of any modeling and simulation effort.

8.6 Exercises
8.6.1 Questions
1. Describe the wet hand layup process by using these words and terms: tool (mold)
surface, gel coat, reinforcement material, resin, and rollers.
2. What industry widely uses the wet hand layup process?
3. What are the advantages and disadvantages of the wet hand layup process?
4. List three common processes used to make advanced thermoset fiber composites.
5. What process has traditionally been used to manufacture very large composite struc-
tures in the aerospace industry?
6. Describe the autoclave process by using these words and terms: preimpregnated, plies,
prepregs, tapes stack, tool surface, high pressure and temperature, air pockets, excess
resin, autoclave, large pressure vessel, heating element, consolidate and cure.
7. Which one requires higher pressure and temperature during processing, thermoset or
thermoplastic composites? Why?
8. What are the main advantages and disadvantages of the autoclave process as compared
to other processes?
9. Describe a typical stacking order of layers in an autoclave process. Explain the purpose
of the different layers.
10. What is the role of consolidation in the autoclave process?
11. What are the three most important process parameters in the autoclave process that
influence the part quality?
12. What are the typical ranges of temperatures and pressures exercised in autoclave
processing?
13. What is the drawback to using fully impregnated tapes with smooth surfaces in the
autoclave process?
14. How many stages are there in autoclave processing? Describe each stage.
15. Increasing the autoclave pressure prevents possible void growth. This suggests one
should use as high autoclave pressure as possible. However, there is an important
reason why the autoclave pressure is not increased to maximum pressure. What is
that reason?
16. Why is air not suitable for pressurizing the autoclave at high temperatures? What
gas is commonly used for this purpose?
17. List the common errors involved in the material and cure preparation step in the
autoclave process.
18. What are the resulting effects of incorrect autoclave pressure and temperature profile
on the composite part?

19. Why is the mathematical modeling of flow and consolidation in autoclave processing
important?
20. Under what conditions during autoclave processing would one expect the pressure
gradient and the resin flow to be primarily in the thickness direction rather than
in the in-plane directions? What is the corresponding simplified partial differential
equation to relate the fiber volume fraction to the pressure?
21. List the most commonly used liquid composite molding (LCM) processes.
22. What are the two groups in which you can classify LCM processes?
23. Describe the five stages of the resin transfer molding (RTM) process.
24. What are the major advantages and disadvantages of RTM compared to other processes?
25. What are the main differences between RTM and SCRIMP?
26. Among RTM and vacuum bagged VARTM, which process should be selected if small
dimensional tolerances are required? Compare these two processes in terms of initial
investment and labor cost.
27. Describe the following for a reinforcing fabric: fiber volume fraction, permeability,
wettability and sizing.
28. What are the common fibers and fabrics used in LCM?
29. What are the major ingredients of a resin system?
30. List the desired behavior of a good resin system.
31. What factors determine the types of fabric and resin system to be used in LCM? Give
examples.
32. What materials are used for the manufacturing of molds (tools)? Describe their
advantages and disadvantages.
33. Why is the design of a mold important?
34. What are the undesired effects of improper design of gate and vent locations?
35. Why do some molds need heating/cooling channels machined into them?
36. Suppose that you have a flow rate controlled injection system for RTM. In order to
reduce the fill time and hence the cycle time, should you set the injection flow rate to
the maximum? Explain.
37. Why are the mathematical models of resin flow and cure and the simulation codes
based on these models important?
38. What are the major issues in LCM?
39. What is fiber wash out? What causes it?
40. What is racetracking? What causes it? Is it always undesired? What are the major
consequences of racetracking on the resin flow?

41. Describe the injection compression molding process. What must be calculated care-
fully before injecting the resin?
42. Under what conditions in LCM can resin flow be modeled using Darcy's law?
43. In LCM, when can the resin flow be modeled in two dimensions instead of three
dimensions? Can the heat transfer model also be simplified into two dimensions?
44. When and how are the resin flow and cure models coupled?
45. When is the modeling of resin flow inside a dual scale porous medium important?
What modification should be made to the mass conservation equation if dual scale
flow is to be considered?
46. Although a unique numerical solution of resin pressure distribution can be obtained
for a completely filled mold under a given set of gate and vent boundary conditions,
why do the simulation codes apply a time marching scheme to solve the pressure and
flow front location?
47. In order to measure the permeability of a preform at a given fiber volume fraction,
how is a one-dimensional experiment performed? What variables and parameters are
recorded in each experiment? What relationship is used? What causes error in the
measured value?
48. What is the heat dispersion coefficient? Under what conditions can it be neglected?
49. What physical phenomena occur during the filament winding process? Briefly explain
them.

1. All the advanced thermoset fiber composite processes evolved from the wet hand layup
process in which the goal was either to the process to reduce cost,
to improve treatment, eliminate or reduce emissions of to the
environment, improve dimensional and/or increase the
content in the composite.
2. In order to manufacture a thermoset composite part as large as 30 meters in diameter
and over 50 meters in length, process is used. industry uses this
process for years to manufacture large parts.
3. The largest existing autoclave in the U.S. is at the commercial aircraft plant
in
4. Autoclaves are usually made of steel as they are subjected to high pressure
and temperature.
5. In autoclave process layup stacking, are used to absorb excess resin in the
thickness direction. The material allows for uniform distribution of vacuum
over the surface of the part. A covers the whole stacking assembly.
The role of this plate is to improve the of the part and improve
by applying uniform pressure and minimizing ply movement.

6. The goal of autoclave consolidation is to force and excess out of
the structure.
7. There are typically three stages of autoclave processing. In Stage I, and
are ramped up inside the autoclave. In Stage II, the autoclave is maintained
at the processing pressure and temperature to allow and As
the cure reaction proceeds and generates heat due to polymerization, in stage III,
the is lowered to allow the excess from the reaction to diffuse
through the part but the is maintained, to prevent voids from
8. The most widely used gas for pressurizing the autoclave is Air is unsuitable
at high temperatures due to the risk of
9. The goal in autoclave processing is to develop the most optimal and
cycles to manufacture free composite part.
10. The warpage of composite parts that are autoclaved is linked to the
developed in the part and the differences in the coefficient of _: of the
1
composite both along the fibers and in the transverse directions.
11. In the autoclave process, void growth can be minimized by modeling resin
and hence controlling the autoclave
12. The resin flow model of the autoclave process enables complete of fibers.
13. The temperature model of the autoclave process allows the engineers to reduce tem-
perature within the composite and hence to avoid resin degradation.
14. In order to overcome the long fill time disadvatage of VARTM, process was
developed and patented under the Corporation's name. In this process, a
very fabric is placed on top 'of the preform. Since it has very
to resin flow, resin saturates this layer quickly and then flows into the reinforcing
preform in the direction.
15. of a reinforcing preform is a measure of resistance to resin flow. It is neither
a scalar, nor a vector, but it is a
16. is a measure of how easily the interior of a fiber bundle is wetted as resin
moves around the bundle.
17. is a coating on the fiber surface to increase the wettability property and
also to increase the bond between the and the
18. Cores such as and are included inside large and thick parts to
lower the cost, increase the moment of inertia, and reduce the weight of the part.
19. Alternative to cores, internal inflatable might be used in thick parts such
as tennis racquets and rotor blades.
20. and fabrics cannot be used in stamping of fabrics with thermo-
formable binder process as they don't during the stamping stage.
21. Most of the injection equipment is designed for either controlled, or
controlled injections.

22. Among the most commonly used thermoset resins in LCM, has the lowest
performance, easiest processing and lowest cost. On the other extreme end,
has the highest performance, most difficult processing and highest cost.
23. The part is demolded when the matrix reaches a strength such that the
part will not deform or warp after being taken out of the mold.
24. Microvoids are created because the inside a fiber tow region is very different
than the of the region between the fiber tows in woven and stitched fabrics.
voids are created as resin races along the tows and encircles itself along
a stitch. When resin flow is faster in between the tows, then voids are
trapped in between the fiber bundles.
8.6.3 Problems
1. Assume that (i) the resin used in an autoclave is Newtonian, (ii) the Reynolds number
is low, and (iii) the voids are spherical. If P is the void pressure, Pr is the resin
pressure, R is the radius of the void, and a is the surface tension, find an expression
for these process variables so that the void growth will be suppressed. If you can vary
the temperature and pressure within the autoclave, how will it affect the void growth?
Would you set the pressure to be maximum for autoclave control? Explain why.
2. Equation (8.2) relates the void growth to viscosity, void radius, surface tension, pres-
sures of void and the resin. Can you express R(t) in closed form? How would you
solve R(t) numerically, with an initial condition R(0) — R0, and what data will you
need?
3. Consider an autoclave that is made of welded steel of thickness 20 mm. The autoclave
is a cylindrical tube of diameter 0.5 m and length of 1 m. The tooling and part thermal
inertia can be considered negligible as compared to the autoclave inertia. How long
will it take to heat the autoclave from room temperature of 25°C to 350°C, if the
heater power supplied to the autoclave is 20 kW?
4. By referring to Figures 8.12 and 8.13, answer the following questions: (a) It takes ti
minutes for the mid-point of the composite to reach a fiber volume fraction of about
0.61 from the initial value of 0.53. How long will it take for the entire composite to
be above fiber volume fraction of about 0.70? (b) If it takes t% minutes for the resin
pressure at the top layer to reach its maximum value Pmax, at roughly what time(s)
the resin presure at this location reaches Pmax/27 Explain why there is more than
one unique time values to your answer.
5. Consider a resin flow racetracking along a rectangular channel of height of h = 5 mm
and a width of w = 2.5 mm. If all four walls of the channel are assumed to be
nonporous, calculate the permeability Krace of the channel to be used as a parameter
in one-dimensional Darcy's law.
6. Thermal design criteria require you to keep the temperature differential between the
center and the surface of the composite to less than 20° C. You know that a cooling
rate of 5 Watts/sec for a 6 mm thick composite was able to do so for an epoxy resin.
For a second part of 8 mm thickness, what is the maximum cooling rate you can
impose to meet the thermal design criteria?

7. Resolve Example 8.5 assuming that the transient temperature is important. See
example 5.5 on the details for solving transient thermal problems.
8. Suppose that a resin is injected from the left edge of a rectangular mold cavity from
a line source at a constant pressure of P = Pvent + AP. There is a line vent at the
right edge of the mold. Assume that there is no racetracking and a uniform preform.
Hence the flow is one-dimensional. The mold has a length of L — 1 m, a thickness
of h = 0.01 m and a width of w = 0.2 m. The preform has a porosity of 0.5 and a
uniform permeability of 2 * 10~9 m2 along the resin flow direction, resin viscosity is
/j, — 0.2 Pa.s. (i) Calculate the flow rate when the mold is half full for AP = 1 bar.
(ii) If the length of the mold is changed to L = 2 m, and viscosity is reduced to
/j, = 0.15 Pa.s, what will be the flow rate when the mold is 50% full?
9. In the previous problem, if the air inside the mold is initially at 1 bar, but the vent is
kept closed, what will be the steady state void size if AP = 10 bar assuming that the
entrapped air inside the void doesn't dissolve into the resin and behaves as an ideal
gas.
10. Considering an unsteady state one-dimensional permeability experiment, plot the flow
front Xf(t) and injection pressure P;nj(i) as a function of time at two different values of
sink term, s — 0 and 0.002 s"1 if the preform width w = 0.2 m, thickness h = 0.005 m,
porosity <$> = 0.4, permeability Kxx = l*10~ 10 m 2 , resin viscosity /j, = 0.15 Pa.s, and
flow rate Q = 4*10~6 m3.
11. For Gz » I in RTM applications, the steady-state temperature distribution is given
by T _Tm — 1 — erf(£) where £ = —i z a z z x an(i z 'ls the distance from the wall towards
the center in the thickness direction. If Tin — 20°C and T0 = 150°C, plot the composite
temperature, T, as a function of z along the thickness direction at a downstream
location (far away from the injection ports).

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Process Modeling

MARCEL DEKKER, INC. NEW YORK • BASEL

Copyright 2003 by Marcel Dekker, Inc. All Rights Reserved.

This book is printed on acid-free paper.

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World Wide Web

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Current printing (last digit):

PRINTED IN THE UNITED STATES OF AMERICA

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1. Computers in Manufacturing, U. Rembold, M. Seth, and J. S. Weinstein

Copyright 2003 by Marcel Dekker, Inc. All Rights Reserved.

Additional Volumes in Preparation

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Yolanda Chetwynd, Madhu and Diana Advani;

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2 Overview of Manufacturing Processes

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4 Constitutive Laws and Their Characterization

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6 Short Fiber Composites

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7 Advanced Thermoplastic Composite Manufacturing Processes

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1.1 Motivation and Contents

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Figure 1.1: Fiber composite made from fibers and resin.

Carbon Tapes and Fabric

Figure 1.2: Different fiber forms.

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Figure 1.3: Curing is the process of cross-linking a thermoset polymer.

Figure 1.4: Polymer resin types used to make composites.

the composite manufacturing process.

1.3 Polymer Matrices for Composites

The polymer matrix in a composite will consist mainly of a thermoplastic or thermoset

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Figure 1.5: Typical fabrics and schematics with continuous fibers.

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3-D Cylindrical 3-D Braiding 3-D Orthogonal Angle-Interlock

Figure 1.6: More detailed architectures of reinforcing fiber preforms [10].

Melt Flow Random Discontinuous Continuous

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" r"* ,'- f- -" f~ '

Figure 1.8: Schematic of the molecular structure: a) Amorphous Thermoplastic, b) Semi-

The thermoplastic properties are determined by the resulting microstructure, which is

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Figure 1.9: Change in crystallization rate as a function of temperature. Tg is the glass

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1.3.2 Comparison Between Thermoplastic and Thermoset Polymers

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Table 1.2: Comparison of different material viscosities [13].

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>j<£^££--' >•••••• •'• •••^.«'v,;, ./W..W.,,,,

It is difficult to stack the layers in a desired orientation when draping multi-layers of

1.4.1 Fiber-Matrix Interface

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