Excerpt from the Proceedings of the COMSOL Conference 2010 Paris

Effective thermal conductivity of composite: Numerical and

experimental study

M. Karkri1*
1
Université Paris Est Créteil Van de Marne, CERTES, 61 avenue du Général de Gaulle, 94010
Créteil Cedex, France
* Corresponding author: [email protected]

Abstract: In this paper, thermal properties of transfer in the medium. Auriault and Ene [8]
composites are investigated numerically and have investigated the influence of the interfacial
experimentally. In the numerical study, finite- thermal barrier on the effective conductivity and
elements method is used to modelize heat on the structure of the macroscopic heat transfer
transfer and to calculate the Effective Thermal equations. Using the finite elements method,
Conductivity (ETC) of the composite for three Veyret at al. [9] studied the heat conductive
elementary cells, such as simple cubic (SC), transfer in the periodic distribution of the filler in
body centered cubic (BCC) and face centered the composite materials. In their study,
cubic (FCC). The effect of the filler calculation was carried out on two and three-
concentrations, the ratio of thermal dimensional geometric spaces. The same method
conductivities of filler to matrix material and the was used by Ramani and Vaidyanathan [10] that
Kapitza resistance of the contact inclusion/matrix have incorporated the effect of microstructural
on the effective conductivity was investigated. A characteristics such as filler aspect ratio,
periodical method was used to measure interfacial thermal resistance, volume fraction,
simultaneously thermal conductivity, specific and filler dispersion to determine the effective
heat and diffusivity of the composite consisting thermal conductivity of a composite with
of epoxy resin matrix filled with brass spheres. A spherical and parallelepipedic fillers. The
comparison between the numerically calculated thermal conductivity has increased from
thermal conductivities, measured and analytical 0.32 W .m −1K −1 for pure PA6 to 2.09 W .m −1K −1
ones for various samples is made and the for spherical copper powder filler with a 50%
significance of the findings will be discussed in volume fraction. A numerical approach to
the paper. calculate the ETC of granular reinforced
composite was proposed by Cruz [11]. Many
Keywords: Thermal properties, Composite other contributing works were attributed to Yin
materials, Finite elements method, Analytical et al. [12], Kumlutas et al. [13] and Jiang et al.
models, Inverse problem. [14]. Recently, ANSYS software was used by
Liang [15], to perform the numerical simulation
1. Introduction of the heat-transfer process in hollow-glass-bead
(HGB)-filled polymer composites. The effects of
The knowledge of the effective thermal the content and size of the HGB on the effective
conductivity of composites is becoming thermal conductivity was identified. The
increasingly important in many engineering effective thermal conductivity of the
application and in technological developments. polypropylene (PP)/HGB composites was
Numerous theoretical and empirical models have estimated at temperatures varying from 25 to 30
been proposed to predict the effective thermal °C. Lattice Monte Carlo (LMC) and finite
conductivity [1-4]. Numerous numerical studies element analyses were used on the ETC of
of thermal conductivity of filled polymer were sintered metallic hollow spheres structures,
conducted in the past. Deissler’s [5] works were Fiedler et al. [16]. In their work, the LMC
extended by Wakao and Kato [6] for a cubic or calculation strategy is enhanced in order to
orthorhombic array of uniform spheres in incorporate temperature dependence of thermal
contact. Shonnard and Whitaker [7] have conductivity and specific heat in transient
investigated the influence of contacts on two- thermal analyses [17]. In this paper, the effective
dimensional models. They have developed a thermal conductivity of brass spheres/resin
global equation with an integral method for heat epoxy is investigated numerically and
experimentally. The ETC was calculated using Matrix :
∇ (λm∇τ ) = 0
the COMSOL software. The obtained values are
(1)
compared with experimental results and some
existing theoretical and semi-empirical models. τ = τ 1 , z = +b and τ = τ 2 , z = −b (2)
τ = (τ1 + τ 2 ) / 2 , z = 0 (3)
2. Prediction methods of effective thermal
∂τ (4)
conductivity λm = (σ − τ ) / rc , matrix ∩ sphere
∂n
2.1. Mathematical modeling and Finite ∂τ (5)
− λm = 0, lateral faces
Element Solution. ∂n
Sphere :
Using the finite-element software COMSOL
3.5b, thermal analysis was carried out for the
( )
∇ λ f ∇σ = 0 (6)
∂σ (7)
three-dimensional conductive heat transfer. −λf = (τ − σ ) / rc sphere ∩ matrix
About the geometry, we considered three unit ∂n
cells corresponding to some arrangements such
as simple cubic (SC), body centered cubic (BCC) Where n is the normal unit vector pointing from
and face centered cubic (FCC). The simple cubic the filler to the matrix. In order to simplify the
body is composed of a sphere of radius r problem and to decrease the computing time,
centered in a cubic cavity of dimensions (2 × b )3 dimensionless parameters and variables were
used:
(Figure 1).
X = x/r , Y = y/r and Z = z / r : the
z dimensionless space variables.
b , −b τ1 S = (2σ − τ1 − τ 2 ) / (τ1 − τ 2 ) : the unknown inner
temperatures field.
y T = (2τ − τ 1 − τ 2 )/ (τ 1 − τ 2 ) : the unknown outer
temperatures field. B = (2b − 2r ) / 2r : the
0
reduced resistance of the matrix layer between
nearest spheres. D = λm / λ f is the conductivity
x
b , −b b , −b ratio between the two phases. C = rc λm / r is the
τ2
reduced contact resistance located at the sphere
Figure 1. Simple cubic body. interface.
The heat transfer in the elementary cell is E = λeff / λm : the effective thermal conductivity.
governed by the stationary heat transfer The effective thermal conductivity E is
equations. At the interphase the temperature calculated versus four parameters (the relative
potential jumps across the interface. The thermal contact resistance between particle and
associated normal component of the heat flux is matrix C, the half distance between the particles
continuous and is proportional to the jump in divided by the sphere radius B, the filler volume
temperature potential. The boundary conditions fraction φ and the ratio of thermal conductivity
at the edges of the elementary cell are of between the two phases D). In order to obtain
adiabatic type except at the upper and lower high accuracy for the ETC computation with
faces where temperature is prescribed with σ each model (SC, BCC and FCC), the refinement
and τ the filler and the matrix temperatures mesh around small geometrical features and on
respectively and rc the thermal contact the upper face ( z = b ) was considered (Fig. 2).
resistance. According to the symmetries, only In the light of a previous work [18], the effective
one-sixteenth of the original simple cubic cell thermal conductivity for each model is calculated
needs to be meshed (Fig. 2). The mathematical versus the heat flux crossing the elementary
equations representing the heat transfer model cells.
are given by the equations system (1-7).
 B+1
S1 S1 filler amount φ BCC is correlated to B by:

1 m
φBCC = π / 3(1 + B) , with :
3

z  
1/16 of sphere dT 1 dS
y QBCC =  ∫∫
 dZ 1 D
dS + ∫∫ dZ
dS 2 

(11)
0  s1 s2 
x B
(a)
S3 + S2
S1
S1 2.2. Experimental study
S2
S1
In our experimental set-up, the matrix material
is an epoxy resin of VANTICO Company. The
Araldite® LY5052 is mixed to 38% weight of
Aradur® 5052. The brass spheres (70%Cu, 30%
(b) (c)
Zn, ρbrass = 8530 Kg / m 3 ) of 3.18 mm and 6.35
mm of diameter with a thermal conductivity of
Figure 2: Mesh of elementary cell for SC (a) and 124 W .m −1K −1 were placed in aluminum mold
FCC (b) and BCC (c) models
cavity ( 45 × 45mm 2 ). Three samples were
- Effective thermal conductivity of simple cubic model: prepared under the same conditions: the first two
are presented in figures 3 and 4. The first
The heat flux crossing the simple cubic configuration is a simple cubic with brass
elementary cell is defined by: spheres of 6.35 mm diameter and the second one
B +1  Y = X is an hexagonal arrangement, with a maximum
dT 
 dY dX
QSC =

0  0
∫ ∫ dZ Z = B +1 

(8) volume fraction(14)with brass spheres (3.18 mm
diameter). The third sample is a stacking of three
layers of spheres with a 6.35 mm diameter which
The effective thermal conductivity and the filler represents a face centered cubic model for its
volume fraction of the SC model are given by: central part (Figure 5).
E = 2QSC /(1 + B) ; φSC = π / 6(1 + B)3
- Effective thermal conductivity of FCC model (Figure
3):

The heat flux crossing the face centered cubic

elementary cell is defined by:
 dT 1 dS 
 s1
∫∫
 dZ dYdX + D dZ dYdX
s2 
∫∫
QFCC =   (9) Figure 3: Sample (a) and computed elementary cell
+ 1 dS dYdX3
 D dZ ∫∫ 

 s3 
The effective thermal conductivity and the filler
volume fraction of the FCC model are given by:
E = 2QFCC /(1 + B ) and
(10)
φFCC = 2π / 3(1 + B)3

- Effective thermal conductivity of BCC model : Figure 4: Sample (b), epoxy resin / brass
spheres of diameter 3.18mm and computed
The heat flux for this case is calculated and the elementary cell
effective thermal conductivity is deduced from
the following relation: E = 2QBCC /(1 + B ) . The
 τ1

l SC Figures 7 and 8 show the variation of the ETC

λSC, eff SC
2 model for face centered cubic (FCC) and body centered
cubic (BCC) for different contact resistances and
filler volume fractions φ . Similar behavior can
FCC model be noted with the SC model. As seen from the
λFCC , eff figures, for low filler volume fraction φ ≤ 50% ,
lFCC
the calculated effective conductivities are nearly
the same for both BCC and FCC models. The
maximum effective thermal conductivity for both
BCC and FCC models was calculated in the
perfect interface case, i.e. no jump temperature
lSC λSC, eff SC
across the resin/spheres interface
model
2 ( EBCC = 6.34 and EFCC = 5.97 respectively).

τ2
Figure 5: Sample (c) and the computed φ = 60% φ = 50% φ = 40%
φ = 30% φ = 20% φ = 10%
elementary cell: calculation of the effective 7
φ = 5%
thermal conductivity 6
Effective conductivity (E)

5
3. Results and discussion
4

3.1. Numerical results- effect of filler volume 3

fraction and thermal contact resistance

2

Thermal conductivity as described in the section 1

2.1, was computed by the 3D-finite element 0

-5 -4 -3 -2 -1
0.0
method, as a function of three quoted parameters 1.0x10 10 10 10 10
C [-]
B, C and D. Computation of about 150 E values
has showed that a decrease in the contact Figure 7: Effect of the thermal contact resistance
resistance C or of the inner resistance D leads to on the ETC for different filler volume fractions
a raise of the effective thermal conductivity. The
first set of results for the simple cubic-cell is (FCC model, D = 10−5 ).
reported in figure 6. We observe that the lower
φ = 60% φ = 50% φ = 40%
and the higher limits of simple cubic thermal 7
φ = 30% φ = 20% φ = 10%
φ = 5%
conductivity E are, respectively, 2.30 and 6.28.
6
Effective conductivity (E)

26 5
24 B= 0 φ = 52.4 %
22 B= 0.001 φ = 52.2%
4
B=0.0025 φ = 52.0 %
Effective conductivity ( E )

20 B=0.01 φ = 50.8 %
18 B=0.025 φ = 48.6 % 3
B=0.1 φ = 39 %
16

14 2
12

10 1
8
6 0
-5 -4 -3 -2 -1
4 0.0 1.0x10 10 10 10 10
2 C [-]
-15 -14 -6 -5 -4 -3 -2 -1
10 10 10 10 10 10 10 10
C [-]
Figure 8: Effect of the thermal contact resistance
Figure 6: ETC versus C and B, SC model on the ETC for different filler volume fractions
( D = 10−5 ) (BCC model, D = 10 −5 )
3.2. Comparison between analytical models
and numerical simulations 3.5

To illustrate the difference between the 3.0

Effective conductivity (E)

numerical and analytical models, we have plotted
in figure 9 the ETC versus the ratio of the 2.5

thermal conductivity of filler to the one of the

matrix material for a φ = 52% volume fraction 2.0 Models φ = 52% , C = 0.1
Hashin and Sthrikman
−1 −3
and C = 10 . Note that as D = λm / λ f ≥ 10 , it SC
FCC
1.5
BCC
appears that both numerically and analytically
computed thermal conductivities increase very 1.0
-5 -4 -3 -2 -1
slightly and tends to a constant value. Therefore, 10 10 10
D
10 10

the use of higher conductive filler

( λ f f 103W .m −1.K −1 ) is not interesting to Figure 9: Calculated ETC and Sthrikman
enhance thermal composite conductivity. Thus, prediction versus the inner resistance D (C =
typically brass or aluminum fillers seem to be 0.1, φ= 52%)
ideal materials from this point of view. We can
observe that the effective conductivities of FCC 10
Num erical M odels :
and BCC models are fairly close to the 9 SC (D = 10 )
-4

-4
FC C (D = 10 )
Sthrikman model.
Effective conductivity (E)

8 -4
BCC (D = 10 )
7 Lewis and Nielsen M odel
φ max = 52 %
φ max = 68 %
The examination of these results shows that 6
φ max = 74 %
the difference between the Sthrikman model and 5

4
the numericals ETC lies between 2.4% and 7.9%
3
for the SC model and about 17% for the BCC
[ ]
model. On another side, for D ∈ 10 −3 ,10 −1 , it is
2

interesting to show that the difference between 0

0 10 20 30 40 50 60 70
the analytical and the numerical ETC decreases φ (%)
from 5% for simple cubic model to the value of
13% of the BCC model. The results from our Figure 10: Calculated ETC and Nielsen
numerical calculation and Lewis & Nielsen prediction versus the filler volume fraction φ
model versus filler volume fraction are shown in (%), C = 10−5
figure 10 ( D = 10−4 , C = 10−5 ). It is found that
the analytical0 models predicts the same 3.3. Comparisons between simulations,
tendency and represents a relatively good analytical model and experimental data
agreement with the numerical results and the
effective thermal conductivity increases slightly The thermal conductivity and diffusivity of the
from 1 to 2.29 for φ ∈ [0% − 30%] . This samples are measured simultaneously by using a
indicates that spheres are dispersed in matrix and so-called periodic method, using multi-harmonic
they are not interacting with each other. heating signals and inverse problem [19]. The
However, a deviation from the numerical results sample (a) is composed of a brass sphere of
is observed when the percentage of inclusions is radius r = 3.17 mm centered in parallelipipedic
larger φ ≥ 40% and a better agreement is epoxy matrix. Figure 3 shows the calculated
elementary cell and the effective thermal
achieved with φmax = 74% . On the other hand,
conductivity is given by the following equation:
for filler volume fraction greater than 30%, the E( a ) = 2QSC (1 + BSC , m ) . BSC , m is the measured
conductive filler cause an exponential increases
in the effective thermal conductivity of the distance between the sphere and the upper
composite (for example from 2.29 to 6.34 for surface divided by the sphere radius. The second
BCC model). sample is an hexagonal arrangement, especially
in the central part, figure 4. Hence, based on the
computed dimensionless heat flux on the upper 1.52%. We can also observe the influence of this
surface of the elementary cell parameter on the effective thermal conductivities
( B +1) 3  Y = X / 3  of the sample (a) and (b). It may be seen that the
 dT 
QH = ∫ 
 ∫ dZ Z = B +1
dY dX the effective

differences between Ec and Em decrease when
0  0  Bm decreases, it means when the volume
thermal conductivity can be re-written: fraction φ increases. Thus, it seems that the
E(b ) = 2QH (1 + BH , m ) / 3 . The third sample (c) variation measurement-models is lower at a
is a stacking of three layers. The upper and the weak volume fraction. This indicates that the
lower layers represent a simple cubic elementary control of the parameter Bm is significant to
cell with BSC , m = 0 and a thickness of lsc / 2 = r . measure the effective thermal conductivity and
The medium layer is a face centered cubic to understand the heat transfer behavior of the
composites.
elementary cell with BFCC = 0.455 and a
thickness of lFCC = 2 2 r (Figure 5). Hence the
10
2.5
9 E
effective thermal conductivity of the sample (c) 8
2.0

Effective conductivity (E)

elementary cell is:
E(C ) = ESC EFCC l(c ) / (E FCC l sc + ESC l FCC )
7 1.5

6 1.0 φ (% )

where ESC = 2QSC , EFCC = 2QFCC / (1 + BFCC ) 5

0 10 20 30

( )
Measurements:
Sample a

and l( c ) = 2r 2 + 1 are the effective thermal 4 Sample b

Sample c

3 Lewis and Nielsen

φmax = 52.4 %
conductivities for simple cubic and face centered 2
Numerical Models:
SC φmax = 60.5 %
FCC φmax = 68 %
cubic arrangements and the thickness of the face BCC φmax = 74 %
1
centered cubic model, respectively. In order to 0 10 20 30 40 50 60 70
φ (%)
illustrate the difference between the measured
effective conductivities, the calculated values Figure 11: Calculated, measured effective
from FEM simulations Ec and the analytical thermal conductivities and Nielsen model versus
predictions, we assume the perfect contact filler volume fraction φ (%). The conductivity
between the brass spheres and the epoxy matrix. ratio between resin matrix and brass
Figure 11 shows the comparison between the spheres: D = 0.00165 .
analytical prediction, the calculated values and
the measured data of the thermal conductivity of
4. Conclusions
epoxy-resin/brass-spheres composite. It can be
seen that the Nielsen values are fairly close to the
experimental measured data of E. Relatively, the Prediction of the thermal conductivity of
composite materials is crucial in a number of
analytical results with φmax = 68% are closer to
industrial processes. All the theoretical and
the experimental measured data of Em than those empirical models fail to predict ETC of
with φmax ≠ 68% . The experimental values Em at composites in the whole range of filler content.
As seen from this study, Hashin and Sthrikman
about 20°C are compared to the calculated and Lewis & Nielsen models predict fairly well
values Ec from FEM simulations. The results thermal conductivity values up to 30% by
show that the difference between Ec and Em is volume of brass spheres whereas beyond 30% of
inclusion content, all models underestimate the
lower than 2%. It is interesting to note that the
thermal conductivity of the composite. From the
parameter Bm plays a fundamental role on the
thermal conductivity measurements for three
heat transfer between the matrix and spheres and samples of composite at volume fraction from
thus influences largely the value of effective 49% to 57%, it may be concluded that thermal
thermal conductivity. For the samples (c), the
conductivity has increased from 0.2 W .m −1K −1
parameter Bm is very low ( Bm ≅ 0) in this case
for pure epoxy resin to 1.94 W .m −1K −1 .
the difference between Ec and Em is about
Furthermore, the measured values were found to
be in good agreement with numerical data, Graphite Particles, Journal of Reinforced Plastics
especially for sample (b). The influence of the and Composites. 21, 1619 (2002).
reduced outer resistance B of the matrix layer 13. Kumlutas D., Tavmana I. H., Coban M. T.,
between nearest spheres on the ETC is presented Thermal conductivity of particle filled
and trends are discussed. It is shown that B plays polyethylene composite materials, Journal of
a significant role in the composite heat transfer. Composite Science and Technology. 63, 113
(2003)
5. References 14. Jiang M., Ostoja-Starzewski M., Jasiuk I.,
Apparent thermal conductivity of periodic two-
1. Zalba B., Marín J. M., Cabeza L. F., Mehling dimensional composite, Journal of the
H., Review on thermal energy storage with phase computational Materials Science. 25, 329 (2002).
change: materials, heat transfer analysis and 15. Liang J. Z., Li F. H., Simulation of heat
applications, Applied Thermal Engineering. 23 transfer in hollow glass bead filled
251(2003). polypropylene composites by finite element
2. Milton G. W., The theory of composites, method, Polymer Testing. 26, 419 (2007).
Cambridge University Press, Cambridge, UK; 16. Fiedler T., Löffler R., Bernthaler T., Winkler
2002. R., Belova I. V., Murch G. E., Öchsner A.,
3. Furmañski P., Heat conduction in composites: Numerical analyses of the thermal conductivity
Homogenization and macroscopic behavior, of random hollow sphere structures, Materials
Applied Mechanics Review. 50, 327(1997). Letters, 63, 1125(2009).
4. Mirmira, S. R., Fletcher L. S., Comparative 17. Fiedler T., Belova I. V., Öchsner A., Murch
Study of Thermal Conductivity of Graphite Fiber G. E., Non-linear calculations of transient
Organic Matrix Composites, Proceeding of the thermal conduction in composite materials,
5th ASME/JSME Joint Thermal Engineering Computational materials science. 45, 434 (2009).
Conference, San Diego, C. A., Paper A JTE99- 18. Danes F., Garnier B., Dupuis T., Predicting,
6439 (1999). Measuring, and Tailoring the Transverse
5. Deissler R. G., Boegli J. S., An Investigation Thermal Conductivity of Composites from
of Effective Thermal Conductivities of Powders Polymer Matrix and Metal Filler, Int. J.
in. Various Gases, Trans ASME. 80,1417 (1958) Thermophysics. 24, 771(2003).
6. Wakao N., Kato K., Effective thermal 19. Karkri M., Jarny Y., Mousseau P., Inverse
conductivity of packed beds, Chemical heat transfer analysis in a polymer melt flow
Engineering of Japan. 2, 24 (1969). within an extrusion die, Inverse Problems in
7. Shonnard D. R., Whitaker S., The effective Science and Engineering.13, 355 (2005).
thermal conductivity for a pointcontact porous
medium: an experimental study, Int. J. Heat
Mass Transfer. 32, 503(1989).
8. Auriault J-L., ENE H. I., Macroscopic
modelling of heat transfer in composites with
interfacial thermal barrier, Int. J. Heat Mass
Transfer, 37, 2885(1994).
9. Veyret D., Cioulachtjian S., Tadrist L.,
Pantaloni J., Effective Thermal Conductivity of a
Composite Material: A Numerical Approach,
Journal of Heat Transfer. 115, 866(1993).
10. Ramani K., Vaidyanathan A., Finite Element
Analysis of Effective Thermal Conductivity of
Filled Polymeric Composites, Journal of
Composite Materials. 29, 1725(1995).
11. Cruz ME, Computational methods and
Experimental Measurements X, WIT Press,
Southampton, UK, 657 (2001).
12. Yin Y., Tu S.-T., Thermal Conductivities of
PTFE Composites with Random Distributed