Natural Fiber-Reinforced Polymer Composites
Natural Fiber-Reinforced Polymer Composites
Natural Fiber-Reinforced Polymer Composites
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Review
Applied Chemistry Research Centre, PCSIR Labs Complex, Lahore-54600, Pakistan, and 2Institute of Chemistry,
University of the Punjab, Lahore, Pakistan
Received April 2006, accepted March 2007
Communicated by Dr. Shafiq A. Khan
Summary: Natural fibers have been used to reinforce materials for over 3,000 years. More recently
they have been employed in combination with plastics. Many types of natural fibers have been investigated for use in plastics including Flax, hemp, jute, straw, wood fiber, rice husks, wheat, barley, oats,
rye, cane (sugar and bamboo), grass reeds, kenaf, ramie, oil palm empty fruit bunch, sisal, coir, water
hyacinth, pennywort, kapok, paper-mulberry, raphia, banana fiber, pineapple leaf fiber and papyrus.
Natural fibers have the advantage that they are renewable resources and have marketing appeal. The
Asian markets have been using natural fibers for many years e.g., jute is a common reinforcement in
India. Natural fibers are increasingly used in automotive and packaging materials. Pakistan is an agricultural country and it is the main stay of Pakistans economy. Thousands of tons of different crops are
produced but most of their wastes do not have any useful utilization. Agricultural wastes include wheat
husk, rice husk, and their straw, hemp fiber and shells of various dry fruits. These agricultural wastes
can be used to prepare fiber reinforced polymer composites for commercial use. This report examines
the different types of fibers available and the current status of research. Many references to the latest
work on properties, processing and application have been cited in this review.
Introduction
Composites are materials that comprise
strong load carrying material (known as reinforcement) imbedded in weaker material
(known as matrix). Reinforcement provides
strength and rigidity, helping to support structural load. The matrix, or binder (organic or inorganic) maintains the position and orientation
of the reinforcement. Significantly, constituents
of the composites retain their individual, physical and chemical properties; yet together they
produce a combination of qualities which individual constituents would be incapable of producing alone [1].
Wood [2] is natural three-dimensional
polymeric composite and consists primarily of
cellulose, hemicellulose and lignin. In addition,
wood
is an original and natural composite. The
__________________________
E-mail: [email protected]
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biological world offers other examples of composites in bone and teeth, which are essentially
composed of hard inorganic crystals in a matrix
of tough organic collagen.
Historical examples of composites [3] are
abundant in literature. Significant examples
include the use of reinforcing mud walls in
houses with bamboo shoots, glued laminated
wood by Egyptians (1500 BC) and laminated
metals in the forging of swords (1800 AD). In
the 20th century, modern composites were used
in 1930s, where glass fibers reinforced resins.
Boats and aircrafts were built out of these glass
composites, commonly called fiberglass. Since
the 1970s, the application of composites has
widely increased due to development of new
fibers such as carbon, boron and aramids, and
new composite systems with matrices made of
metal and ceramics.
130
Types of Composites
For the sake of simplicity, however, composites can be grouped [4] into categories based
on the nature of the matrix each type possesses.
Methods of fabrication also vary according to
physical and chemical properties of the matrices and reinforcing fibers.
Polymer Matrix Composites (PMCs)
The most common advanced composites
are polymer matrix composites. These composites consist of a polymer thermoplastic or thermosetting reinforced by fiber (natural carbon or
boron). These materials can be fashioned into a
variety of shapes and sizes. They provide great
strength and stiffness along with resistance to
corrosion. The reason for these being most common is their low cost, high strength and simple
manufacturing principles.
Metal Matrix Composites (MMCs)
Metal matrix composites, as the name implies, have a metal matrix. Examples of matrices in such composites include aluminum, magnesium and titanium. The typical fiber includes
carbon and silicon carbide. Metals are mainly
reinforced to suit the needs of design. For example, the elastic stiffness and strength of metals can be increased, while large co-efficient of
thermal expansion, and thermal and electrical
conductivities of metals can be reduced by the
addition of fibers such as silicon carbide.
Ceramic Matrix Composites (CMCs)
Ceramic matrix composites have ceramic
matrix such as alumina, calcium, aluminosilicate reinforced by silicon carbide. The advantages of CMC include high strength, hardness,
high service temperature limits for ceramics,
chemical inertness and low density.
Matrices
Reinforcing Fibers
Matrices
The role of matrix in a fiber-reinforced
composite is to transfer stress between the fibers, to provide a barrier against an adverse
environment and to protect the surface of the
fibers from mechanical abrasion. The matrix
plays a major role in the tensile load carrying
capacity of a composite structure. The binding
agent or matrix in the composite is of critical
importance. Four major types of matrices have
131
been reported: Polymeric, Metallic, Ceramic
and Carbon. Most of the composites used in the
industry today are based on polymer matrices.
Polymer resins have been divided broadly into
two categories: Thermosetting and Thermoplastics.
Thermosetting
Thermoset [5] is a hard and stiff crosslinked material that does not soften or become
moldable when heated. Thermosets are stiff and
do not stretch the way that elastomers and thermoplastics do. Several types of polymers have
been used as matrices for natural fiber composites. Most commonly used thermoset polymers
are epoxy resins and other resins (Unsaturated
polyester resins (as in fiberglass) Vinyl Ester,
Phenolic Epoxy, Novolac and Polyamide) [13].
Unsaturated polyesters [6] are extremely
versatile in properties and applications and have
been a popular thermoset used as the polymer
matrix in composites. They are widely produced industrially as they possess many advantages compared to other thermosetting resins
including room temperature cure capability,
good mechanical properties and transparency.
The reinforcement of polyesters with cellulosic
fibers has been widely reported. Polyester-jute
[7,8], Polyester-sisal [9], polyester-coir [10]
polyester-banana-cotton [11], polyester-straw
[12], polyester-pineapple leaf [13], and polyester-cotton-kapok [14], are some of the promising systems.
Thermoplastics
Thermoplastics [5] are polymers that require heat to make them processable. After
cooling, such materials retain their shape. In
addition, these polymers may be reheated and
reformed, often without significant changes in
their properties. The thermoplastics which have
[15, 16]
[17, 18]
[19]
[16, 20, 21]
[22, 23]
[24, 25]
[26]
[27, 28]
132
dustry. Natural fibers have many significant advantages over synthetic fibers. Currently, many
types of natural fibers [30] have been investigated for use in plastics including flax, hemp,
jute straw, wood, rice husk, wheat, barley, oats,
rye, cane (sugar and bamboo), grass, reeds, kenaf, ramie, oil palm empty fruit bunch, sisal,
coir, water, hyacinth, pennywort, kapok, paper
mulberry, raphia, banana fiber, pineapple leaf
fiber and papyrus. Thermoplastics reinforced
with special wood [2] fillers are enjoying rapid
growth due to their many advantages; lightweight reasonable strength and stiffness. Some
plant proteins are interesting renewable materials, because of their thermoplastic properties.
Wheat gluten [31] is unique among cereal and
other plant proteins in its ability to form a cohesive blend with viscoelastic properties once
plasticized. For these reasons, wheat gluten has
been utilized to process edible or biodegradable
films or packing materials. Hemp [32] is a bast
lingocellulosic fiber, comes from the plant Cannabis sativa and has been used as reinforcement
in biodegradable composites.
Composites based on biologically degradable polyester amide and plant fiber (flax and
cottons) [33] with good mechanical properties,
such as sufficient water resistance and biodegradability, have also been investigated.
Kenaf, Hibiscus cannabinus L, a member
of hibiscus family is also a biodegradable and
environmentally friendly crop. It has been found
to be an important source of fiber for composites
and other industrial applications. Aziz et al. [6]
studied the mechanical properties of composites
manufactured from polyester resin with Kenaf
fiber that blows to a height of at least 10 meter. Traditionally, hemp has been used to make
ropes but these days its fiber is used to make
items such as clothing, toys and shoes. The fiber
is fully biodegradable, is non-toxic and may be
recycled.
133
America and has been used to develop bamboo reinforced thermosetting plastic (epoxy
and polyester) [43,44]. Thwe et al. [45] have
investigated the effect of environmental aging
on the mechanical properties of bamboo-glass
fiber reinforced polymer matrix hybrid composite. Okubo et al. [46] have fabricated bamboo
fiber eco-composites for ecological purposes
with the conventional hot press method. They
studied their static strength and internal state
after their fabrication, and concluded that high
weight content of bamboo fiber enabled the
bamboo composites to increase their strength in
the most effective way, when the bamboo fiber
was modified into the cotton shape.
Yang et al. (36-37) have studied the effect of compatibilizing agents on the mechanical properties and morphology of thermoplastic
polymer composites filled with rice husk flour.
As the filler loading increases, the composites
made without any compatibilizing agent show
decreased tensile strength and more brittleness,
but greatly improved mechanical properties by
incorporation of the compatibilizing agent. The
poor interfacial binding between the filler and
the polymer matrix causes the composites to
have decreased tensile strength, but the tensile
strength and modulus improve with the addition of compatibilizing agent. Wheat straw has
been used for making composites, panel boards
and anion exchangers where the straw is used
in powder form rather than in the fibrous form.
A limited number of studies have reported the
use of wheat straw fibers for production of
composites (38-39). Panthapulakkal et al. [40]
has processed and characterized wheat straw
fibers to evaluate their potential as reinforcing
material for thermoplastic composites. Jute is
also one of the most common agro fibers used
as a reinforcing component for thermoplastics
and thermosetting matrices [41,42]. Bamboo is
an abundant natural source in Asia and South
Natural fibers [4] are generally lignocellulosic in nature, consisting of helically wound
cellulose microfibrils in a matrix of lignin and
hemicellulose. According to a Food and Agricultural Organization survey, Tanzania and
Brazil produce the largest amount of sisal. Henequen is grown in Mexico. Abaca and hemp are
grown in the Philippines. The largest producers
of jute are India, China, and Bangladesh. Presently, the annual production of natural fibers
in India is about 6 million tons as compared to
worldwide production of about 25 million tons.
:
:
:
:
:
Kenaf
Roselle
Sisal
Abaca
Coir
:
:
Borneo
Yugoslavia, China
Nigeria, Guyana, Siera Leone, India
Hondurus, Mauritius
India, Egypt, Guyana, Jamaica, Ghana,
Malawi, Sudan, Tanzania
Iraq, Tanzania, Jamaica, South Africa,
Cuba, Togo
Borneo, Guyana, Malaysia, Sri Lanka,
Togo, Indonesia, Tanzania
East Africa, Bahamas, Antiqua, Kenya,
Tanzania, India
Malaysia, Uganda, Philippines, Bolivia
India, Sri Lanka, Philippines, Malaysia
134
Fiber Source
World
Production
103 Tons
Origin
Fiber Source
World
Production
103 tons
Origin
Abaca
70
Leaf
Nettles
Abundant
Stem
Bamboo
10,000
Stem
Abundant
Fruit
Banana
200
Stem
Palm rah
Abundant
Stem
Broom
Abundant
Stem
Ramie
100
Stem
Coir
100
Fruit
Roselle
250
Stem
Cotton Lint
18,500
Stem
Rice Husk
Abundant
Fruit/grain
Elephant Grass
Abundant
Stem
Rice Straw
Abundant
Stem
Flax
810
Stem
Sisal
380
Stem
Hemp
215
Stem
Sun Hemp
70
Stem
Jute
2,500
Stem
Wheat Straw
Abundant
Stem
Kenaf
770
Stem
Wood
1,750,000
Stem
Linseed
Abundant
Fruit
the constituents contribute to the overall properties of the fiber. Hemicellulose is responsible
for the biodegradation, microabsorption and
thermal degradation of the fiber as it shows
least resistance, whereas lignin is thermally stable but prone to UV degradation. The percentage composition of each of these components
varies for different fibers. Generally, the fiber
contains 60-80 % cellulose, 5-20 % lignin and
up to 20 % moisture. The cell wall of the fibers
undergoes pyrolysis with increasing processing
temperature and contributes to char formation.
These charred layers help to insulate the lignocellulose from further thermal degradation.
135
Table 3. Chemical composition, moisture content, and microfibrillar angle of vegetable fibers.
Flax
71
18.6-20.6
2.2
2.3
Moisture
Content
(Wt %
8-12
Hemp
70-74
17.9-22.4
3.7-5.7
0.9
6.2-12
0.8
2.6.2
Jute
611-71.5
13.6-20.4
12-13
0.2
12.5-13.7
0.5
Kenaf
45-57
21.5
8-13
3-5
Ramie
68.6-76.2
13.1-16.7
0.6-0.7
1.9
7.5-17
0.3
7.5
Nettle
86
Sisal
66-78
10-14
10-14
10-22
Henequen
77.6
4-8
13.1
PALF
70-82
Banana
63-64
Abaca
56-63
Fiber
Cellulose
(Wt %)
Hemicelluloses
(Wt %)
Lignin
(Wt %)
Pectin
(Wt %)
Waxes
Microfibrillar
Angle (Deg)
1.7
5-10
11-17
10
5-12.7
10
11.8
5
12-13
10-22
14
10-12
1
5-10
19
11
Cotton
85-90
5.7
Coir
32-43
0.15-0.25
Cereal Straw
38-45
15-31
42
46
0-1
7.85-8.5
40-45
3-4
12-20
0.6
-30-49
136
137
cal treatments (cold plasma treatment, corona
treatment) and chemical treatments (maleic
anhydride organosilanes, isocyanates, sodium
hydroxide permanganate and peroxide) [50].
Mechanical properties [51] of natural fibers
are much lower than those of glass fibers but
their specific properties, especially stiffness, are
comparable to the glass fibers.
Chemical modification of natural fibers
One of the major problems associated with
the use of natural fibers in composites is their
high moisture sensitivity leading to severe reduction of mechanical properties and delamination. The reduction in mechanical properties
may be due to poor interfacial bonding between
resin matrices and fibers. It is therefore necessary to modify the fiber surface to render it more
hydrophobic and also more compatible with
resin matrices. An effective method of chemical modification of natural fibers is graft copolymerisation. The resulting co-polymer displays
the characteristic properties of both fibrous cellulose and grafted polymer [52,53]. One of the
most explored chemical modifications is the
acetylation-esterification of cellulose-OH, by
reaction with acetic anhydride. This reaction reduces hydrophilicity and swelling of lignocellulosics and their composites [54].
The effect of chemical treatment of natural fibres with sodium alginate and sodium hydroxide has also been reported for coir, banana
and sisal fibres by Mani et al. [55]. This modification results in an increase in adhesive bonding and thus improves ultimate tensile strength
up to 30%. Mitra et al. [56] have reported that
treatment of jute with polycondensates such as
phenol-formaldehyde, melamine-formaldehyde
and cashew nut shell with liquid-formaldehyde
improves the wetability of jute fibres and reduces water regain properties. Samal and Ray
[57] have studied the chemical modification
of pineapple leaf fibers using alkali treatment,
138
bers (mainly: cellulose and lignin) has been
found to be quite different in comparison with
that observed between them and glass surface,
in the sense that with cellulose macromolecules,
only prehydrolyzed silanes undergo the reaction
with cellulose surface [73]. Besides the chemical bonding theory, other theories such as the
interpenetrating networks theory have also been
proposed. This theory states that the matrix diffuses inside the silane interphase to form an entangled network [74-76].
A number of attempts have been carried
out to understand the silane-cellulose system
[77-79]. Thus, the interaction of silane coupling
agents with cellulosic fibers and the effect of
some parameters, such as pH, the initial amount
of silane with respect to cellulose and the adsorption contact time, on their anchoring capability
onto the fiber surface have been ascertained.
Different spectroscopic techniques have been
used to show the presence of silane and to quantify its amounts on the substrate and to elucidate
the structure of the anchored siloxane network
on the fibers surface [78]. Then, using epoxy
and unsaturated polyester resins Abdelmouleh
et al. [79] have shown that the fiber treatment
with silane coupling agents, bearing functional
group able to react with the matrix, enhances
significantly the mechanical strength of the final composite [28]. Recently, Abdelmouleh et
al. [80] have studied three silane agents (different by the functionality of the radical moiety
appended to silicon atoms) to treat delignified
cellulose fibers in order to improve their adhesion low density polyethylene and nitrile rubber matrix. The effect of these treatments on the
mechanical properties of the ensuing composites and on their water uptake ability has been
investigated accordingly. Poor adhesion [47]
at the interface means that the full compatibilities of the composite cannot be exploited and
which leaves it vulnerable to environmental attacks that may weaken it, thus reducing its life
139
span. Insufficient adhesion between hydrophobic polymers and hydrophilic fibers results in
poor mechanical properties of natural fiber reinforced polymer composites. Gassan et al. [81]
have improved the tensile, flexural strength and
stiffness of jute-epoxy composites by treating
the fibers with silane. Tripathy et al. [82] have
found that delignification by bleaching produces better interfacial bond between the jute fiber
and the polyester matrix, and hence results in
better mechanical properties of the composites.
The absorption of steam by sisal, hemp and banana fiber/novalac resin composites has been
found to reduce after esterification of the OH
groups with the maleic anhydride [83]. The tensile strength of maleic anhydride treated fiber
composites is higher than that of the untreated
fiber composites. Luo et al. [38] found an increase in the mechanical properties of green
composites prepared from the pineapple leaf fibers and polyhydroxy butyrate-co-valerate resin (a biodegradable polymer) [84] with the fiber
in longitudinal direction. However, a negative
effect of the fibers on properties in transverse
direction has been observed observed. Gauthier
et al. [85] reported that adhesion may be improved by using coupling agents like maleic
anhydride to incorporate hydroxyl groups on
the matrix through hydrophilization and consequently enhancing the wetting effect of the
resin on the fibers. Mwaikambo and Ansell [86]
treated hemp, jute, sisal and kapok fibers with
various concentrations of NaOH and found 6%
to be the optimized concentration in terms of
cleaning the fiber bundle surfaces, yet retaining
a high index of crystallinity.
Sharifah et al. [87] studied the effect of
the chemically modified polyester resin on the
mechanical properties of the natural fiber composites and its compatibility with natural fibers.
Natural fiber properties are highly variable and
depend on conditions of growth. It is therefore
very difficult to get the same mechanical properties after repeated testing.
140
141
where biodegradable resins have been incorporated as the matrix material [96]
It has been recently predicted that the most
important technologies of the future that incorporate natural fiber composite materials will be
natural fibers for injection moulded products
(32%) followed by natural fibers with a bioplastic matrix (19%) and modified fibers for use in
advanced applications (19%)( Fig.1 [97]).
[9]
[10]
[11]
Concluding remarks
Natural fibers, when used as reinforcement, compete with such technical fibers as
glass fiber. The advantages of technical fibers
are good mechanical properties; which vary
only little, while their disadvantage is difficulty
in recycling. Several natural fiber composites
reach the mechanical properties of glass fiber
composites, and they are already applied, e.g.,
in automobile and furniture industries. Till date,
the most important natural fibers are Jute, flax
and coir. Natural Fibers are renewable raw materials and they are recyclable.
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