Materials and Design 65 (2015) 454–461

Contents lists available at ScienceDirect

Materials and Design

journal homepage: www.elsevier.com/locate/matdes

Polypropylene composites based on lignocellulosic fillers: How the filler

morphology affects the composite properties
Ilhem Naghmouchi a, Francesc X. Espinach b, Pere Mutjé c, Sami Boufi a,⇑
a
University of Sfax, Faculty of Science, LMSE, BP 1171-3000 Sfax, Tunisia
b
Design, Development and Product Innovation, Dept. of Organization, Business, University of Girona, c/M. Aurèlia Capmany, n° 61, Girona 17071, Spain
c
Group LEPAMAP, Department of Chemical Engineering, University of Girona, c/M. Aurèlia Capmany, n° 61, Girona 17071, Spain

a r t i c l e i n f o a b s t r a c t

Article history: In this research, composite materials were made from wood flour (WF) or olive stone flour (OSF) as
Received 3 August 2014 reinforcement, polypropylene (PP) as polymer matrix, and maleated polypropylene (MAPP) as coupling agent,
Accepted 16 September 2014 by using injection molding. The effects of the filler loading and coupling agent on the physical properties
Available online 28 September 2014
of the composites, in terms of tensile and impact strength, water absorption and wear resistance were
studied. The macromechanical properties were explained by the morphological features of the reinforce-
Keywords: ments. Composites containing coupling agents exhibited the best mechanical properties, and reduced the
Composites
negative impacts of water absorption. The difference in the morphology of the two lignocellulosic fillers
Wood flour
Olives residue
was found to be a key factor controlling the properties of the composites and the evolution of their prop-
Mechanical properties erties against water absorption.
Ó 2014 Elsevier Ltd. All rights reserved.

1. Introduction
Biomass-fiber-reinforced polymer composites have received
much attention because of their low density, nonabrasive, combus-
tible, nontoxic, low cost, and environmentally friendly properties
[1–3]. Another important property of these reinforcing elements
is their ability for noise insulation, making them candidates for
the manufacture of lightweight soundproofing solutions. The pos-
sibility for energetic recycling at the end of their life is also to be
considered as lignocellulosic fillers are used [4]. Because of all
these attributes, lignocellulosic based composites gained increas-
ing interest of both academic and industrial communities. Poten-
tial markets include: automotive parts for light-weight elements
with soundproofing properties, building profiles such as decking,
siding, fencing, deck boards, wearing surfaces, and window frames
[5]. However, in addition to these advantages, natural fillers have
some disadvantages as well, such as the wide dispersion of their
properties (tensile and flexural strengths, stiffness, morphology. . .)
according to their origin [6]. Furthermore, natural fibers, unlike the
synthetic fibers, are thermally unstable, and its use is limited to
temperatures below 220 °C [7]. Another major drawback concern-
ing natural fillers is their inherent hydrophilic and polar nature,
⇑ Corresponding author. Tel.: +216 74 276 400; fax: +216 74 274 437.
E-mail address: Sami.Boufi@fss.rnu.tn (S. Boufi).
making necessary the use of coupling agents to improve the inter-
facial adhesion between the fibers and the hydrophobic matrixes,
and accordingly to benefit of their reinforcing potential [8].
Agriculture generates co-products, by-products and waste
streams that are currently not properly taken care of both in envi-
ronmental and economic terms. The use of such agricultural mate-
rials, that are largely available throughout the world, as a source of
fillers or reinforcements to the industry not only provides a renew-
able source, but could also generate a non-food source of economic
development for farming and rural areas [9,10]. Furthermore, the
use of biomass for the production of composite materials can be
an interesting option for countries with few wood resources. In
the case of the Mediterranean regions’ olive oil producing countries,
the olive oil extraction processes generates huge amounts of solid
lignocellulosic residue, representing 30% by weight of the olive fruit.
Given the chemical composition of this residue, mainly lignin, hemi-
cellulose and cellulose, different strategies have been developed for
its exploitation, being the most common its incineration for energy
generation [11]. Nonetheless, alternative uses of agricultural
wastes, such as their exploitation as a sustainable reinforcement
for composites, are regarded as potentially important within the
field of materials technology [12–15]. In fact, polypropylene (PP)
ground olive stone residue (OSF) reinforced composite are expected
to show high stiffness values, due to the high hardness of the olive
stones. This has been corroborated by other publications that

http://dx.doi.org/10.1016/j.matdes.2014.09.047
0261-3069/Ó 2014 Elsevier Ltd. All rights reserved.
 I. Naghmouchi et al. / Materials and Design 65 (2015) 454–461
studied the use of OSF reinforced PP [10,11], where it was found that
the stiffness of the composites increased as the OSF content was
increased. However, it was found that properties as tensile strength,
impact strength and water absorption depend on the matrix type,
the coupling agent and the filler treatment.
While wood, OSF and other lignocellulosic fillers showed simi-
lar chemical compositions, the morphology and aspect ratio of
OSF is quite different from the other fillers. Accordingly, it was con-
sidered interesting to investigate to what extent these differences
were likely to affect the mechanical properties, and the water sen-
sitivity of the composite. Within this objective, wood flour (WF)
and OSF reinforced PP composites, with and without MAPP, were
produced and tested. This work studies the evolution of the
mechanical properties against the reinforcing fibers content, as
well as the effects of MAPP presence. It also investigates the effects
of the water absorption on such properties.
2. Materials and methods
2.1. Materials
The composites were prepared using homopolymer polypropyl-
ene, (PP) (Isplen PP090 G2M) which was provided by Repsol-YPF
(Tarragona, Spain) as the polymer matrix. This PP is a fluid injec-
tion-molding grade with a melt flow index of 55 g/10 min (accord-
ing to ISO 1133 standard) to facilitate the dispersion and
processability of the composite material Polypropylene functional-
ized with maleic anhydride (MAH-PP) (Epolene G3015), which
was acquired from Eastman Chemical Products (Spain) and used as
coupling agent to improve the interface adhesion and compatibility
fiber/matrix.
2.2. Methods
2.2.1. Olive stone flour preparation
Olive stone flour (OSF) was obtained from the residues of the
olive oil production. After the separation of the olive oil, the resi-
due is composed of skin (epicard), pulp (mesocarp), and stone
(endocarp). The solid residue was treated with hexane to recover
the remaining oil. Then the residue was dried and separated into
shell and stone by means of screening ventilation. The resulting
stone residue was ground into fine flour that represents about
20–25% of the whole olive fruit.
2.3. Filler characterization
Olive stones were chopped using a knives mill from Agrimsa
(Spain) equipped with a set of sieves. The obtained particles mea-
sured from 50 to 400 lm.
2.3.1. Chemical composition and morphological analysis
The determination of the basic chemical composition was con-
ducted following TAPPI standard protocols. (TAPPI T 257 cm-02)
[16]. Samples were first submitted to Soxhlet extraction with eth-
anol/toluene and water. Then the chemical contents were deter-
mined using the following methods, Ash (Tappi T 211 om-93)
[17], extractive (Tappi T264 om-07) [18], Klason lignin (Tappi
T222 om-88) [19], and hemicelluloses (Tappi T249-cm-85) [20].
The length and aspect ratio of OSF filler were determined by
Morfi analyses using a TECHPAP LB 01 Morfi equipment (fiber con-
tent of 0.300 g/L).
2.4. Preparation of composite
PP composite materials comprising 20–70 wt.% of OSF and WF
were compounded by means of a Brabender internal mixing
455
machine. The mixing process was performed at 80 rpm rotor speed
and a temperature of 190 °C for 10 min. The obtained blends were
ground by means of a knives mill, dried and stored for at least 24 h
before processing. For the coupled composites containing, PP and
MAPP were mixed before the addition of the reinforcement.
The test samples were produced with a steel mold in an
injection-molding machine (Meteor 40, Mateu and Solé). Ten test
specimens from each obtained composite blend were used for
the experiment. The processing temperatures were 175, 175, and
190 °C (the machine has three heating areas), the last correspond-
ing to the injection nozzle. First and second pressures were 120
and 37.5 kgf/cm2, respectively.
2.5. Mechanical characterization
The specimens were stored in a Dycometal conditioning cham-
ber at 23 °C and 50% relative humidity for 48 h, in agreement with
the ASTM: D638-10 standard. Afterwards, composites were
assayed in a Universal testing machine (InstronTM 1122), fitted
with a 5 kN load cell and operating at a rate of 2 mm/min. Young’s
modulus was analyzed using extensometer in dog-bone speci-
mens. The notched Izod impact strength was measured according
to ASTM: D6110-10 using a Zeiss apparatus provided with a ham-
mer of 2.074 kg weight and 382 mm arm length. Results were
obtained from the average of at least 5 samples.
2.6. Scanning electron microscopy (SEM)
Scanning electron microscopy (SEM) was obtained with a Zeiss
DMS 960A, controlled from a computer workstation. Samples were
previously prepared by coating their surfaces with gold by
sputtering.
2.7. Moisture content (Mt)
Coupled and uncoupled composites were immersed in distilled
water at 23 °C for different periods of time, and water uptake was
determined gravimetrically. Moisture absorption (Mt) was deter-
mined by the weight gain relative to the samples’ dry weight.
The moisture content of a sample was computed as follows:
Wt  W0
 
Mt ¼  100 ð1Þ
W0
where W0 and Wt denote the dry weight of the sample and the
weight at any specific time t, respectively.
2.8. Wear resistance
The wear resistance was evaluated by rub–wear action under
specific conditions, measuring the weight loss after certain number
of cycles. The effect of the OSF and WF addition on the wear
behavior of PP–OSF and WF composites was assessed using a Taber
abrasion test.
3. Results and discussion
The chemical composition and morphological features of WF
and OSF are given in Table 1. Both fillers are lignocellulosic mate-
rials composed of three important constituents: cellulose, lignin
and hemicelluloses. OSF showed higher lignin and hemicelluloses
contents than WF, while WF showed higher cellulose contents.
The difference in lignin content could account for the higher stiff-
ness of OSF relative to WF.
Morphological analysis showed that the average fiber lengths
of WF and OSF were 310 ± 50 lm and 125 ± 50 lm respectively.
456 I. Naghmouchi et al. / Materials and Design 65 (2015) 454–461

Table 1 the percentage of reinforcement, this was the expected behavior,

Chemical composition and morphological features of WF and OSF. considering good fiber dispersion inside the matrix. A similar
WF OSF behavior was reported for ONF reinforced Polyvinyl Chloride com-
Constituent posites [15]. On the other hand, the uncoupled composites showed
Asha 0.7 ± 0.5% 5 ± 0.5% a linear increase of the Young’s modulus up to 40% fiber contents,
Extractible 3 ± 0.3% 1.5 ± 0.3% then the value levelled or even fell down. The Young’s module
Hemicellulose 26 ± 2% 35 ± 2% improvements were expected due to the high stiffness of the fillers
Cellulose 45 ± 3% 25 ± 3%
Lignin 25.3 ± 2% 35 ± 2%
compared to that of the matrix. This behavior, already noted for
WF composites, has been assigned to the formation of aggregates
Morphological features
CrI 45 ± 2% 35 ± 2%
of lignocellulosic particles as the filler content exceeds a critical
Average lengtha (lm) 310 ± 50 125 ± 50 threshold [21]. The presence of the coupling agent improved the
Average diametera (lm) 22 ± 2 27 ± 2 compatibility with the matrix via the chemical connectivity thus
Aspect ratio 14 ± 1 4.4 ± 1 reducing the interaction among the lignocellulosic filler and pre-
a
Determined from Morfi analysis. venting the risk of their aggregation.
If the stiffening effects of the two fillers are compared, then it is
observed that the WF has more efficiency than the OSF. Further-
The average diameters of the WF and OSF were found to be
more, as the evolution of the property is almost linear against fiber
22 ± 2 lm and 27 ± 2 lm respectively. The data account for aspect
content, the gap between the Young’s modulus of the WF and the
ratios (ratio between fiber, length and diameter) of 14 and 4.4 for
OSF reinforced composites increases with the fiber content. This
WF and OSF, respectively. SEM observation of the WF and OSF
difference may be due to the lower aspect ratio shown by OSF
(Fig. 1), showed a fibrous shape for WF with broad distribution regarding WF as shown by the SEM analysis (Fig. 1). It is accepted
in length ranging from 100 up to 1000 lm and a narrow width cen-
that the aspect ratio has an important role in the final mechanical
tred on 20 lm. On the other hand OSF showed a rather elliptical characteristics of composite materials. In that sense, Tsai–Pagano
shape, with a fraction being in the granular form and a broad dis-
model [22] (Eq. (2)) and Halpin–Tsai equations incorporate the
tribution in size ranging from 50 to about 400 lm. aspect ratio in the equations. The modulus of the composite with
randomly oriented fibers is given by:
3.1. Mechanical properties
3 11 5 22
Fig. 2 shows the evolution of the Young’s modulus of the com- ECt ¼ E þ E ð2Þ
8 8
posites against the filler contents in the presence or absence of
MAPP. It was found that the Young’s modulus of the composite Here, E11 and E22 are the longitudinal and transversal elastic modu-
materials that incorporated a 5% MAPP, increased steadily with lus, calculated by the Halpin–Tsai equations:

A A

WF WF

B B

OSF OSF

Fig. 1. SEM micrograph showing the particle characteristics of the WF and OSF used in the study.
 I. Naghmouchi et al. / Materials and Design 65 (2015) 454–461 457

7000 7000
with MAPP without MAPP
6000 6000

5000 5000

E (MPa)

E (MPa)
4000 4000

3000 3000

2000 2000
PP+OSF+5%MAPP PP-OSF
1000 PP+WF+5%MAPP PP-WF 1000

0 0
0 10 20 30 40 50 60 70 0 10 20 30 40 50 60 70 80
Filler content (%) Filler content (%)

Fig. 2. Evolution of the tensile modulus vs lignocellulosic filler content for coupled and uncoupled OSF and WF composites.

f f
1 þ 2ðl =d Þgl V f reinforced composites is well known. The use of MAPP coupling
E11 ¼ Em
t ð3Þ agent promotes the interaction between natural fibers and PP
1  gl V f
matrix at the interface thus improving the fibers–matrix compati-
1 þ 2  gt V f bility. The proposed coupling mechanism is hydrogen bonding and
E22 ¼ Em
t ð4Þ
1  gt V f covalent ester linkage generated by the chemical reaction of the
anhydride groups of the MAPP and the hydroxyl groups of the fiber
Being the parameters gl and gt given by:
surface [23]. For uncoupled OSF/PP and WF/PP, the interface
between the fibers and the matrix is poor. That poor interface
ðEtf =Em
t Þ1
gl ¼ f f
ð5Þ can be confirmed by inspection of Fig. 4A and B, which shows
ðEt =Em
f
t Þ þ 2ðl =d Þ the voids between fiber and matrix, and particles that were deb-
ðEtf =Emt Þ1
onded and pulled out from the PP matrix, in contrast with Fig. 4C
gt ¼ ð6Þ and D, which presents the changes in the interface when a coupling
ðEtf =Emt Þþ2
agent is used, with particles tightly bound to the PP matrix.
where l f and d f are the length and the diameter of the ONF. The different behavior of the tensile strength for the composites
Fig. 3 shows the evolution of the tensile strength of the compos- reinforced with WF or OSF may be a consequence of their morphol-
ites against the filler contents in the presence or absence of MAPP. ogy and aspect ratio [24–26]. In fact, in short fibers composites the
The composites prepared without MAPP showed a decrease in ten- aspect ratio is believed to play a key role in the reinforcing capabil-
sile strength with increasing fiber content, indicating that both of ities of a fiber. The axial loads are transmitted to the fiber in form of
WF and OSF are acting as fillers. A similar behavior was found in shear stress along its surface, and then transformed in axial loads
the case of jute strands [21]. On the other hand, when a 5% MAPP inside the fiber. Two cases must be considered depending on the
was added to the composites formulation, the WF based compos- critical length (Lc), which is the minimum length necessary for
ites showed a linear increase in tensile strength up to 60% WF con- the maximum stress in the fiber to reach the fiber fracture stress
tents, then the value levelled. The role of WF changed to that of (Eq. (6)) [27]. Accordingly, subcritical fibers support an average
reinforcement. On the other hand, the composites reinforced with stresses given in Eq. (7), while supercritical fibers carry average
OSF that incorporated a 5% MAPP maintained roughly the same stresses as indicated in Eq. (8). The tensile strength of the compos-
level of their tensile strength when increasing the fiber contents. ites is thus the sum of the contributions from subcritical and
The effect of MAPP in the tensile strength of natural fiber supercritical fibers, and the matrix, following Eq. (9) [21,28]:

With MAPP Without MAPP

60 60

50 50

40 40
σ (MPa)
σ (MPa)

30 30

20 20
PP+OSF+5%MAPP
10 PP+OSF 10
PP+WF+5%MAPP PP+WF

0 0
0 10 20 30 40 50 60 70 0 10 20 30 40 50 60 70 80
Filler content (%) Filler content (%)

Fig. 3. Evolution of the tensile strength vs lignocellulosic filler content for coupled and uncoupled OSF and WF composites.
458 I. Naghmouchi et al. / Materials and Design 65 (2015) 454–461

16
A B
14 OSF+5% MAPP

OSF
12
WF
10
WF+ 5 % MAPP

M∞
8

OSF/PP + 5%MAPP WF/PP + 5%MAPP 2

0
C D 0 10 20 30 40 50 60 70
Filler content (%)

Fig. 6. Plot of M1 vs filler loading for the coupled and uncoupled composite OSF
and WF–PP composite.

of the fillers. During an impact, the energy is absorbed by a set of

mechanisms, matrix deformation, fiber fracture, interfacial deb-
onding, crack deflection and fiber pull-out. The toughest materials
are able to absorb more energy during the fracture propagation
without breaking. Fig. 5 shows the evolution of the notched Charpy
Fig. 4. SEM micrograph of the tensile fractured surface for (A) uncoupled OSF, (B)
uncoupled WF, (C) coupled OSF, and (D) coupled WF. impact strength of the composites against the filler contents in the
presence or absence of MAPP. The addition of MAPP coupling agent
improved the Charpy impact strength for both filler. This is due to
F
rmax
f d the enhancement in the filler–matrix interfacial adhesion in pres-
LFc ¼ ð7Þ ence of MAPP that increased the energy dissipation by interfacial
2s
debonding. However, WF imparted improvements in the impact
LF  s
r F ¼ F
For LF < LFc ð8Þ strengths while OSF contributed to lower this property. The dimi-
"d F
!# nution on the impact properties was also observed in the case of
EF ec d ONF reinforced Polyvinyl Chloride [15]. Here again, the difference
r F ¼ EF ec / 1  For LF P LFc ð9Þ
4sLF in the filler’s morphology is on the origin of the disparity in the
" # "
F
!# impact strength. More specifically, (i) the elliptical shape of OSF
s  LF / EF ec d
rc ¼ F
þ EF ec / 1  þ ð1  /ÞEm e ð10Þ promoted the stress concentration at the tip of the particles;
d 4sLF (ii) the lower WF fiber diameter favored the fiber fracture and fiber
pull-out to be operative, and (iii) the higher aspect ratio of WF
where s and rmaxf are the interfacial shear stress of the composite
promoted also fracture propagation along the interfacial area.
and the tensile strength of the fiber, Em and EF the Young’s modulus
of the matrix and the fiber reinforcement respectively, ec the strain
at break of the composite, and LF and dF the fiber’s mean length and 3.3. Water uptake
diameter, respectively. It is reported that the value of Lc is often
higher than 300 lm [29]. The most serious handicap related to the use of lignocellulosic
filler in composite materials is their high sensitivity to water,
3.2. Impact strength which adversely affects their mechanical performances as well as
their long term durability, namely in outdoor use. This sensitivity
The fracture behavior of polymers is strongly affected by the is not only due to the inherent hydrophilic character of the filler,
addition of rigid particles and is dependent of the shape and size, but also to defects such as voids, pores and cracks in the interfacial
chemical nature, surface structure, volume loading, and orientation zone filler/matrix that favor the diffusion and the accumulation of

5 with MAPP without MAPP 5

4 PP/WF 4
Re (KJ/m )
Re (KJ/m )

PP/WF
2

3 3

2 PP/FNO 2
PP/FNO
1 1

0 0
0 10 20 30 40 50 60 70 80 0 10 20 30 40 50 60 70 80
Filler content (%) Filler content (%)

Fig. 5. Evolution of the notched Charpy impact strength as a function of the lignocellulosic filler loading for WF and OSF, coupled and uncoupled PP composites.
 I. Naghmouchi et al. / Materials and Design 65 (2015) 454–461 459

60 STRENGTH MODULUS
7000

Tensile strength (MPa)

50 PP-WF 6000
(before immersion)
40 5000
PP-OSF

E (MPa)
(before immersion) 4000
30
3000
20
2000
10 PP-WF PP-OSF
(After immersion) (Ater immersion) 1000

0 0
0 10 20 30 40 50 60 0 10 20 30 40 50 60 70
OSF (wt%) OSF (wt%)

Fig. 7. Evolution of the tensile modulus and tensile strength vs filler loading for coupled and uncoupled OSF and WF composites after immersion for 60 days in water.

A 0.4

0.35
Weight loss (%)

0.3

0.25
OSF+5%MAPP
WF+5%MAPP

0.2
0 20 40 60 80
Filler content (%)

PP/60%WF /5%MAPP PP/60% OSF/5%MAPP

Fig. 8. (A) Wear weight loss vs filler content. (B) SEM observation of the surface of coupled composite with 60% WF and OSF.

water within the composite through capillary effect. Furthermore,
the aspect ratio of the filler favors the contact between the fibers
through a percolating path favoring water transport by capillarity
through the filler network [30].
Fig. 6 shows the evolution of the water uptake under immersion
condition of the composites against the filler contents in the pres-
ence or absence of MAPP.
In the case of OSF, the water uptake rapidly increased during
the ten first days and then leveled off reaching the absorption
water equilibrium within about one month of immersion in water
at 25 °C. when comparing WF and OSF-based PP composites
(Fig. 6), it comes out that for both fillers, the addition of the cou-
pling agent led to 20–40% decreases of the water uptake with
respected to the uncoupled sample, namely over a filler content
of 20%. This significant reduction might be attributed to the better
wetting of the OSF particles by the polymer as well as the
improved interfacial adhesion that reduced the water accumula-
tion within the interfacial voids separating the filler and the PP
matrix [21]. Furthermore, it can be seen that the coupled OSF–PP
composite exhibited a lower extent of water absorption over 20%
460 I. Naghmouchi et al. / Materials and Design 65 (2015) 454–461
filler contents. The lower sensitivity of PP–OSF based composites to
water absorption is likely associated with OSF ultrastructure.
Actually, while the OSF particles are compact and exempt of any
porosity (see MEB observation in Fig. 2), WF is known to exhibit
a porous ultrastructure, the presence of which favored the water
accumulation within WF fibers by capillarity [30].
The evolution of the tensile modulus and strength of the
composites, after immersion in water for 40 days, to reach the
adsorption equilibrium, was also studied and the results were
given in Fig. 7.
It was found a dramatic fall in both the Young’s modulus and
tensile strength for WF-PP composites after immersion in water.
Meanwhile, OSF–PP composites showed less sensitivity to water,
with a non-meaningful evolution in modulus and strength after
water absorption. The influence of water ageing on the mechanical
properties was also observed in the case of laminated epoxy–flax
fiber composites [31]. The porous character of WF is likely at the
origin of the higher sensitivity of WF–PP composites to water in
terms of the evolution in the mechanical properties. The diffusion
and the accumulation of water within WF led to the expansion of
lignocellulosic fibers and generated shear stresses that favored
the fiber–matrix debonding, leading to microcracking mechanisms
in the matrix around swollen fibers, leading to a decrease in the
strength of the composite. In addition, the absorption of water by
WF brought plasticization of the fibers and accordingly a decrease
in their stiffness. This explains the drop in the modulus following
the water absorption.
3.4. Wear resistance
Wear or abrasion resistance is an important property for com-
posite material intended for applications exposed to severe wear-
ing actions, such as decking or flooring for indoor and outdoor
use. Results, shown in Fig. 8A indicated an increase in the weight
loss for the composites as the filler content was increased, meaning
that the filler addition made the composite more sensitive to abra-
sion than the neat matrix. In the case of a PVC matrix it was
reported that the addition of wood particles enhanced the wear
resistance of the composite,[32]. The decrease in the wear resis-
tance was likely due to the increase in the stiffness of the compos-
ite as the lignocellulosic filler was added to the PP matrix.
However, the weight loss seems less pronounced for OSF–PP com-
posites than for WF–PP composites. Two reasons might account for
this difference, on the one hand, the higher modulus of the com-
posite when WF was used, and on the other hand the lower surface
roughness of OSF–PP composites compared to that of WF–PP
composites, as confirmed by SEM observation of the surface of both
composites (Fig. 8B).
4. Conclusions
PP composites based on WF and OSF, with filler loading up to
70 wt.%, were prepared by injection molding. The main emphasis
of this study is to show how the morphological features of the
lignocellulosic reinforcement is likely to affect the mechanical
properties and the water sensitivity of the composite. WF and
OSF are two lignocellulosic filler with different morphology. The
former has a fibrous shape with a broad distribution in length,
ranging from 40 lm up to 1000 lm, and narrow distribution in
width, being centred on 20 lm, while the later exhibited elliptical
shape and distribution in size ranging from 50 to about 400 lm.
For the two fillers, the addition of MAPP coupling agent at 5% per
filler was essential to reach the optimum reinforcing effect, in term
of the modulus as well as the strength. However, at the same filler
loading, WF imparted higher tensile modulus and strength than
OSF. This difference in the mechanical properties was assigned to
the difference in the morphology and the aspect ratio between
the two fillers.
The water absorption of the composite under immersion condi-
tion was shown to be also sensitive to the filler type. OSF–PP com-
posite exhibited a lower water absorption than WF–PP composites,
namely over 20% filler content. This resulted in an important fall in
both, the tensile modulus and tensile strength for WF, while the
OSF–PP composites were less water sensitive with non-meaningful
evolutions in modulus and strength after water absorption. The
difference in the filler ultrastructure was proposed to be on the
origin of this important evolution in the composites strengths.
The wear resistance of the composite was sensitive to the filler
content and type. The filler addition made the composite more sen-
sitive to abrasion than the neat matrix. The decrease in the wear
resistance was explained by the increase in the stiffness of the
composite with the lignocellulosic filler. However, the addition of
OSF led to a lower drop in the wear resistance than WF.
Acknowledgments
The authors would like to express their gratitude to ‘‘Ministère
de l’enseignement superieur et de la recherche scientifique de
Tunisie,’’ and OLEVARUM-Company for their financial support of
this research through PNRI grant.
References
[1] Akil HM, Omar MF, Mazuki AAM, Safiee S, Ishak ZAM, Abu Bakar A. Kenaf fiber
reinforced composites: a review. Mater Des 2011;32:4107–21.
[2] Baillie C. Green composites: polymer composites and the
environment. Elsevier; 2004.
[3] Dittenber DB, GangaRao HVS. Critical review of recent publications on use of
natural composites in infrastructure. Compos Part A – Appl Sci Manuf
2012;43:1419–29.
[4] John MJ, Thomas S. Biofibres and biocomposites. Carbohydr Polym
2008;71:343–64.
[5] Ashori A. Wood-plastic composites as promising green-composites for
automotive industries! Bioresour Technol 2008;99:4661–7.
[6] Azwa ZN, Yousif BF, Manalo AC, Karunasena W. A review on the degradability
of polymeric composites based on natural fibres. Mater Des 2013;47:424–42.
[7] Yang HS, Wolcott MP, Kim HS, Kim HJ. Thermal properties of lignocellulosic
filler-thermoplastic polymer bio-composites. J Therm Anal Calorim
2005;82:157–60.
[8] Abdelmouleh M, Boufi S, Belgacem MN, Dufresne A. Short natural-fibre
reinforced polyethylene and natural rubber composites: effect of silane
coupling agents and fibres loading. Compos Sci Technol 2007;67:1627–39.
[9] Nagarajan V, Mohanty AK, Misra M. Sustainable green composites: value
addition to agricultural residues and perennial grasses. ACS Sustainable Chem
Eng 2013;1:325–33.
[10] Kengkhetkit N, Amornsakchai T. A new approach to ‘‘Greening’’ plastic
composites using pineapple leaf waste for performance and cost
effectiveness. Mater Des 2014;55:292–9.
[11] Pattara C, Cappelletti GM, Cichelli A. Recovery and use of olive stones:
commodity, environmental and economic assessment. Renew Sustain Energy
Rev 2010;14:1484–9.
[12] Ihemouchen C, Djidjelli H, Boukerrou A, Fenouillot F, Barres C. Effect of
compatibilizing agents on the mechanical properties of high-density
polyethylene/olive husk flour composites. J Appl Polym Sci 2013;128:2224–9.
[13] Papanicolaou GC, Koutsomitopoulou AF, Sfakianakis A. Effect of thermal
fatigue on the mechanical properties of epoxy matrix composites reinforced
with olive pits powder. J Appl Polym Sci 2012;124:67–76.
[14] Amar B, Salem K, Hocine D, Chadia I, Juan MJ. Study and characterization of
composites materials based on polypropylene loaded with olive husk flour. J
Appl Polym Sci 2011;122:1382–94.
[15] Naghmouchi I, Mutjé P, Boufi S. Polyvinyl chloride composites filled with olive
stone flour: mechanical, thermal, and water absorption properties. J Appl
Polym Sci 2014;131:41083–93.
[16] TAPPI method T257 cm-02. Sampling and preparing wood for analysis. Atlanta,
GA, USA: TAPPI Press; 2002.
[17] TAPPI method T211 om-93. Ash in wood, pulp, paper and paperboard:
combustion at 525 °C. In: TAPPI test methods. Atlanta, GA, USA: TAPPI Press;
2000.
[18] TAPPI method T264 om-07. Wood extractive in ethanol–toluen mixture. In:
Tappi test methods. Atlanta, GA, USA: TAPPI Press; 2007.
[19] TAPPI method T222 om-88. Acid-insoluble lignin in wood and pulp. Atlanta,
GA, USA: TAPPI Press; 1988.
 I. Naghmouchi et al. / Materials and Design 65 (2015) 454–461
[20] TAPPI method T249 cm-85. Carbohydrate composition of extractive free wood
and wood pulp by gas–liquid chromatography. In: Tappi test methods. Atlanta,
GA, USA: TAPPI Press; 1999.
[21] Lopez JP, Boufi S, El Mansouri NE, Mutje P, Vilaseca F. PP composites based on
mechanical pulp, deinked newspaper and jute strands: a comparative study.
Compos Part B – Eng 2012;43:3453–61.
[22] Affdl JCH, Kardos JL. The Halpin–Tsai equations: a review. Polym Eng Sci
1976;16:344–52.
[23] Li QX, Matuana LM. Effectiveness of maleated and acrylic acid-functionalized
polyolefin coupling agents for HDPE–wood-flour composites. J Thermoplast
Compos Mater 2003;16:551–64.
[24] Zimmermann MVG, Turella TC, Santana RMC, Zattera AJ. The influence of wood
flour particle size and content on the rheological, physical, mechanical and
morphological properties of EVA/wood cellular composites. Mater Des
2014;57:660–6.
[25] Vallejos ME, Espinach FX, Julian F, Torres L, Vilaseca F, Mutje P.
Micromechanics of hemp strands in polypropylene composites. Compos Sci
Technol 2012;72:1209–13.
461
[26] Faludi G, Link Z, Renner K, Móczó J, Pukánszky B. Factors determining the
performance of thermoplastic polymer/wood composites; the limiting role of
fiber fracture. Mater Des 2014;61:203–10.
[27] Cox HL. The elasticity and strength of paper and other fibrous materials. Br J
Appl Phys 1952;3:72–9.
[28] Bowyer WH, Bader MG. Reinforcement of thermoplastics by imperfectly
aligned discontinuous fibers. J Mater Sci 1972;7:1315–21.
[29] Belhassen R, Boufi S, Vilaseca F, López JP, Méndez JA, Franco E, et al.
Biocomposites based on Alfa fibers and starch-based biopolymer. Polym Adv
Technol 2009;20:1068–75.
[30] Wang W, Sain M, Cooper PA. Study of moisture absorption in natural fiber
plastic composites. Compos Sci Technol 2006;66:379–86.
[31] Assarar M, Scida D, El Mahi A, Poilâne C, Ayad R. Influence of water ageing on
mechanical properties and damage events of two reinforced composite
materials: flax–fibres and glass–fibres. Mater Des 2011;32:788–95.
[32] Jeamtrakull S, Kositchaiyong A, Markpin T, Rosarpitak V, Sombatsompop N.
Effects of wood constituents and content, and glass fiber reinforcement on
wear behavior of wood/PVC composites. Compos B Eng 2012;43:2721–9.