Journal of Reinforced Plastics and

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Recent Development in Natural Fiber Reinforced Polypropylene Composites

Ramakrishna Malkapuram, Vivek Kumar and Yuvraj Singh Negi
Journal of Reinforced Plastics and Composites 2009 28: 1169 originally published online 20
November 2008
DOI: 10.1177/0731684407087759
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Recent Development in Natural Fiber

Reinforced Polypropylene Composites
RAMAKRISHNA MALKAPURAM, VIVEK KUMAR AND YUVRAJ SINGH NEGI*
Polymer Science and Technology Program, Department of Paper Technology
Indian Institute of Technology Roorkee, Saharanpur Campus
Saharanpur, UP, India
ABSTRACT: This review article describes the recent developments of natural fiber reinforced
polypropylene (PP) composites. Natural fibers are low-cost, recyclable, and eco-friendly materials.
Due to eco-friendly and bio-degradability characteristics of these natural fibers, they are considered
as strong candidates to replace the conventional glass and carbon fibers. The chemical, mechanical,
and physical properties of natural fibers have distinct properties; depending upon the cellulosic
content of the fibers which varies from fiber to fiber. The mechanical properties of composites are
influenced mainly by the adhesion between matrix and fibers. Chemical and physical modification
methods were incorporated to improve the fibermatrix adhesion resulting in the enhancement of
mechanical properties of the composites. The most important natural fibers are jute, flax, and coir
and their novel processing technics to develop natural fiber reinforced composites are also described.
KEY WORDS: natural fibers, polypropylene, chemical and physical modifications, processing,
properties.

INTRODUCTION
N THE RECENT past considerable research and development have been expanded in
natural fibers as a reinforcement in thermoplastic resin matrix. These reinforced plastics
serve as an inexpensive, biodegradable, renewable, and nontoxic alternative to glass or
carbon fibers. The various advantages of natural fibers over man-made glass and carbon
fibers are low cost, low density, competitive specific mechanical properties, reduced energy
consumption and biodegradability. Thermoplastic materials that currently dominate as
matrices for natural fibers are polypropylene(PP), polyethylene, and poly(vinyl chloride)
while thermosets, such as phenolics and polyesters, are common matrices. With a view to
replacing the wooden fittings, fixtures and furniture, organic matrix resin reinforced with
natural fibers such as jute, kenaf, sisal, coir, straw, hemp, banana, pineapple, rice husk,
bamboo, etc., have been explored in the past two decades.
There is an increasing demand from automotive companies for materials with sound
abatement capability as well as reduced weight for fuel efficiency. Natural fibers possess
excellent sound absorbing efficiency and are more shatter resistant and have better energy
management characteristics than glass fiber reinforced composites. In automotive
parts, such composites not only reduce the mass of the component but also lower the

*Author to whom correspondence should be addressed. E-mail: dr_negi57@hotmail.com

Journal of REINFORCED PLASTICS

AND

COMPOSITES, Vol. 28, No. 10/2009

0731-6844/09/10 116921 $10.00/0

DOI: 10.1177/0731684407087759

SAGE Publications 2009
Los Angeles, London, New Delhi and Singapore

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R. MALKAPURAM ET AL.

energy needed for production by 80%. Eco-friendly composites can be made by replacing
glass fibers with various types of ligno-cellulose fibers. However, such composites have a
distinct disadvantage of load-bearing capability compared to glass fiber reinforced
thermoplastics. The variation in the properties of natural fibers is another important
aspect that has to be considered. Demands for natural fibers in plastic composites is forecast
to grow at 1520% annually with a growth rate of 1520% in automotive applications, and
50% or more in selected building applications. Other emerging markets are industrial and
consumer applications such as tiles, flower pots, furniture, and marine piers [1].
Development of new composite products from the easily renewable natural materials
has a strong potential to deliver novel biodegradable and/or readily recyclable materials
suitable for the automotive and packaging industry, thereby replacing not so easily
renewable fossil fuel-based polymers/plastics.
Complete matrix fusion to facilitate thorough fiber impregnation, formation of strong
fiber/matrix interfacial bonding, and matrix-to-fiber stress transfer efficiency are vital
requirements for the manufacture of reliable, eco-friendly natural composites that can
possess better mechanical properties and withstand environmental attacks. Bledzki and
Gassan [2] have stated that the quality of the fibermatrix interface is significant for the
application of natural fibers as reinforcement fibers for plastics. Physical and chemical
methods can be used to optimize this interface. These modification methods are of
different efficiency for the adhesion between matrix and fiber.
However, the main problem of natural fiber/polymer composites is the incompatibility
between the hydrophilic natural fibers and the hydrophobic thermoplastic matrices. It
necessitates the use of compatibilizers or coupling agents in order to improve the adhesion
between fiber and matrix [3].
Matrix or fiber modification is therefore necessary to improve the compatibility between
fiber and matrix. Maleated polyolefins are used to modify the matrix. Such modification of
the matrix develops the interactions between the anhydride groups of maleated coupling
agents and the hydroxyl groups of natural fibers. For the purpose of making engineering
parts with a wide study on the effect of different coupling agents, such as silanes, maleic
anhydride grafted polypropylene (PPgMA) or modification by acetylation, has been
reported in the literature.
In the present article an attempt has been made to review the state of the art of
organocellulosic fiber reinforced polyolefin composites. The various types of natural fibers
used for such reinforcement are described. The modifications of fiber and matrix are
discussed and the mechanical properties of composites are described also. Performance of
the composites is summarized.
LIGNOCELLULOSIC FIBERS OR MATERIALS
Several types of lignocellulosic materials have been investigated in PP [412].
Cellulosic fibers from other sources have been reported in polyolefin composites by
several authors. A comprehension review of the cellulosic-based materials in composites
has appeared recently [2]. The lignocellulosic fibers that have been used in polyolefins
include cellulose fiber [412], wood fiber [1322], flax [2329], Cannatis sativa (hemp)
[3035], jute [1,25,33,3537], pinewood fiber [3841], sisal [3,33,4244], rice husk [4548],
saw dust [4850], lugffa sponge fiber [3,51], wheat straw [52], paper sludge [53], coconut
fiber [33,54], kenaf [55,56], kapok/cotton [57], pineapple leaf [58], basalt [59], vetiver [60],
bio flour [61], bamboo fiber [62], and date palm fiber [63].

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Natural Fiber Reinforced Polypropylene Composites

CHEMICAL COMPOSITION OF SOME NATURAL FIBERS

In Table 1 cotton has the maximum content of cellulose ranging from 85 to 95%. The
other fibers have cellulose along with lignin and other components such as hemicellulose,
pectin wax, etc., in varying quantities. The various chemical constituents of a specific
natural fiber also vary considerably.
MECHANICAL PROPERTIES OF LIGNOCELLULOSIC MATERIALS
The structure, chemical composition, microfibrillar angle, and cell dimension defects are
the most important variables that affect the overall properties of the fibers. A fiber is more
ductile if the microfibrils have a spiral orientation to the fiber axis. If the microfibrils are
oriented parallel to fiber axis then the fibers are inflexible and rigid. The natural fibers
exhibit considerable variation in diameter along with the length of individual filaments.
In Table 2 the properties of these fibers are summarized.
Table 1. Chemical composition of some natural fibers.
Fiber

Cellulose
(wt%)

Lignin
(wt%)

Hemicellulose
(wt%)

Pectin
(wt%)

Wax
(wt%)

Moisture
content (wt%)

Jute
Hemp
Kenaf
Flax
Ramie
Sunn
Sisal
Henquen
Cotton
Kapok
Coir
Banana
PALF

6171.5
70.274.4
3139
71
68.676.2
67.8
6778
77.6
82.7
64
3643
6367.6
7082

1213
3.75.7
1519
2.2
0.60.7
3.5
811
13.1

13
4145
5
512

13.620.4
17.922.4
21.5
18.620.6
13.116.7
16.6
10.014.2
48
5.7
23
1020
19

0.4
0.9

2.3
1.9
0.3
10

23
34

0.5
0.8

1.7
0.3
0.4
2.0

0.6

12.6
10

10
8
10
11

8
8.7
11.8

Table 2. Mechanical properties of natural fibers.

Fiber

Density
(g/cm3)

Diameter
(km)

Tensile
strength (MPa)

Youngs
modulus (GPa)

Elongation
at break (%)

Jute
Hemp
Kenaf
Flax
Ramie
Sunn
Sisal
Cotton
Kapok
Coir
Banana
PALF

1.31.45

1.5
1.

1.45
1.51.6

1.15

25200

50200

100450

2080

393773
690

3451100
400938
1.171.9
468640
287800

131175
1.77.9
4131627

1326.5

27.6
61.4128

9.422.0
5.512.6

46

34.582.5

1.161.5
1.6
2.7
2.73.2
1.23.8
5.5
37
78
1.2
1540
1.59.0
1.6

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R. MALKAPURAM ET AL.

The properties are affected by the chemical constitutents and complex chemical
structure of natural fibers. The angle between the axis and the fibril of the fiber
(microfibrillar or spiral angle) also affect the strength of the fibers. Mechanical
properties are higher if this is smaller. Least tensile strength is shown by coir fibers
which may be attributed to low cellulose content and considerably high microfibrillar
(41458 for coir, 208 for sisal, 148 for PALF, and 108 for flax while other fibers such as
jute, ramie, and hemp, have values 510). The lignin content of the fibers influence its
structure properties and morphology. The waxy substances of the natural fibers affect
the fiber wettability and adhesion characteristics. In specific strength the natural fibers
can be compared with glass fibers.
SURFACE MODIFICATIONS OF LIGNOCELLULOSIC FIBERS
Physical Methods
Reinforcing fibers can be modified by physical and chemical methods. Physical
methods, such as stretching, calandering, thermotreatment, and the production of hybrid
yarns do not change the chemical composition of the fibers. Physical treatments change
structural and surface properties of the fiber and thereby influence the mechanical
bondings to polymers.
Chemical Methods
Strongly polarized cellulose fibers are inherently incompatible with hydrophobic
polymers when two materials are incompatible; it is often possible to bring about
compatibility by introducing a third material that has properties intermediate between
those of the other two. There are several mechanisms of coupling in materials:
. weak boundary layers coupling agents eliminate weak boundary layers,
. deformable layers coupling agents produce a tough, flexible layer,
. restrained layers coupling agents develop a highly crosslinked interphase region, with
a modulus intermediate between that of substrate and of the polymer,
. wettability coupling agents improve the wetting between polymer and substrate
(critical surface tension factor),
. chemical bonding coupling agents form covalent bonds with both materials, and
. acidbase effect coupling agents alter acidity of substrate surface.

The development of a definitive theory for the mechanism of bonding by coupling

agents in composites is a complex problem. The main chemical bonding theory alone is not
sufficient. So the consideration of other concepts appears to be necessary, which include
the morphology of the interphase, the acidbase reactions at the interface, surface energy,
and the wetting phenomena.
Change of Surface Tension
The surface energy of fibers is closely related to the hydrophilicity of the fiber. Some
investigations are concerned with methods to decrease hydrophilicity. The modification of
woodcellulose fibers with stearic acid hydrophobizes those fibers and improves their

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Natural Fiber Reinforced Polypropylene Composites

dispersion in PP. A treatment with poly(vinyl acetate) increases the mechanical properties
and moisture repellence.
Impregnation of Fibers
A better combination of fiber and polymer is achieved by impregnation of the
reinforcing fabrics with polymer matrices compatible to the polymer. For this purpose
polymer solutions or dispersions of low viscosity are used.
Graft Copolymerization of Matrix
An effective method of chemical modification of matrix and natural fibers is graft
copolymerization. This reaction is initiated by free radicals of the cellulose molecule. The
cellulose is treated with an aqueous solution with selected ions and is exposed to a high
energy radiation. Then the cellulose molecule cracks and radicals are formed. Afterward
the radical sites of the cellulose are treated with a suitable solution (compatible with the
polymer matrix), for example vinyl monomer (i.e., acrylonitrile, methyl methacrylate,
polystyrene, etc.). The resulting co-polymer possesses properties characteristic of both
fibrous cellulose and grafted polymer.
For example, the treatment of cellulose fibers with hot polypropylenemaleic anhydride
(MAHPP) copolymers [3] provides covalent bonds across the interface. The mechanism
of reaction can be divided into two steps: activation of the copolymer by heating
(t 1708C) (before fiber treatment), and esterification of cellulose.
After this treatment the surface energy of the fibers is increased to a level much closer to
the surface energy of the matrix. Thus, a better wettability and a higher interfacial

HO

H
2
C

O
PP chain

HO

PP chain

H
2
C

C
O

C
H

C
H

Cellulose fiber

H2
C

H2
C
C
H

CH3

O
C
O

C
H

CH3

O
Cellulose fiber

Cellulose fiber

CH3

O
O

OH
+
OH

+ H2O

O
O
H

C
O
H

H2
C
C
H

Figure 1. Mechanism of interaction of cellulose fibers with maleated PP.

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CH3

1174

R. MALKAPURAM ET AL.
O
R HN C O Cell

R N = C = O + H O Cell

Figure 2. Formation of urethane linkage by reaction of isocyanate and hydroxyl groups of cellulose.

Cellulose + Lignin

C=O

C=O

C=O

NH

NH

NH
CH2

CH2

CH

CH2

CH

CH2

CH2

CH

CH2

Polystyrene
Figure 3. Interaction between PS Matrix and PMPPIC modified cellulose fibers.

adhesion is obtained. The PP chain permits segmental crystallization and cohesive

coupling between the modified fiber and the PP matrix.
Modification of Lignocellulosic Fibers with Isocyanates
The reactivity of cellulosic hydroxyl groups with a variety of reagents can resolve the
fibers hydrophobicity such as treatment reduces:
. the number of cellulose hydroxyl groups, which are available for moisture pick-up,
. the hydrophilicity of the fibers surface, and
. the swelling of the fiber, by creating a crosslinked network due to covalent bonding,
between matrix and fiber.

The mechanical properties of composites reinforced with wood fibers and PVC or PS as
resin can be improved by an isocyanate treatment of cellulose fibers [52,61].
Polymethylenepolyphenylisocyanate (PMPPIC) in pure state or solution in plasticizer
can be used. Isocyanates are chemically linked to the cellulose matrix through strong
covalent bonds: both PMPPIC and PS contain benzene rings, and their delocalized
electrons provide strong interactions, so that there is an adhesion between PMPPIC and
PS.
The isocyanatic treatment is reported to be more effective than the treatment with
silane. Similar results are obtained, when PMPPIC is used for the modification of the
fibers or polymer matrix.
Triazine Coupling Agents
Triazine derivatives form covalent bonds with cellulose fibers. The triazine derivatives
are used to reduce the moisture absorption of cellulose fibers and their composites.

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1175

Natural Fiber Reinforced Polypropylene Composites

Cellulose fiber

H2NR

HN

CI

CI

CI

CI

CI
R
HN
N

H
O

CI

Cellulose fiber
Figure 4. Modification of cellulose fibers with triazine derivatives.

Organosilanes as Coupling Agents

Organosilanes are the main group of coupling agents for glass-fiber reinforced polymers.
They have been developed to couple virtually any polymer to the minerals, which are used
in reinforced composites.

PROCESSING AND PROPERTIES OF NATURAL

FIBER REINFORCED PP COMPOSITES
Khondker et al. [1] have reported that the jute/PP unidirectional composites, specimens
with only 20% of jute fiber (Vf ) content, show remarkable improvement in tensile
and bending properties when compared to those of the virgin PP specimens. The
improvements in the mechanical properties are broadly related to various factors, such as
the wettability of resin melts into fiber bundles, interfacial adhesion, orientation, and
uniform distribution of matrix-fibers and the lack of fiber attrition and attenuation during
tubular braiding process.
The water absorption properties of coir, sisal fibers reinforced PP composites in water
at three different temperatures, 23, 50, and 708C, were studied. A decrease in tensile
properties of the composites was demonstrated, showing a great loss in mechanical
properties of the water-saturated samples compared to the dry samples [3].
The hardness and elastic modulus of a cellulose fiber-reinforced PP composite were
investigated by nano-indentation with a continuous stiffness technic. A line of indents was
produced from the fiber to the matrix. There was a gradient of hardness and modulus
across the interphase region. The distinct properties of the transition zone were revealed by
14 indents, depending on nano-indentation depth and spacing [4].
The high-tenacity man-made cellulose filament yarn (rayon tyre cord yarn) reinforced
PP, polyethylene, high impact polystyrene (HIPS), and poly(lactic acid) (PLA) composites.

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R. MALKAPURAM ET AL.
Table 3. Continuous fiber reinforced PP composites.

Fiber

Processing technic

Jute yarn
Non wovens of flax and sisal fiber
Uni-directional lyocell fiber
Hightenacity cellulosefilament yarn
(rayon tyre cord yarn)
Unidirectional and multidirectional
flax fiber
Flax fiber yarn
Flax fiber yarn
Jute fiber yarn
Sisal fiber yarn
Kapok/cotton fabric

Reference
number

Tubular braiding technic, compression molding

EXPRESS processing (Extrusion press processing)
Compression molding
Pultrusion technic applied to conventional
co-rotating twin-screw extruder and composite
specimens prepared by injection molding
Heated press in a mold

1
2
4
5

23

Pultrusion and compression molding

Vacuum heating and compression molding
Twin-screw extruder and injection molding
Single-screw extruder and injection molding
Hydraulic press

28
29
36
42
57

Table 4. Short fiber reinforced PP composites.

Fiber
Cellulose fiber
Flax fiber
Flax fiber
Chopped jute fiber
Pinewood fiber
Sisal fiber
Chopped sisal fiber
Kenaf fiber
Pineapple leaf fibre
Vetiver grass
Bamboo fiber
Date palm leaves

Processing technic
Twin-screw extruder and hydraulic press
Haake rheomix and injection molding
Twin-screw extruder and injection molding
Shear K-mixer and injection molding
Laboratory sigma blade mixer and injection molding
Melt mixing (Haake rheocord mixer), solution mixing
(toluene) followed by extrusion and compression molding
Haake rheocord mixer
Compression molding through a sheet stacking technic
Hydraulic press using film stacking technic
Internal mixer and injection molding machine
Haake rheocord and injection molding
Single-screw extruder and injection molding

Reference
number
6
26
27
37
41
43
44
55
58
60
62
63

The pultrusion compounding method developed for highly homogeneous composites. For
a fiber load of 30 wt%, typical values for tensile strength, modulus, Charpy unnotched,
and notched impact strength are 80 MPa, 3.5 GPa, 85 kJ/m2, and 12 kJ/m2, respectively.
A high impact resistance level is maintained also at low temperatures where the matrix
material becomes brittle. For the other matrix materials, similar reinforcing effects are
observed, except for the impact behavior of HIPS, where the reinforcing fibers interfere
with the impact modification of the matrix polymer. In contrast, the impact characteristics
of PLA are drastically improved increasing the unnotched and notched Charpy strengths
by 380% and 200%, respectively [5].
Amash and Zugenmaier [6] investigated the thermal, morphological and dynamic
mechanical properties of PPcellulose fiber (CF) composites. The effects of drawing on the
structure and physical properties of PPCF composites were also studied. By increasing
draw ratio, the melting peak of PP shifted to higher temperatures suggesting a constrained
melting, and the uniaxial elastic modulus was considerably enhanced. The biggest

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1177

Natural Fiber Reinforced Polypropylene Composites

Table 5. Particulate fiber reinforced PP composites.
Fiber

Processing technic

Sisal, coir, luff sponge and

cellulose from pulp fiber
Cellulose whiskers
Rice husk and wood flour fiber
Alfa, bleached soft wood,
Avicel fibers
Cellulose fibers
Eucalyptus wood, ground
corncob and spent brewery
grain fibers
Cellulose fibers
Eucalyptus wood fibers
Lignocel fiber
Pine free saw dust
Kraft pulp of eucalyptus fiber
Hard wood dust
Aspen pulp fiber
Pinewood flour
Liquified wood mill
Wood fiber
Wood fiber
Flax (pulp) fiber
Chopped hemp fiber
Hemp strands
Hemp fiber
Sisal, kenaf, hemp,
jute and coir
Hemp fiber
Jute and hemp fiber

Reference
number

Brabender mixer and processed by

compression molding
Solvent mixing followed by hot press
Twin-screw extruder and injection molding
Brabender mixer and compression molding

7
8
9

Melt mixing (plastomill) and compression molding

Brabender and hydraulic press

10
11

Droplet method
Hot press
High-speed mixer and injection molding
Single-screw extruder and compression molding
Twin-screw extruder and injection molding
Mixer and injection molding
Haake rheomix 600 equipped with roller blades
rotor and compression molding
woodtruder and die
Haake rheomix, single-screw extruder
and injection molding
Twin-screw extruder and compression molding
Single-screw extruder and compression molding
Twin-screw extruder and injection molding
Powder impregnation through compression
molding and extrusion followed by injection molding
Heated roll mixer and injection molding
Brabender internal mixer and compression molding
Compression molding using a film stacking method

12
12
14
15
16
17
18

Twin-screw extruder and injection molding

Single fiber embedded inside two previously
built sheets of PP matrix by
compressing at melting point
Two roll mill and injection molding

Bleached soft wood

pine fibers
Pinewood saw dust
Granules prepared by single-screw extruder
Wood material of radiate pineMixer and hot press
(Pinus radiate)
Rice husk flour filler
Single-screw extruder and injection molding
Saw dust/Rice husk
Kinetic mixer and injection molding
Rice husk
Twin-screw extruder and injection molding
Rice husk
Single-screw extruder and injection molding
Saw dust
Mixer and compression molding
Saw dust
Haake rheo mixer and compression molding
Luffa fiber
Haake rheocord mixer and compression molding
Wheat straw fibers
Brabender mixer and injection molding
Paper sludge
Single-screw etruder and compression molding
Coconut fiber
Haake rheocord mixer and compression molding
Layer of kenaf
Plied up alternatively and pressed in a heated press
Rice husk
Pellets processed by twin-screw extruder

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19
20
21
22
24
30
31
32
33
34
35

38
39
40
45
46
47
48
49
50
51
52
53
54
56
61

1178

R. MALKAPURAM ET AL.

influence was observed for the samples of PPspun cellulose and the lowest for neat PP.
In addition to the fibrillar structure of the oriented PP, the highly CF orientation and
the efficient compatibilization in composites are responsible for the effects observed in
the drawn samples.
The nanocomposite films of isotactic PP reinforced with cellulose whiskers highly
dispersed with surfactant were prepared for the first time and compared with either bare or
grafted aggregated whiskers. The nanocomposites obtained with the surfactant-modified
whiskers exhibited enhanced ultimate properties when compared to the neat matrix or to
the composites containing the other filler types [7].
The tensile and Izod impact strength properties of rice-husk flour and wood flour as the
reinforcing filler and different compatibilizing agents, by assessing their mechanical
properties and the morphological characteristics of their fracture surfaces. The tensile
properties of the composites made with the twin-screw extruding system were better than
those of the composites made with the single-screw extruding system, due to the improved
dispersion of the filler. The tensile strength and modulus of the lignocellulosic fillerPP
composite made with the twin-screw extruding system were improved in the case of the
composite made without any compatibilizing agent and significantly improved in the case
of the composite made with the compatibilizing agent, as compared with those made with
the single-screw extruding system. The Izod impact strengths of the composites made
with the two different extruding systems were almost the same, the degree of dispersion
of the fillers might influence the notched impact performance, but the similar impact
strength of both samples with different extruding processes might be due to the fact that
impact test is not discriminating enough to reveal the difference in dispersion status of the
present composites [8].
The mechanical properties of the CFs reinforced polyethylene composites increased
with increasing the average fiber length and the composite materials prepared using
both matrices and cellulose fibers treated with g-methacryloxypropyltrimethoxy silane
(MPS), and g-mercaptoproyltrimethoxy silanes (MRPS) displayed good mechanical
performances. On the other hand, with hexadecyltrimethoxy-silanes (HDS) bearing
merely aliphatic chain only a modest enhancement on composite properties was
observed [9].
Qiu et al. [10] have reported that PP with higher molecular weight revealed stronger
interfacial interaction with cellulose fibers in the composites, compared with the lower
molecular weight PP; the composites derived from higher molecular weight of PP exhibited
stronger tensile strength at the same cellulose content.
Georgopoulos et al. [11] have investigated that the loading of LDPE with natural fibers
leads to a decrease in tensile strength of the pure polymer. On the other hand, Youngs
modulus increased due to the higher stiffness of the fibers. Although the properties of
some blends are acceptable for some applications, further improvement is necessary, by
optimizing fiberpolymer interface characteristics.
Joly et al. [12] have optimized the fiber treatments for PP/cellulosic-fiber composites.
In one method the grafting of a PP chain by an ester bond capable of co-crystallizing or
entangling with the fibers was used. While the modification of cellulose fiber was done by
isocyanates for improvement in the rupture, initiation strength was observed by PP
modification of fibers resulting in the crack propagation strength.
The tensile strength of the PP-wood-based composites decreased significantly with
increasing wood fiber content and no significant change in modulus of elasticity was found
for any weight fraction of wood fiber. Fiber pullout was observed on most of the

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Natural Fiber Reinforced Polypropylene Composites

1179

PP composite fracture surfaces examined using SEM. These results indicate a lack of
adhesion between PP and wood fiber [13].
Tensile and flexural tests of foamed composites were investigated as a dependence
of function of density (specific properties) of foamed specimens and compared with
nonfoamed composites based on MAHPP has improved the physico-mechanical
properties up to 80%. Chemical foaming agents have also an effect on surface roughness
of the composites which decreased surface roughness of the foamed composites compared
to the nonfoamed composites. Water absorption and thickness swelling of the composites
were also investigated. The density of microfoamed hard wood fiberPP composites
reduced around 30% and decreased up to 0.741 g/cm3 by using an exothermic chemical
foaming agent. Optical microscopy showed that the cells are round and cell sizes are
affected by chemical foaming agents. Tensile and flexural tests are performed on the
foamed composites to investigate the dependence of these properties on the density
(specific properties) of foamed specimens and compared with nonfoamed composites and
MAHPP has improved the physico-mechanical properties up to 80% [14].
The impact fracture behavior of PP/wood fiber composites modified with maleated
PP as compatibilizer and poly(butadiene styrene) rubber as impact modifier has been
studied by a Charpy impact testing method. The neat PP and unmodified PP/wood
fiber composite exhibit brittle fracture and nearly elastic behavior while the impact
modifier and compatibilizer cause elastic to elasticplastic transition dominated by
unstable crack propagation. Both the impact modifier and the compatibilizer toughen the
PP matrix enhance the total fracture energy of the modified composites. While the crack
initiation energy is mostly only a little material dependent and reflects the matrix behavior,
the crack propagation energy is much more influenced by the morphology [15].
Novel compatibilizer (m-TMI-g-PP) with isocyanate functional group was synthesized
by grafting m-isopropenyl-a,a-dimethylbenzyl-isocyanate (m-TMI) onto isotactic PP in a
twin-screw extruder. The effect of filler concentration on the mechanical properties
of bleached kraft pulp of eucalyptus reinforced PP composites, prepared by using
m-TMI-g-PP as the compatibilizer, was investigated. The addition of the compatibilizer
resulted in greater reinforcement of composites, as indicated by the improvement in
mechanical properties. Tensile strength of composites so prepared increased by almost
45%, whereas 85% increase in flexural properties was observed [16].
Costa et al. [18] have evaluated the tensile and flexural performance of PPwood fiber
composites. The effect of these variables on tensile strength, Youngs modulus, elongation
at yield and flexural strength was determined through a 22
31 factorial design (where the
variables chosen were: fiber content (F ), percentage of MAPP coating on the wood fiber
(C ) and type of matrix (M )). The mechanical properties (responses) selected from tensile
data were stress at maximum load (TS), tensile modulus (TM) and elongation at yield (E ).
The selected responses of flexural data were stress at maximum load (FS) and flexural
modulus (FM). Using standard least-squares parameter estimation procedures and
statistical analysis, empirical models were built and parameter values and co-variances
were computed. The analysis of variance of the experimental and predicted data shows
that the constructed models provide a fair approximation of actual experimental
measurements. Finally, experimental details regarding the preparation of optimum
composites as predicted by empirical models are discussed.
Jungil Son and his coworkers analyzed the effect of process additives, that is, maleated
PP (MAPP), and a nucleating agent on the viscoelastic properties of different types
of extruded PPwood plastic composites manufactured from either a PP homopolymer,

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a high crystallinity PP, or a PP impact copolymer using dynamic mechanical thermal

analysis. The woodplastic composites were manufactured using 60% pine wood flour and
40% PP on a Davis-Standard Woodtruder. Dynamic mechanical thermal properties,
polymer damping peaks (tan ), storage modulus (E0 ), and loss modulus (E00 ) were
measured using a dynamic mechanical thermal analyzer. To analyze the effect of the
frequency on the dynamic mechanical properties of the various composites, DMA tests
were performed over a temperature range of 201008C, at four different frequencies (1, 5,
10, and 25 Hz) and at a heating rate of 58C/min. From these results, the activation energy
of the various composites was measured using an Arrhenius relationship to investigate the
effect of MAPP and the nucleating agent on the measurement of the interphase between
the wood and the plastic of the extruded PP woodplastic composites [19].
Van de Valde and Kiekens [23] have analyzed the unidirectional (UD) and
multidirectional (MD) flax/PP composites at different process times and temperatures.
The UD composites of boiled flax combined with MAA-PP show the best mechanical
properties. Contrary to the UD composites, flax treatment did not lead to the expected
property improvements for MD composites.
The composites were compounded with two kinds of flax fibers (natural flax and
flax pulp) and PP. The applied treatments were maleic anhydride (MA), maleic
anhydridepolypropylene copolymer (MAPP) and vinyl trimethoxy silane (VTMO).
The treatment effects on the fibers have been characterized by infrared spectroscopy. Two
technics have been used to determine the surface energy values: the dynamic
contact angle method for the long flax fibers and the capillary rise method for the
irregular pulps. The use of different methods involves a small discordance in
the wettability values. Nevertheless, the three treatments reduce the polar component
of the surface energy of the fiber. Composites containing MAPP showed highest
mechanical properties, whilst the MA and VTMO-treated fiber showed virtually no
improvement compared to untreated ones [24].
Keener et al. [25] used maleated coupling agents to strengthen the composites containing
fillers and fiber reinforcements. The established role of maleated polyolefins results from
two main factors, economical manufacturing and the efficient interaction of maleic
anhydride with the functional surface of fiber reinforcements. Peak performance was
demonstrated in agrofiber PP composites by selecting a maleated coupler that has the
appropriate balance of molecular weight and maleic anhydride content.
Arbelaiz et al. [26] have studied the effect of fiber treatments with maleic anhydride,
maleic anhydride PP copolymer, vinyltrimethoxy silane, and alkalization on thermal
stability of flax fiber and crystallization of flax fiber/PP composites. In order to compare
thermal stability of flax fibers, thermogravimetry (TG) analysis was used. Kinetic
parameters have been determined by the Kissinger method. Results showed that all
treatments improved thermal stability of flax fibers. Addition of flax fiber increased
crystallization rate of PP as revealed by DSC, pressure volume temperature (PVT)
measurements and polarized optical microscopy (POM) technics. Besides depending on
fiber surface treatment and crystallization temperature, flax fiber/PP composites also
showed transcrystallinity.
The mechanical properties (i.e., tensile strength and stiffness) of flax/PP composites are
effectively improved by compatibilization of the fiber/matrix interphase. The most
important factor limiting the properties of the composites lies in the intricate structure of
the fibers themselves, after the interfacial strength is optimized, the internal fiber structure
becomes the weakest point [27].

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Pultrusion technic developed for flax reinforced PP commingled yarn containing

discontinuous flax and PP fibers. Rectangular cross-sectional profiles produced by
using a self-designed pultrusion line. In a series of experiments carried out with yarns of
two different flax fiber contents, the pultrusion parameters were varied. In particular,
the preheating and die temperatures and also the pulling speed, which are the most
relevant parameters regarding the potential future pultrusion of natural fiber composite
profiles at industrial scale. A complete characterization of each profile was conducted
in order to examine the influence of processing parameters on the profile quality.
The mechanical properties were evaluated by performing three-point bending as well as
Charpy impact tests [28].
Unidirectional composites from filament wound nontreated flax yarns and PP
fabricated foils composite have exhibited axial stiffness and strength in the range
2729 and 251321 MPa, respectively. A modified version of the rule-of-mixtures,
supplemented with parameters of composite porosity content and anisotropy of fiber
properties, was developed to improve the prediction of composite tensile properties [29].
The tensile strength of hemp strand/PP composites can be as high as 80% of the
mechanical properties of glass fiber/PP composites [31].
The composites of isotactic PP with hemp fibers (Cannabis sativa), functionalized
by means of melt grafting reactions with glycidyl methacrylate (GMA) were prepared
by batch mixing. The modification of fibers (hempGMA) and polyolefin
matrix (PP-g-GMA), as well as the addition of various compatibilizers (PP-g-GMA,
SEBS, SEBS-g-GMA), were carried out to improve the fibermatrix interactions.
All composites displayed higher tensile modulus (2.9 GPa) and lower elongation at
break as compared to plain PP; compatibilization with PP-g-GMA (10 phr) resulted in an
increased stiffness of the composites as consequence of an improved fibermatrix
interfacial adhesion [32].
Kenaf, hemp, and sisal composites showed comparable tensile strength and modulus
properties but in impact properties hemp appears to outperform kenaf. The tensile
modulus, impact strength and the ultimate tensile stress of kenaf reinforced PP composites
were found to increase with increasing fiber weight fraction. Coir fiber composites
displayed the lowest mechanical properties, but their impact strength was higher than that
of jute and kenaf composites. In most cases the specific properties of the natural fiber
composites were found to compare favorably with those of glass [33].
Pickering et al. [34] investigated the optimization of New Zealand grown hemp fiber
reinforced PP composites. The optimum growing period was found to be 114 days,
producing fibers with an average tensile strength of 857 MPa and a Youngs modulus of
58 GPa. The strongest composite consisted of PP with 40 wt% fiber and 3 wt% MAPP,
and had a tensile strength of 47.2 MPa, and a Youngs modulus of 4.88 GPa.
Doan et al. [36] investigated the effect of maleic anhydride grafted PP (MAPP) coupling
agents on the properties of jute fiber/PP composites.
The addition of 2 wt% MAPP to PP matrices improved the adhesion strength with jute
fibers and the mechanical properties of composites.
Effect of impact modifier on 0, 4, 9, and 14 wt% indicated that both impact and tensile
properties showed increasing trend with the compatibilizer but the reverse was true for the
flexural properties [37].
Girones et al. [38] studied the PP-based composites, reinforced with surface modified
pine fibers. Tensile modulus increased only by 12% after incorporation of untreated fibers
to PP matrix. Treatment with silane led to a significant rise (about 60% compared with

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that of unfilled matrix) in tensile modulus. A higher effect was noted for MRPS, followed
by MPS, HDS, and g-aminopropyltrimethoxysilane (AMPS). Flexural modulus was
amplified by 130% with fiber addition and modestly enhanced after silane treatment
compared with that of untreated fibers, flexural modulus increased by 6, 5, 20, and 8% in
the presence of MPS, HDS, AMPS, and MRPS, respectively.
Borysiak and Doczekalska [39] studied the wood sawdust/PP composites based on
polish timber species pine wood (Pinus silvestris L.) as a softwood species and beech wood
(Fagus silvatica L.) as a hardwood species. The size of wood saw dust ranged from 0.5 to
1.0 mm. Three different types of wood/PP mixture were prepared: (1) PPuntreated wood,
(2) PPNaOH treated wood, and (3) PPesterified wood with maleic anhydride. In this
study, the kinetic parameters of crystallization of PP by differential scanning calorimetry
(DSC) were investigated. It is interesting that crystallization of PP depends on the kind of
wood. The chemical treatment of wood caused changes of crystal conversion and half
crystallization time of PP matrix.
Wechsler and Hiziroglu [40] have studied woodplastic composite (WPC) specimens
having 60 and 80% particle and fiber of radiata pine (Pinus radiata) mixed with PP
(plastic), and four different additives, namely Structor TR 016 which is a coupling agent,
CIBA anti-microbial agent (IRGAGUARD F3510) as fungicide, CIBA UV filter coating
(TINUVIN 123S), CIBA blue pigment (Irgalite), and their combinations. Based on the
initial finding of this study static bending properties of the samples enhanced by the above
chemicals were added into both particle and fiber-based specimens. Thickness swelling of
the samples were also improved by the presence of additives in the panels. Micrographs
taken on a scanning electron microscope (SEM) revealed that coupling agent and pigment
resulted in more homogeneous mixture of wood and plastic together. The particle-based
samples had rougher surface characteristics than those of fiber-based ones. No significant
influence of chemicals added in the samples was found on surface roughness values of the
samples manufactured from particle and fiber of radiata pine.
Pickering and Ji [41] studied the effects of poly[methylene (polyphenyl isocyanate)]
(PMPPIC) and MAPP coupling agents, separately and combined, on the strength and
Youngs modulus of New Zealand radiata pine-reinforced PP composites. A modest
improvement compared to the unreinforced matrix strength of 4% and much greater
improvement of 123%, substantially greater than reported elsewhere in the literature, were
obtained using PMPPIC and MAPP, respectively. Youngs modulus improvements
compared to the unreinforced matrix of 77 and 177% were obtained using PMPPIC and
MAPP, respectively.
The processing of sisal fiber reinforced PP composites by injection molding was reported
by Li and his coworkers. The tensile properties for PP, high temperature (HT) and low
temperature (LT) specimens were compared. It was observed that the incorporation of
10 wt% of sisal fibers increases Youngs modulus by about 150%, and the tensile strength
was increased by about 10%. The reinforcement efficiency for LT specimens is slightly
higher than HT samples [42].
Joseph et al. [43,44] prepared sisal fiber reinforced PP composites by melt-mixing and
solution-mixing methods. The methods enhanced the tensile properties of the
composites. The effect of fiber content and chemical treatments on the thermal
properties of sisal/PP composites was also evaluated. It was found that treated fiber
composites show superior properties compared to the untreated system. DSC
measurements exhibited an increase in the crystallization temperature and crystallinity,
upon the addition of fibers to the PP matrix. This is attributed to the nucleating effects

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of the fiber surfaces, resulting in the formation of transcrystalline regions. On

increasing the fiber content, the melting peak of the PP component was shifted to
higher temperatures suggesting a constrained melting.
Han-Seung yang et al. [45] prepared a particle-reinforced composite, in that rice-husk
flour as the reinforcing filler and PP as the thermoplastic matrix polymer, and its
mechanical and morphological properties examined as a function of the amount of
compatibilizing agent used. In the sample preparation, four levels of filler loading (10, 20,
30, and 40 wt%) and three levels of compatibilizing agent content (1, 3, and 5 wt%) were
used, and in the tensile test, six test temperatures (30, 0, 20, 50, 80, and 1108C) and five
crosshead speeds (2, 10, 100, 500, and 1500 mm/min) were used. The tensile strengths of
the composites decreased as the filler loading increased, but the tensile properties
were significantly improved with the addition of the compatibilizing agent. Both the
notched and the unnotched Izod impact strengths were almost the same with the addition
of compatibilizing agent.
Sain et al. [46] studied flammability of PP, rice husk filled PP composites, and flame
retarding effect of magnesium hydroxide for these composites by horizontal burning
rate and oxygen index tests. Despite the presence of a coupling agent, the addition of
flame-retardants shows a negative impact on the tensile and flexural properties of the
composites and the properties show a reduction of 17 and 15%, respectively, compared to
the composite without flame retardant
Coutinho et al. [49] studied the influence of the amount of MAPP coating of vinyl-tris
(2-methoxy ethoxy) silane treated woodfibers (2 or 10 wt%), type of matrix (PP or MAPP)
and composition (10, 20, or 30 wt%) on the tensile and flexural performance of PPwood
fiber composites was studied. The effect of these variables on tensile strength, Youngs
modulus, elongation at yield, and flexural strength was determined through a 22
31
factorial design. The analysis of variance of the experimental and predicted data show
that the constructed models provide a fair approximation of actual experimental
measurements. Finally, experimental details regarding the preparation of optimum
composites as predicted by empirical models were discussed.
Suarez et al. [50] studied the morphological behavior of composites of PP or PP plus
MAPP and saw dust coated with 22.4 wt% MAPP were prepared under fixed processing
conditions (mixing temperature, rate of rotation and mixing time). SEM was performed to
analyze the tensile fracture surfaces and the interfacial fiber/matrix adhesion. The tensile
properties of composites with up to 10% MAPP have not been improved by increasing
MAPP content. This has been attributed to the poor filler/matrix adhesion. The addition
of higher MAPP content to the PP composites produces better adhesion of saw dust to PP
matrix and an increase in the tensile strength.
The effects of coupling agents on the mechanical, morphological, and water sorption
properties of luffa fiber (LF)/(PP) composites were studied. In order to enhance the
interfacial interactions between the PP matrix and the luffa fiber, three different types of
coupling agents, (3-aminopropyl)-triethoxysilane (AS), 3-(trimethoxysilyl)-1-propanethiol
(MS), and maleic anhydride grafted polypropylene (MAPP) were used. The PP composites
containing 215 wt% of LF were prepared in a torque rheometer. The tensile properties of
the untreated and treated composites were determined as a function of filler loading.
Tensile strength and Youngs modulus increased with employment of the coupling agents
accompanied by a decrease in water absorption with treatment due to the better adhesion
between the fiber and the matrix. The maximum improvement in the mechanical
properties was obtained for the MS treated LF composites. The interfacial interactions

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improved the filler compatibility, mechanical properties, and water resistance of

composites. The improvement in the interfacial interaction was also confirmed by the
Pukanszky model. Good agreement was obtained between the experimental data and the
model prediction [51].
Panthapulakka et al. [52] studied the potential of wheat straw fibers prepared by
mechanical and chemical processes as reinforcing additives for thermoplastics was
investigated. Fibers prepared by mechanical and chemical processes were characterized
with respect to their chemical composition, morphology, and physical, mechanical, and
thermal properties. Composites of PP filled with 30% wheat straw fibers were prepared
and their mechanical properties were also evaluated. The fibers prepared by chemical
process exhibited better mechanical, physical, and thermal properties. Wheat straw fiber
reinforced PP composites exhibited significantly enhanced properties compared to virgin
PP. However, the strength properties of the composites were less for chemically prepared
fiber filled composites. This was due to the poor dispersion of the fibers under the
processing conditions used. These results indicate that wheat straw fibers can be used as
potential reinforcing materials for making thermoplastic composites.
Jang and Lee [53] fabricated the paper sludge/PP composites. Flame retardants like
Saytex8010, TPP, Mg(OH)2, and antimony trioxide were introduced into the composites
for improvement of the flame retardancy and was measured with the UL94 test.
Rozman et al. [54] studied the effect and mechanical properties of lignin as a
compatibilizer in the coconut fiberPP. Composites with lignin as a compatibilizer possess
higher flexural properties as compared to the control composites. The results also show
that tensile properties do not improve as lignin is incorporated. SEM results display some
proof of an enhanced compatibility at the interfacial region.
Shibata et al. [56] fabricated the lightweight laminate composites made from kenaf and
PP fibers by press forming. The effects of the number of kenaf layers, heating time, and
kenaf weight fraction on the flexural modulus of the composite specimen were
investigated. The flexural modulus increased with increasing number of kenaf layers and
heating time. The increase of the number of kenaf layers contributed to homogeneous PP
dispersion in the composite board. This is because more kenaf layers caused better contact
between kenaf and PP and prevented PP fibers from shrinking by heating. The increase of
heating time contributed to better wetting between kenaf and PP.
Mwaikambo et al. [57] showed that kapok/cotton fabric has been used as reinforcement
for conventional PP and maleic anhydride grafted PP resins. Treating the reinforcement
with acetic anhydride and sodium hydroxide has modified the fabric (fibers). Thermal
and mechanical properties of the composites were investigated. Results show that fiber
modification gives a significant improvement to the thermal properties of the plant fibers,
whereas tests on the mechanical properties of the composites showed poor tensile strength.
Mercerization and weathering were found to impart toughness to the materials, with
acetylation showing slightly less rigidity compared to other treatments on either the fiber
or the composites. The modified PP improved the tensile modulus and had the least
toughness of the kapok/cotton reinforced composites. MAiPP reinforced with the plant
fibers gave better flexural strength and the same flexural modulus at lower fiber content
compared with glass fiber reinforced MAiPP.
Arib et al. [58] investigated the tensile and flexural behaviors of pineapple leaf fiberPP
composites as a function of volume fraction. The tensile modulus and tensile strength of
the composites were found to be increasing with fiber content in accordance with the rule
of mixtures.

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Czigany [59] manufactured the basalt fiber reinforced, PP matrix hybrid composites
in the process of carding, needle-punching, and pressing. Hemp, glass, and carbon fibers
were applied besides basalt fiber in these composites. In order to achieve a sufficient
interfacial adhesion, the fibers were treated with the reaction mixture of maleic acid
anhydride and sunflower oil. The hybrid effect in these composites was examined as a
function of fiber content and fiber combination. The strength properties of hybrid
composites improved owing to surface treatment and this was proven by mechanical tests
and microscopic analysis, as well. Acoustic emission methods revealed that there is a
correlation between the physical parameters of sound waves that occurred during failure
and the mechanical properties.
Ruksakulpiwat et al. [60] prepared the injection molded vetiverPP composites at
various ratios of vetiver content and vetiver length. When compared to PP, vetiverPP
composites exhibited higher tensile strength and Youngs modulus but lower elongation
at break and impact strength. An increase in vetiver content led to an increase in
viscosity, heat distortion temperature, crystallization temperature, and Youngs modulus
of the composites. On the other hand, the decomposition temperature, tensile
strength, elongation at break, and impact strength decreased with increasing
vetiver content. The chemical treatment of the vetiver grass improved the mechanical
properties of the composites.
Kim et al. [61] investigated the effect on thermal properties of the addition of
two different compatibilizing agents, maleic anhydride (MA)-grafted polypropylene
(MAPP) and MA-grafted polyethylene (MAPE), to bio-flour-filled, PP, and low
density polyethylene (LDPE) composites. The effect of two different types of MAPE
polymer, MA-grafted high-density polyethylene (HDPE-MA) and MA-grafted linear
LDPE (LLDPE-MA), was also examined. With increasing MAPP and MAPE content,
the thermal stability, storage modulus (E_ ), tan max peak temperature (glass transition
temperature: Tg) and loss modulus (Emax) peak temperature ( relaxation) were
slightly increased. The thermal stability, E_ and E__ of MAPE-treated composites were
not significantly affected by the two different MAPE polymers. The melting temperature
(Tm) of the composites was not significantly changed but the crystallinity (Xc) of
MAPP- and MAPE-treated composites was slightly increased with increasing MAPP
and MAPE content. This enhancement of thermal stability and properties could
be attributed to an improvement in the interfacial adhesion and compatibility
between the rice husk flour (RHF) and the matrix due to the treatment of compatibilizing
agent. Attenuated total reflectance (FTIR-ATR) analysis confirmed this result
by demonstrating the changed chemical structures of the composites following
MAPP and MAPE addition.
Liao et al. [62] have studied the resistance of bamboo fiber reinforced PP composite
(BFRP) and bamboo-glass fiber reinforced PP hybrid composite (BGRP) to hygrothermal
aging, and their fatigue behavior under cyclic tensile load, were studied. Injection molded
samples were exposed in water at 258C for up to 6 months and at 758C for up to 3 months.
Tensile strength and elastic modulus of BFRP and BGRP samples have shown moderate
reduction after aging at 258C after 6 months; however, they were reduced considerably
after aging at 758C for 3 months. Moisture absorption and tensile strength degradation are
suppressed by using MAPP as a coupling agent in both types of composite systems. BFRP
and BGRP samples were also loaded cyclically at maximum cyclic load of 35, 50, 65, and
80% of their ultimate tensile stress. Results suggest that BGRP has better fatigue
resistance than BFRP at all load levels tested.

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Abu-Sharkh and Hamid [63] studied the degradation characteristics of the date palm
leaves compounded with PP and UV stabilizers. Enhanced stability imparted by the
presence of the fibers in the composites, enhanced interfacial adhesion resulting from
oxidation of the polymer matrix can be the source of retention of mechanical strength.
FUTURE WORK
There is an increasing demand from auto companies for materials with sound abatement
capability as well as reduced weight for fuel efficiency; therefore, the use of natural fibers
over man-made glass and carbon fibers. However, the properties of these natural fiber
reinforced composites are dependent on the properties of the fiber and the adhesion
between fiber and matrix. The enhancement of the properties of the composites can be
achieved by chemical modificatons of matrix and the fiber.
CONCLUSIONS
The chemical, mechanical, and physical properties of natural fibers have distinct
properties; cellulose content of these fibers varies from fiber to fiber. The moisture content
lowers the mechanical properties. The mechanical properties of composites are influenced
mainly by the adhesion between matrix and fibers. As in the case of glass-fibers, the
adhesion properties can be changed by pre-treating the fibers. Novel processing
techniques, chemical and physical modification methods are developed to improve the
fiber-matrix adhesion resulting in the enhancement of mechanical properties of
the composites. Up to now, the most important natural fibers are jute, flax, and coir.
Yet the development of novel processing and modification methods is not finished.
Further improvements can be expected, so that it might become possible to substitute
technical-fibers in composites quite generally. Natural fibers are low-cost, recyclable and
eco-friendly materials. Eco-friendliness and bio-degradability of these natural fibers may
replace the glass and carbon fibers.
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