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Applied Composite Materials 10: 365379, 2003.

2003 Kluwer Academic Publishers. Printed in the Netherlands.

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Wood Fibre Reinforced Polypropylene Composites:


Effect of Fibre Geometry and Coupling Agent on
Physico-Mechanical Properties
ANDRZEJ K. BLEDZKI and OMAR FARUK
Institut fr Werkstofftechnik, Kunststoff- und Recyclingtechnik, University of Kassel,
Mnchebergstr. 3, D-34109 Kassel, Germany. e-mail: kutech@uni-kassel.de
(Received 13 February 2003; accepted 26 June 2003)
Abstract. Wood fibre reinforced polypropylene composites at fibre content 50% by weight have
been prepared and different types of wood fibres (hard wood fibre, soft wood fibre, long wood fibre
and wood chips) were treated with coupling agent (MAH-PP) to increase the interfacial adhesion with
the matrix to improve the dispersion of the particles and to decrease the water sorption properties of
the final composite.
The present study investigated the tensile, flexural, charpy impact and impact properties of wood
fibre reinforced polypropylene composites as a function of coupling agent and fibre length and
structure.
From the results it is observed that wood chips-PP composites showed better tensile and flexural
properties comparative with the other wood fibre-PP composites with the addition of 5%MAHPP, which is around 65% and 50% for tensile strength and flexural strength respectively. Hard
wood fibre-PP composites showed better impact characteristic values comparative to other wood
fibre-PP composites with the addition of 5%MAH-PP and damping index decreased about to 60%.
Charpy impact strength also increased up to 60% with the addition of 5%MAH-PP for long wood
fibre-PP composites. Water absorption and scanning electron microscopy of the composites are also
investigated.
Key words: wood fibre-polypropylene composites, maleated polypropylene, fibre length and
geometry, mechanical properties, water absorption.

1. Introduction
Recent studies based on wood fibre-thermoplastic composites have described the
use of wood fibres as low cost reinforcing filler in several thermoplastics [13].
These composites have received attention from industry due to the thermoplastic
nature of wood fibre-thermoplastic composites, which allows processing of the
composites using traditional processing techniques and recycling of the resultant
products or wastes at the end of their useful life.
A recent review report describes the reinforcement of natural and wood fibres
into polymer considering fibre structure, modification of fibre, processing, prop Corresponding author.

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ANDRZEJ K. BLEDZKI AND OMAR FARUK

erties, applications and recent developments of natural and wood fibre reinforced
polymer composites [4].
Wood or lignocellulosic-filled polymer composites have received a lot of attention particularly on the types of fibre, filler characteristics, types of coupling agents
and so forth. The utilisation of wood or in general lignocellulosic material as reinforcing component in polymer composites has become more attractive particularly
for price driven/high volume applications [514].
Still concerning the geometry of the cellulosic fibre, man-made fibres emerging
from a spinneret are cylindrical with approximately constant diameter and specific
area. This is not the case for cellulosic fibres that present many defects caused by
twisting [15] in the stacking of the cellulose chains. These defects are apparent as
knees at the fibre surface and constitute points where the fibre may rapture more
easily. In addition, an important parameter is the aspect ratio (length/diameter),
which has an influence on the mechanical properties of the composite [16]. Bledzki
et al. [17] described that the aspect ratio of wood including its physical structure,
mechanical properties and density change from species to species. For example,
soft wood fibres (spruce) are more flexible compared to fibres derived from aspen
or birch (hard woods).
There has been much work done in the last two decades to bring together
wood fibre, which is an irregular, hygroscopic, thermally sensitive and polar polymer. On the other hand, polypropylene, which is an apolar, hydrophobic, highly
crystalline polymer, requiring relatively high temperature to melt together with a
compounding partner.
The technology of polymer blends and alloys offers nowadays a whole range
of chemical compatibilisers and processing aids. The effect of those processing
aids includes changing surface tensions, promoting fibre wettability, lubricating,
facilitating the fusion of individual resin particles, so lowering the thermal load
(temperature and heating time) during processing, and creating possible physical
or chemical bonds between components.
Many publications have discussed the effectiveness of MAH-PP as a coupling
agent in natural and wood fibre reinforced polymer composites [1827]. MAH-PP
is experimented with wood fibre reinforced polymer composites dependence on
concentration of MAH-PP, different filler content of wood fibre, strength properties
exposure to boiling and cyclic water and oven drying tests, evaluated in an accelerated weather test, shore D hardness test, IR absorption and FTIR studies. The MAH
treated wood-polymer composites showed 23 times more hardness [20] than that
of the untreated composites and MAH treatment restricted swelling and water and
steam absorption in the composites. It was also compared the properties with other
maleated polymer (SEBS-MAH). SEBS-g-MA [21] gave Shore hardness of 78
with respect to 70 for PP and increased simultaneously Youngs modulus (100%),
yield stress (20%) and notched Izod impact strength (24%).
In this work, we have studied the uses of MAH-PP as the coupling agent in
order to prepare different types of wood fibre (hard wood fibre, soft wood fibre,

WOOD FIBRE REINFORCED POLYPROPYLENE COMPOSITES

367

long wood fibre and wood chips) reinforced polypropylene composite with an aim
to be used in automotive and building materials.
2. Experimental
2.1. MATERIALS
2.1.1. Polymeric Matrix
Polypropylene (Stamylan P17M10) was provided as granules by DSM, Gelsenkirchen, Germany. Its melting temperature was 173 C and melting index was
10.5 dg/10 min at 230 C. Its density at room temperature was 0.905 g/cm3 .
2.1.2. Coupling Agent
A commercially available maleic anhydride-polypropylene copolymer (MAH-PP)
was used as a coupling agent for fibre treatment and it was obtained from Clariant
Corp., Frankfurt, Germany. It was used 5% by weight relative to the wood fibre
content and was expected to improve the compatibility and adhesion between the
wood fibre and the PP matrix.
2.1.3. Wood Fibres
Standard hard wood fibre (Lignocel HBS 150-500) and soft wood fibre (Lignocel
BK 40-90) with particle size of 150 m500 m, were supplied by J. Rettenmaier
& Shne GmbH + Co., Germany.
Long wood fibre (particle size 4 mm25 mm) was obtained from Johnson Controls, Lneburg, Germany and wood chips were supplied by Werzalit AG + Co.KG,
Oberstenfeld, Germany.
SEM micrographs (Figures 1 and 2) show the difference of fibre length and
geometry for different types of wood fibres used. It shows that the size variation is
large and that the particles have also great variations in the shape. It can be seen
that the particles are not dispersed and only the cell level and the particles would
be classified as rodlike fibre bundles.
2.2. COMPOUNDING AND SAMPLE PREPARATION
Polypropylene granules with hard wood fibre and soft wood fibre (50% by weight)
were mixed by twin-screw extruder (Haake extruder, Rheomex PTW 25/32) with
and without coupling agent. Long wood fibre and wood chips (50% by weight)
were mixed with PP and coupling agent in a high speed mixer (Henschel, type
HM40 KM120) due to its length. All the wood fibres were initially dried at 80 C
in an air-circulating oven for 24 hours before mixing. The cold agglomerate and
extruded granules were dried again at the same condition (80 C, 24 hours) before
the sample preparation by injection moulding process.

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ANDRZEJ K. BLEDZKI AND OMAR FARUK

Figure 1. SEM micrographs of different used wood fibres before blending [(a) hard wood
fibre, (b) soft wood fibre, (c) long wood fibre and (d) wood chips].

2.3. TESTING
Tensile and flexural tests were performed at a test speed of 2 mm/min according
to EN ISO 527 and EN ISO 178 for different wood fibre-PP composites with and
without coupling agent on a Zwick UPM 1446. All tests were performed at room
temperature (23 C) and at a relative humidity of 50%.
An EN ISO 179 charpy impact test was carried out using 10 unnotched samples.
In each case a standard deviation < 15% (drop weight) was used to calculate the
charpy impact strength.
To measure the impact characteristics values, the specimens were tested by
using a low-velocity falling weight impact tester (EN ISO 6603-2) at room temperature in non-penetration-mode. The impactor had a mass of 0.75 kg and the
impact energy was 0.96 Joules. The results of the impact test can be described by
two separate issues (Figure 3):

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369

Figure 2. SEM micrographs of (a) hard wood fibre, (b) soft wood fibre, (c) long wood fibre
and (d) wood chips.

(a) Force-deflection curve: the force-deflection curve refers to all the materials
behaviours including the damage initiation defined by the first significant drop
of the force.
(b) Characteristic values: loss energy (Wv ) as a measure of dissipated energy and
strain energy (Ws ) as a measure of the stored energy, and the damping index
( ) as ratio of loss energy to strain energy.

2.4. WATER UPTAKE


The water uptake of wood fibre-PP composite samples was measured as a function
of time according to DIN 53495. Specimens (50 50 4 mm) were put in a
water filled container at 23 C for varying lengths (148 hours) of time. The weight
gained by the immersed samples was used to determine the water uptake by the
samples.

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ANDRZEJ K. BLEDZKI AND OMAR FARUK

Figure 3. Typical impact force-deflection curve for natural reinforced polymer composites
including definition of the characteristic values used.

2.5. SEM AND LIGHT MICROSCOPY


The morphology of the wood fibre reinforced PP composites with and without
MAH-PP were investigated using scanning electron microscope (SEM) (VEGA
TESCAN), whereas fractured surfaces of flexural test samples were studied with
SEM after being sputter coated with gold.
3. Results and Discussion
MAH-PP is a well known and widely applied graft copolymer used as a modifier to
enhance the compatibility between fibres and polypropylene. In our previous work
[28], it was investigated that the coupling agent MAH-PP showed best performance
in the concentration of 5% (relative to the wood fibre content) with the wood fibre
composites. Thats why, in our present work the content of MAH-PP was used 5%
for all types of wood fibre-PP composites. With the sufficient fibre loading and
with proper compounding conditions, the mechanical properties of composite are
increased. The various properties of these composites are discussed below.
Tensile properties for the wood fibre-polypropylene composites with the variation of wood fibre (hard wood, soft wood, long wood and wood chips) with and
without coupling agent are shown in Figures 4 and 5. In general, the wood fibrepolypropylene composites showed an increasing trend in mechanical properties
with the addition of MAH-PP. Figure 4 shows that the tensile strength of the composites increases with the addition of 5%MAH-PP in all cases. It also illustrated
that wood chips reinforced polypropylene composites showed the highest strength
while the addition of 5%MAH-PP leads to an increase in strength of nearly 65%. It

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371

Figure 4. Tensile strength of different wood fibre-PP composites with and without coupling
agent [wood fibre content 50% by weight].

Figure 5. Tensile E-modulus of different wood fibre-PP composites with and without
coupling agent [wood fibre content 50% by weight].

indicates that fibre geometry and dimension affect the mechanical properties while
wood chips geometry and dimension is differed from other hard, soft or long wood
fibre which was observed before in Figures 1 and 2.
The change in tensile E-modulus of the composites with 5%MAH-PP followed
the same pattern as that of the strength. The E-modulus increased with 5%MAHPP for all types of wood fibre-PP composites and it maximum increase is 20% for
wood chips reinforced polypropylene composites.
The effect of MAH-PP on the flexural properties of wood fibre-PP composites
can be readily assessed from the Figures 6 and 7. It is observed that the flexural

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ANDRZEJ K. BLEDZKI AND OMAR FARUK

Figure 6. Flexural strength of different wood fibre-PP composites with and without coupling
agent [wood fibre content 50% by weight].

strength (Figure 6) of the composites showed an increasing tendency with the


addition of MAH-PP. Long wood fibre-PP composites showed the higher flexural
strength compare to the other wood fibre-PP composites without 5%MAH-PP. But
with the addition of 5%MAH-PP, the flexural strength of wood chips-PP composites increased the most at which is around 50%. Figure 7 showed that the flexural
E-modulus of the hard wood fibre and soft wood fibre-PP composites were slightly
decreased with the addition of 5%MAH-PP. For wood chips and long wood fibrePP composites, the flexural E-modulus was slightly increased with the addition of
5%MAH-PP. May be fibre length and structure of these two wood fibres plays a
role in the interaction between wood fibre and polypropylene.
Figure 8 shows the variation of charpy impact strength of wood fibre-PP composites with the addition of 5%MAH-PP. From the figure, it is seen that the charpy
impact strength of the hard wood fibre-PP composites are found to be higher than
the other wood fibre-PP composites. However with the addition of 5%MAH-PP
composites, charpy impact strength increased the most for long wood fibre-PP
composites at around 60%.
The impact resistance is the ability of a material and its structure to survive
impact induced damages during an impact issues. The force-deflection curve as
measured in a drop weight impact test refers to associate damage initiation by the
first significant change in the slope of the curve.
Impact resistance of hard wood fibre-PP composites with and without coupling
agent is shown in Figure 9. The improvement in impact resistance of composite
using 5%MAH-PP as a coupling agent is very significant. Figure 10 illustrated the
impact resistance of different wood fire-PP composites with 5%MAH-PP and it is

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373

Figure 7. Flexural E-modulus of different wood fibre-PP composites with and without
coupling agent [wood fibre content 50% by weight].

Figure 8. Charpy impact strength of different wood fibre-PP composites with and without
coupling agent [wood fibre content 50% by weight].

clearly observed that hard wood fibre-PP composites with 5%MAH-PP shows the
highest impact resistance comparative to other wood fibre-PP composites.
Damping index for all samples were calculated by taking the ratio of dissipated energy (loss energy) to the stored energy (strain energy) to measure the
impact characteristic values. The loss energy involves energy which based on irre-

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ANDRZEJ K. BLEDZKI AND OMAR FARUK

Figure 9. Impact resistance (maximum force) of hard wood fibre-PP composites with and
without MAH-PP5% [impact energy 0.96 J, wood fibre content 50% by weight].

Figure 10. Impact resistance (maximum force) of different wood fibre-PP composites with
and without coupling agent [wood fibre content 50% by weight].

versible deformations, energy dissipation due to creation of matrix cracks and their
propagation, debonding, delaminations and finally fibre fracture.
The damping index of different wood fibre-PP composites as a function of
having 5%MAH-PP is shown in Figure 11. It is seen that a relatively high damping index is decreased with the addition of 5%MAH-PP for hard wood fibre-PP
composites around 60%. But without 5%MAH-PP, wood chips and long wood
fibre-PP composites shows smaller damping index than the hard wood and soft
wood fibre-PP composites.

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375

Figure 11. Damping index of different wood fibre-PP composites with and without coupling
agent [wood fibre content 50% by weight].

The flexural fractured surfaces of wood fibre-PP composites with and without 5%MAH-PP examined with SEM are presented in Figures 12 and 13. Figures 12(a) and 13(a) show more fibre pullout, debonding and fibrillation which
are for different wood fibre-PP composites without 5%MAH-PP. The high level
of fibre pullout, debonding and fibrillation for wood fibre-PP composites without
5%MAH-PP is due to the poor adhesion between wood fibres and polymer matrix. Figures 12(b) and 13(b), which represent the microstructure of wood fibre-PP
composites prepared with 5%MAH-PP and the presence of 5%MAH-PP indicate
better interaction between the wood fibre and matrix. These also indicate that there
is some kind of interfacial interaction between wood fibres and PP in the presence
of maleic anhydride. It indicates that maleic anhydride provides good adhesion
between wood fibres and PP. This was expected from the mechanical properties
and lower percentage of water uptake.
The water uptake of soaked samples was also measured as a function of
5%MAH-PP. Results are reported in Figure 14. It can be observed that the wood
fibre-PP composites without MAH-PP show substantially higher water absorption
than the composite with MAH-PP. Indeed, it is well known that the interface between the matrix and wood fibre in composites is an ill-defined but extremely
important part of the material, which can easily allow the absorption of water.
The encapsulation of the fibre with MAH-PP decreases the water sensitivity of the
composite. During the impregnation, MAH-PP reacts with the hydroxyl groups of
the wood fibres to form covalent bonds that are more resistant to water penetration
[29]. Figure 14 also illustrates that long wood fibre and wood chips-PP composites
showed lower hygroscopicity comparative to hard and soft wood fibre-PP com-

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Figure 12. SEM micrographs of fractured surface of hard wood fibre-PP composites [(a) without 5%MAH-PP, (b) with 5%MAH-PP].

Figure 13. SEM micrographs of fractured surface of wood chips-PP composites [(a) without
5%MAH-PP, (b) with 5%MAH-PP].

posites. MAH-PP reduced the hygroscopicity by as much as 75% for soft wood
fibre-PP composites.

4. Conclusions
Four types of wood fibre (hard wood fibre, soft wood fibre, long wood fibre and
wood chips) were used to prepare wood fibre reinforced polypropylene composites.
The effect of coupling agent and fibre length and geometry on the performance of
wood fibre-PP composites has been investigated. From this present investigation,
the following points can be drawn.
Wood chips-PP composites showed better tensile and flexural properties comparative with the other wood fibre-PP composites with the addition of
5%MAH-PP.

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Figure 14. Water uptake of different wood fibre-PP composites with and without coupling
agent [wood fibre content 50% by weight].

A maximum increase in tensile and flexural strength of about 65% and 50%
respectively was observed with the addition of 5%MAH-PP for wood
chips-PP composites.
Hard wood fibre-PP composites showed better impact values compared to
other wood fibre-PP composites with the addition of 5%MAH-PP.
Damping index decreased by 60% with the addition of 5%MAH-PP for hard
wood fibre-PP composites.
Charpy impact strength also increased up to 60% with the addition of
5%MAH-PP for long wood fibre-PP composites.
Long wood fibre and wood chips-PP composites showed lower hygroscopicity
comparative to hard and soft wood fibre-PP composites.
5%MAH-PP reduced the hygroscopicity with a maximum reduction of around
75% for soft wood fibre-PP composites.

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