LPTE #698685, VOL 51, ISS 12

Effects of Acetic Anhydride on the Properties

of Polypropylene(PP)/Recycled Acrylonitrile
Butadiene(NBRr)/Rice Husk Powder(RHP) Composites
Santiagoo Ragunathan, H. Ismail, and K. Hussin
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Effects of Acetic Anhydride on the Properties of Polypropylene(PP)=Recycled Acrylonitrile Butadiene(NBRr)=Rice Husk Powder(RHP) Composites
Santiagoo Ragunathan, H. Ismail, and K. Hussin

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Polymer-Plastics Technology and Engineering, 51: 18, 2012

Copyright # Taylor & Francis Group, LLC
ISSN: 0360-2559 print=1525-6111 online
DOI: 10.1080/03602559.2012.698685

Effects of Acetic Anhydride on the Properties

of Polypropylene(PP)/Recycled Acrylonitrile
Butadiene(NBRr)/Rice Husk Powder(RHP) Composites
Santiagoo Ragunathan1, H. Ismail2, and K. Hussin2

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School of Materials and Mineral Resources Engineering, Universiti Sains Malaysia, Nibong Tebal,
Penang, Malaysia
2
School of Environmental Engineering, Kompleks Pengajian Jejawi,Universiti Malaysia Perlis, Arau,
Perlis, Malaysia

Considerable amount of studies have been carried out on

utilisations natural llers such as sago, sisal, short silk
bre, oil palm empty fruit bunch, rice husk ash, jute bre,
rubber wood powder, jute, hemp, sisal, cotton stalk, kenaf,
sugarcane banana bers and other cellulosic bres as
reinforcement materials in various waste polymeric materials[3,4]. Consequently, it has not been surprising that the use
of lignocellulosic materials in the production of composites
has gained signicant importance in various manufacturing
elds and industry[47].
The main disadvantage encountered during the incorporation of natural lignocellulosic materials into polymers
is the lack of good interfacial adhesion between the two
components, which results in poor properties of the nal
material[8]. The polar hydroxyl groups on the surface of
the lignocellulosic materials have difculty in forming a
wellbonded interface with a non-polar matrix, as the
hydrogen bonds tend to prevent the wetting of the ller
surfaces. Furthermore, the incorporation of lignocellulosic
materials in a synthetic polymer is often associated with
agglomerationas a result of insufcient dispersion, caused
by the tendency of the llers to also form hydrogen bonds
with each other. This incompatibility leads to poor mechanical properties and high water absorption, especially
when the matrix is hydrophilic.
Thus, in order to develop composites with good properties, it is necessary to improve the interface between the
matrix and the lignocellulosic material. There are various
methods for promoting interfacial adhesion in systems
where lignocellulosic[914], silane treatment[15,16], graft
co-polymerization[17], use of compatibilizers[18], plasma
treatment[19], and treatment with other chemicals[20]. These
methods are usually based on the use of reagents, which
contain functional groups that are capable of bonding to
the hydroxyl groups of the lignocellulosic material, while
maintaining good compatibility with the matrix.

PP/NBRr/RHP composites were prepared by incorporation of

rice husk powder at different loadings into PP/NBRr matrix with
an internal mixer at 180
C for 9 min and 50 rpm rotor speed. The
effects of rice husk powder ller loading and acetic anhydride treatment on properties of PP/NBRr/RHP composites were investigated
for processing torque, mechanical properties, water absorption,
swelling behavior, FTIR and SEM. Acetic anhydride-treated
RHP caused a signicant increase in mechanical properties, stabilization torque, water and oil resistance of the PP/NBRr/RHP
composites. Results from FTIR and SEM observations indicate
that better adhesion was observed for all acetic anhydride-treated
composites.
Keywords Acetic anhydride; Morphology; Polypropylene;
Recycled acrylonitrile butadiene rubber; Rice husk
powder; Tensile properties

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INTRODUCTION
In recent years, the incorporation of lignocellulosic
materials as reinforcing agents or as llers in polymer composites has received an increased attention. The addition of
llers has a high impact upon economics for thermoplastics, while a general improvement in certain properties is
also achieved. Lignocellulosic materials exhibit a number
of attractive features including low density, low requirements on processing equipment, less abrasion during
processing, abundance and certainly biodegradability[1,2].
The main advantage of lignocellulosic materials upon
mineral llers is their environmental friendliness.
In general, polymer waste is disposed in large landlls
causing serious problems on the environment, while biodegradable materials are envisaged to be an excellent alternative to tackle this problem, by reducing the waste volume.
Address correspondence to H. Ismail, School of Environmental
Engineering, Kompleks Pengajian Jejawi 3, Universiti Malaysia
Perlis, 02600 Arau, Perlis, Malaysia. E-mail: hana@eng.usm.my

45

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55

60

65

70

75

S. RAGUNATHAN ET AL.

Interfacial compatibilization improves the stress transfer

between the two components and leads to the improvement
of mechanical and physical properties of the produced
80 composites. Esterication by means of acetylation is the
chemical modication procedure, which has been studied
the most[914]. However, so far no work has been reported
on acetylation of RHP using acetic anhydride chemical
treatment for the purpose manufacturing PP=NBRr=
85 RHP composites.
The aim of the present work is to evaluate the effect of
acetic anhydride treatment on rice husk powder as ller in
polymer waste primarily on recycled acrylonitrile butadiene rubber and polypropylene. Processing stabilization
90 torque, mechanical properties, water absorption, swelling
behavior, FTIR and morphological studies of PP=NBRr=
RHP composites were also investigated.
EXPERIMENTAL
Materials
The materials used for the preparation of PP=NBRr=
95
RHP composites are shown in Table 1. The rice husk powQ2 der were ground in a table type pulverizing machine (Rong
Tsong Precision Technology Co. Product Id: RT-34) with
speed of 2850 rpm, sieved at 300500 mm in particle size
100 and dried at 110
C for 24 h in a vacuum oven to produce
rice husk powder of homogeneous fractions.
Acetic Anhydride Treatment
The bers were dipped in glacial acetic acid for 30 min.
The acid was drained, and the bers were dipped in 50%
105 acetic anhydride solution and stirred for 1 h, with ller to
solution ratio at 1:25. A few drops of concentrated sulfuric
acid were also added as catalyze. The bers are nally
washed in distilled water for few times and then dried in
the vacuum oven at 80
C for 24 h.
110

Processing/Sample Preparation
Polypropylene (PP) was mixed with recycled acrylonitrile butadiene rubber (NBRr) and rice husk powder

(RHP) at various loading (0, 10, 15, 20, 30) phr. Rice husk
powder was dried at 110
C for 24 h in a vacuum oven prior
to mixing. A constant PP and NBRr was used at 70 phr and
30 phr, respectively. Table 2 shows the formulation of PP=
NBRr=RHP composites.
The composites were prepared by melt mixing using a
Haake Rheomix Polydrive R 600=610 Mixer at 180 C with
the rotor speed of 50 rpm. PP was charged into the mixing
chamber and melted for 4 min before NBRr was added. At
6 min the RHP was added and the mixing was continued for
another 3 min for a total mixing time of 9 min. PP granules
and NBRr powder were dried for 24 h at 80
C under vacuum
prior to melt mixing in an internal mixer. The compounded
samples were compression-moulded in a Go-Tech compression moulding machine. A seven (7) min of preheating
at 180
C, 2 min of compression at 1000 psi and another
2 min of cooling for sample fabrication. Moulded samples
were cut into dumbbell with a Wallace die cutter S6=1=6.A
according to ASTM D638.
A period of 7-min preheating occurred at 180C, followed by 2 min of compression at 1000 psi and another
2 min of cooling for sample fabrication. Moulded samples
were cut into dumbbell shapes with a Wallace die cutter
S6=1=6.A, according to ASTM D638.

125

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135

Absorption Studies
145
The specimens were dried for 4 h in a vacuum oven at
100
C until a constant weight was attained prior to
immersion in water in thermostated vessels at ambient temperature. Weight gains, after exposure, were recorded by
removal of the specimen from the environment and by 150

Description

Polypropylene(PP)

Homopolymer 6331: Code 3cm=g 0.9: Density

Recycled Acrylonitrile
Butadiene Rubber (NBRr)
Rice Husk Powder (RHP)

Content: 33% of Acrylonitrile Density: 1.0153cm=g

Treatment agent

120

Tensile Test
Tensile tests were carried out according to ASTM D 638
using an Instron machine model 3366. The specimens with
1 mm thickness were cut from the molded sheets using a 140
Wallace die cutter S.A.6=1=6. Tensile modulus, tensile
strength and elongation at break were measured at a
cross-head speed of 5 mm=min and tests were performed
at room temperature (25  3
C).

TABLE 1
Materials specication and description
Material

115

Cellulose 35% Hemicellulose 25% Lignin 20% Ash

17% Density :1.4702cm=g m 500-300: Size
Acetic anhydride

Source
Titan Pro Polymers (M)
Sdn. Bhd. Johor,
Malaysia
Juara One Resources Sdn.
Bhd. Penang, Malaysia
Thye Heng Chan Enterprise
Sdn. Bhd.
Alfa Aesar (M) Sdn Bhd

EFFECTS OF ACETIC ANHYDRIDE ON PP=NBRr=RHP

TABLE 2
Formulation for PP=NBRr=RHP composites
PP=NBRr =RHP composites (phr)
Composite Materials

S1

S2

S3

S4

S5

S6

S7

S8

S9

PP
NBRr
Pure RHP
Acetic anhydride-treated RHP

70
30

70
30
5

70
30
10

70
30
15

70
30
30

70
30

70
30

10

70
30

15

70
30

30

weighing them periodically on a Stanton balance with a

precision of 1 mg. The moisture content at any time t, Mt
as a result of moisture absorption, was calculated by using
Equation (1).

Mt %

W o  Wd
 100%
Wo

where by, Wd and W0 were, weight of dry material (i.e., the

initial weight of the material prior to exposure to the
environment) and weight of moist material. The percentage
equilibrium moisture absorption, Mm, was calculated as an
160 average value of several consecutive measurements that
showed no appreciable additional absorption.
Swelling
ASTM Oil No. 3
Determination of the swelling percentage in ASTM oil
165 No. 3 was carried out in accordance with ASTM D 471 test
method. The test pieces of dimension 30 mm  5 mm 
1 mm were weighed and immersed in ASTM oil No.3 at
room temperature for 70 hours. As for toluene the test,
samples were immersed for 48 hours at room temperature.
170 The swelling percentage of the samples for both ASTM oil
No. 3 and toluene was calculated using Equation. (2).

Swelling %

Fractography Studies
The failure mode of the fracture tensile specimens was
examined using Field Emmision Scanning Electron
Microscope FESEM Model ZEISS 36VP-24-54SUPRA. 185
SEM micrographs were taken at various magnications
for fracture and other observations. Prior to the SEM
observations the fractured ends of the specimens were
mounted on aluminium stubs and were sputter coated
with a thin layer of gold to avoid electrical charging dur- 190
ing examinations.
RESULTS AND DISCUSSION
Processing Properties
Figure 1 shows plot of stabilization torque at end of
mixing 9 min for PP=NBRr=RHP composites. The stabili- 195
zation torque can be a direct measurement for evaluating
the viscosity and processability of molten polymer composite systems. An increase in the torque value means an
increase in the viscosity of the molten polymer composite
systems, whereas processability is decreased. It can be seen 200
that stabilization torque increases gradually with the
increase in ller loading. This is due to the presence of
more rigid ller and interfacial interactions between ller
and matrix, therefore reducing the polymer chains
mobility[22,23].
205

swollen weight  original weight

 100
original weight
2

Fourier Transform Infrared Spectroscopy Analysis

FTIR spectroscopic analysis of the composites was carried out using Perkin Elmer Spectrometer 2000 FTIR. The
ATR (Attenuated Total Reectance) is applied. Scanned
range was 4004000 cm1. Both untreated and acetic
anhydride-treated rice husk powder ller were character180 ized by FTIR to conrm the chemical reaction between
the acetic anhydride and the rice husk powder ller.
175

FIG. 1. Stabilization torque at end of mixing 9 min for PP=NBRr=RHP

composites.

S. RAGUNATHAN ET AL.

At a similar ller loading, the composites with acetic

anhydride-treated ller shows higher stabilization torque
as compared to the composites with untreated ller which
indicates more force is needed for each compounding to
210 be done. This is due to esterication process enhances
interactions between ller and matrix and resulted in the
increases of viscosity of the molten materials for acetic
anhydride-treated RHP. We have reported a similar
observation in our previous study on the PP=NBRr=RHP
215 with PPMAH(Polypropylene Maleic Anyhdride) compatibilization[24], whereby higher stabilization torque resulted
for composites with good interfacial interactions between
RHP and PP=NBRr matrixs.
Tensile Properties
Figure 2 shows plot of tensile strength versus ller loading of PP=NBRr=RHP composites. For composites with
untreated ller, tensile strength decreases with the increasing of ller loading. The reduction of this property may be
because of the weak interaction between ller and matrix as
225 shown in SEM micrographs later in Figure 8. However, for
composites with acetic anhydride-treated ller shows
higher values of tensile strength at similar ller loading.
This was due to the incorporation of non-reinforcing
material into the composites and the inability of RHP to
230 support stress transfer from the PP=NBRr matrices.
The tensile properties of these composites depend on
how RHP is well dispersed in the PP=NBRr matrices.
The tensile strengths at 5 phr and 10 phr RHP remain
almost the same as the tensile strength for the PP=NBRr
235 blends. However, acetic anhydride-treated PP=NBRr=
RHP composites showed signicant increase in tensile
strength. The increases in tensile strength for 5 phr and
10 phr of RHP loading as a result of modication with
acetic anhydride were observed to be about 5.5 MPa and
220

FIG. 2. Tensile strength versus ller loading of PP=NBRr=RHP

composites.

4.1 Mpa, respectively, compared to the PP=NBR=RHP

composites. The ester bond between the hydroxyl group
from RHP and acetic anhydride may enhance the ller
matrix interaction leading to good adhesion.
As mechanical properties of the composite highly
depend on ller dispersion and adhesion of ller in the
disperse matrix phase as shown in the morphological
studies latter. This again due to good stress transfer
between the PP=NBRr matrix and acetic anhydride-treated
RHP. The evidence of better interactions between matrix
and ller can be seen from SEM micrographs shown in
Figure 9.
Similar ndings were reported by Arbelaiz et al.[31],
whereby improvement of stress transfer from the PP matrix
to the ax bre bundle for maleic anhydride treated composites. Jebrane et al.[32] in their research indicated that
the acetylation of lignocelulisic material with acetic anhydride very found to be more readily to interact with lignin.
Hence found to make good interaction with lignocellulosic
materials beside vinyl acetate. Further addition of RHP ller exhibited a decreasing trend in the tensile strength for
both series acetic anhydride-modied and -unmodied
specimen. This observation was attributed to particle
agglomeration due to uneven distribution of llers at high
ller loading. Besides poor ability of RHP llers to absorb
stress and distributing it the PP=NBRr matrix increasing
the stress-concentration points in the composites, which
caused the tensile strength failure[21,26].
Figure 3 shows the elongation at break verses RHP ller
loadings of PP=NBRr=RHP composites. Addition of RHP
to the PP=NBRr=RHP composites exhibited a signicant
decrease in elongation of both acetic anhydride-modied
composites and -unmodied specimens. Elongation at
break shows a decrease of 35% upon the addition of
30 phr of RHP. The decrease in Eb caused by RHP indicates the lignocellulosic ber RHP may act as a hindrance

FIG. 3. Elongation at break versus ber loading of PP=NBRr=RHP

composites.

240

245

250

255 Q3

260

265

270

275

EFFECTS OF ACETIC ANHYDRIDE ON PP=NBRr=RHP

280

285

290

295

300

305

for molecular mobility of the PP=NBRr matrixes. The

brittle behaviour of RHP is also supported by the Young
Modules results, which is discussed later.
However the acetic anhydride-modied composites have
indicated a 15% increase in Eb at 5 phr of RHP. This is
resulted from formation of the ester bond (COO) and evidenced by corresponding carbonyl groups (CO) related
to the ester functions for acetic anhydride. Good matrix
and ller interactions and resulted in higher elongation at
break. The presence of acetic anhydride act a linker to
the RHP ller resulting in greater support and increase in
stiffness. However at higher RHP content the brittle nature
of RHP was exhibited with very small increment of 2% in
Eb at 30 phr of RHP. This due to RHP ller dominant state
in the PP=NBRr=RHP system.
Figure 4 shows plot of tensile modulus versus ller loading of PP=NBRr=RHP composites. Tensile modulus
increases with the increase of ller loading. This observation indicates that the incorporation of RHP ller into
the matrix improves the stiffness of the composites. The
addition of RHP ller into the PP=NBRr matrix reduces
the chains mobility, consequently producing more rigid
composites. At a similar ller loading, tensile modulus
for composites with acetic anhydride-treated ller exhibited
higher tensile modulus compared to composites with
untreated ller. According to Bledzki et al.[26] an increase
in tensile modulus was reported in treated natural vegetable ber due to better interactions between matrix and
ller. Olsen et al.[30] also indicated that formation of covalent bonds between OH groups of cellulose and anhydride
group may be long enough to permit entanglements with
the PP in the interphase. This again supported results for
higher tensile modulus of PP=NBRr=RHP composited in
acetic anhydride-treated RHP llers.

FIG. 4. Tensile modulus versus ller loading of PP=NBRr=RHP

composites.

FIG. 5. Swelling percentage of PP=NBRr=RHP composites with and

without acetic anhydride treatment.

Swelling Test
Figure 5 shows a plot of swelling percentage of PP=
NBRr=RHP composites with and without acetic anhydride
treatment in ASTM oil No. 3 for 70 h. It was found that
swelling percentage increased with increasing of RHP content in both acetic anhydride-treated and untreated PP=
NBRr=RHP composites. This was due to the properties
of natural ber RHP which absorb oil on its surface[3,4,22,23]. However, for the similar composites composition, the treated composites exhibited lower swelling
percentage due to better interaction of RHP particles in
the continuous PP=NBRr matrix, which limit the penetration of oil into the treated composites matrix. This
might due to the ability of acetic anhydride to form better
interaction and a protective layer at the interfacial zone to
consequently prevent the direct diffusion of water and oil
molecules into the composites. We have reported similar
observation on polypropylene-maleic-anhydride (PPMAH)
compatibilization to PP=NBRr=RHP composites in our
previous work[24].

310

315

320

325

FTIR Analysis and Reaction Scheme

330
Figure 6 shows FTIR spectra comparison of untreated
and acetic anhydride-treated ller in the region of
4004000 cm1. The spectra were baseline corrected and
normalized at 1160 cm_1, the major absorbance peak
reecting the C-C ring of the carbohydrate backbone of 335
cellulose. Rice husk is mostly composed of cellulose, hemicellulose, lignins and some pectins. The COH of the cellulose backbone (CO secondary and CO primary alcohols)
corresponded to the 1056 cm1 and 1030 cm1 peaks,
respectively. We also observed an increase of the band at 340
1260 cm1 corresponding to the ester (COO) group formation and a vibration band at 1740 cm1 corresponding
to the carbonyl groups (CO) related to the ester functions
for acetic anhydride-treated RHP. Silmilar ndings were

FIG. 6. FTIR spectra comparison

anhydride-treated RHP ller.

345
Q3 Q8

S. RAGUNATHAN ET AL.

of

untreated

and

acetic

observed by Bessadok et al. on Alfa bers, modied by

chemical treatments acetic anhydride[25].

Water Absorption Properties

Figure 7 shows plot of water absorption of PP=NBRr=
RHP composites with and without acetic anhydride treatment. Each data point represents the average of ve specimens. Water uptake increased with immersion time and
355 increasing ller loading as also reported by other researchers[26,27]. However, in our previous research PP=NBRr=
[28]
Q8 RHP were found to exhibit 2 stage absorption behavior .
The RHP in continues matrix absorb water much easier
compared to the RHP particles encapsulated by NBRr. It
360 can be seen in Figure 7 that ller content had a signicant
effect on water absorption properties of the composites.
350

FIG. 7. Water absorption of PP=NBRr=RHP composites with and

without Acetic anhydride treatment.

It indicates that, the higher the ller content, the higher

the percentage of equilibrium water absorption[27]. This is
due to the fact that, the increases of ller content in composite will increase the number of free OH groups of ligno- 365
cellulosic ber. Free OH groups come in contact with water
through hydrogen bonding which results in water uptake
and weight gain in the composites. At a similar ller loading,
it can be seen that the composites with acetic anhydridetreated ller shows a lower water uptake compared to the 370
composites with untreated ller. This result provides a clear
indication that the RHP treatment with acetic anhydride
enhances the ller-matrix interactions at the interface, thus
decreasing the amount of equilibrium water uptake by the
composites. Ismail et al.[23] reported similar ndings, 375
whereby lower absorption in PP=NR=RHP is attributed to
the ability of the chemical to form a protective layer at the
interfacial zone to consequently prevent the direct diffusion
of water molecules into silane-treated composites.
SEM Micrographs
Figure 8(ab) shows SEM micrographs of fractured surface of PP=NBRr=RHP composites with 15 and 30 phr
RHP loading, respectively. The SEM micrographs shows that
poor adhesion of RHP to the PP=NBRr matrix is the main
factor for the reduction of the tensile strength with an increasing of ller loading in the composites. The incorporation of
RHP ller into the PP=NBRr matrix increases the rigidity
of the material thus reduces the ductility of the composites.
Figure 8(a) shows some noticeable gaps between the ller
and matrix, which is the evidence of poor adhesion between
the ller and matrix. Figure 8(b) shows that the RHP llers
were pulled out from the matrix, which are marked with
the white circles, exhibited more detachment of RHP ller
from the matrix. This is due to the poor dispersion and poor
wettability of the ller by the PP=NBRr matrix.
Figures 9(ab) show SEM micrographs of fractured surface of PP=NBRr=RHP composites with acetic anhydride
ller at 15 phr and 30 phr ller loadings. It can be seen in
Figures 9(ab) with 15 and 30 phr RHP loading,
respectively, good ller and matrix and attachment and
dispersion. The adhesion between ller and matrix were

FIG. 8. (a) SEM micrograps of PP=NBRr=RHP composite without acetic

anhydride for 70=30=15 composition. (b). SEM micrograps of PP=NBRr=
RHP composite without acetic anhydride for 70=30=30 composition.

380

385

390

395

400
Q4

EFFECTS OF ACETIC ANHYDRIDE ON PP=NBRr=RHP

FIG. 9. (a) SEM micrograps of PP=NBRr=RHP composite with acetic

anhydride treatment for 70=30=15 composition. (b). SEM micrograps of
PP=NBRr=RHP composite with acetic anhydride treatment for 70=30=
30 composition.

enhanced with the usage of acetic anhydride. This explains

why higher mechanical properties for PP=NBRr=RHP
were exhibited for acetic anhydride-treated RHP
405 composites. These ndings are supported by the ductile
morphology of the treated composites (Fig. 9b).
CONCLUSIONS
The following conclusions can be made, based on the
results presented in this work.
410

415

420

425

1. The processing torque and tensile modulus and swelling

in oil increases with increasing RHP ller loading in
untreated composites. It is attributed to the brittle
nature of RHP.
2. Acetic anhydride-treated composites exhibits higher
processing stabilization torque, tensile modulus and
elongation at break compared to untreated composites
due to strong interfacial bonding between RHP ller
and PP=NBRr matrices.
3. The acetic anhydride treatment improved the mechanical properties of PP=NBRr=RHP composites. This is
due to the good adhesion between RHP ller and the
PP=NBRr matrices, as shown in the SEM micrograps.
4. Acetic anhydride treatment is effective in reducing water
and oil absorption in PP=NBRr=RHP=composites. This
may due to the ability of acetic anhydride to form better
interactions and a protective layer at the interfacial zone
to consequently prevent the direct diffusion of water
and oil molecules into the composites.
REFERENCES

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435

1. Ismail, H.; Galpaya, D.; Ahmad, Z. Effects of dynamic vulcanization

on tensile properties, morphology and natural weathering of polypropylene=recycled acrylonitrile butadiene rubber (PP=NBRr) blends.
Polym. Plast. Techn. Eng. 2010, 49, 110119.
2. Zhong, O.X.; Ismail, H.; Aziz, N.A.A.; Bakar, A.A. Preparation and
properties of biodegradable polymer lm based on polyvinyl alcohol
and tropical fruit waste our. Composites reinforced with cellulose
based bres. Polym. Plast. Techn. Eng. 2011, 50 (7), 705711.
3. Nabi, S.D.; Jog, J.P. Natural ber polymer composites: A review.
Adv. Polym. Technol. 1999, 18 (4), 351363.

4. Satyanarayana, K.G.; Arizaga, G.G.C.; Wypych, F. Biodegradable

composites based on lignocellulosic bersAn overview. Prog.
Polym. Sci. 2009, 34, 9821021.
5. Tajvidi, M.; Falk, R.H.; Hermanson, J.C. Effect of natural bers on
thermal and mechanical properties of natural ber polypropylene
composites studied by dynamic mechanical analysis. Appl. Polym.
Sci. 2006, 101, 43414349.
6. Ragunathan, S.; Ismail, H.; Hussin, K. Mechanical properties, water
absorption, and swelling behaviour of rice husk powder lled polypropylene=recycled acrylonitrile butadiene rubber (PP=NBRr=RHP)
biocomposites using silane as a coupling agent. BioResources 2011,
6 (4), 37143726.
7. Mohanty, A.K.; Khan, M.A.; Hinrichsen, G. Surface modication of
jute and its inuence on performance of biodegradable jute-fabric=
Biopol composites. Compos. Sci. Technol. 2000, 60, 11151124.
8. Frisoni, G.; Baiardo, M.; Scandola, M.; Lednicka, D.; Cnockaert,
M.C.; Mergaert, J.; Swings, J. Natural cellulose bers: heterogeneous
acetylation kinetics and biodegradation behavior. Biomacromolecules
2001, 2 (2), 476482.
9. Rowell, R.M.; Young, R.A.; Rowell, J.K. Paper and Composites from
Agrobased Resources, CRC Press: Boca Raton, FL, 1997.
10. Khalil, K.A.; Ismail, H.; Ahmad, M.N.; Arrin, A.; Hassan, K. The
effect of various anhydride modications on mechanical properties
and water absorption of oil palm empty fruit bunches reinforced polyester composites. Polym. Int. 2001, 50, 395402.
11. Hill, C.A.S.; Khalil, H.P.S.A.; Hale, M.D. A study of the potential of
acetylation to improve the properties of plant bres. Ind. Crops Prod.
1998, 8, 5363.
12. Sun, R.; Sun, X.F. Structural and thermal characterization of acetylated rice, wheat, rye, and barley straws and poplar wood ber. Ind.
Crops Prod. 2002, 16, 225235.
13. Pothan, L.A.; Thomas, S. Polarity parameters and dynamic mechanical behaviour of chemically modied banana ber reinforced polyester composites. Compos. Sci. 2003, 63, 12311240.
14. Sun, X.F.; Sun, R.C.; Sun, J.X. Acetylation of sugarcane bagasse
using NBS as a catalyst under mild reaction conditions for the production of oil sorption-active materials. Biores. Technol. 2004, 95,
343350.
15. Ichazo, M.N.; Albano, C.; Gonzalez, J.; Perera, R.; Candal, M.V.
Polypropylene=wood our composites: treatments and properties.
Compos. Struct. 2001, 54, 207214.
16. Khalil, H.P.S.A.; Ismail, H. Effect of acetylation and coupling agent
treatments upon biological degradation of plant bre reinforced polyester composites. Polym. Test. 2001, 20, 6575.
17. Mohanty, A.K.; Khan, M.A.; Hinrichsen, G. Inuence of chemical
surface modication on properties of biodegradable jute fabrics
polyester amide composites. Compos. Pt. A 2000, 31, 143150.
18. Nitz, H.; Semke, H.; Landers, R.; Mulhaupt, R. Reactive extrusion of
polycaprolactone compounds containing wood our and lignin. Appl.
Polym. Sci. 2001, 81 (8), 19721984.
19. Mahlberg, R., Niemi, H.E.M., Denes, F., Rowell, R.M. Effect of oxygen and hexamethyldisiloxane plasma on morphology, wettability and
adhesion properties of polypropylene and lignocellulosics. Int. J.
Adhes. Adhes. 1998, 18, 283297.
20. Joseph, K.; Thomas, S.; Pavithran, C. Properties of short sisal
bre-reinforced polyethylene composites. Polymer 1996, 37 (23),
51395149.
21. Tserki, V.; Matzinos, P.; Kokkou, S.; Panayiotou, C. Novel biodegradable composites based on treated lignocellulosic waste our as ller. Part I. Surface modication and characterization of waste our.
Compos. Pt. A 2005, 36, 965974.
22. Premalal, H.G.B.; Ismail, H.; Baharin, A. Comparison of the mechanical properties of rice husk powder lled polypropylene composites with
talc lled polypropylene composites. Polym. Test. 2002, 21, 833839.

440

445

450

455

460

465

470

475

480

485

490

495

500

8
505

510

515

Q5 520

S. RAGUNATHAN ET AL.

23. Ismail, H.; Mega, L. The effects of a compatibilizer and a silane

coupling agent on the mechanical properties of white rice husk ash
lled polypropylene=natural rubber blend. Polym. Plast. Technol.
Eng. 2001, 40, 463478.
24. Ismail, H.; Ragunathan, S.; Hussin, K. The effects of recycled acrylonitrile butadiene rubber content and maleic anhydride modied
polypropylene (PPMAH) on the mixing, tensile properties, swelling
percentage and morphology of polypropylene=recycled acrylonitrile
butadiene rubber=rice husk powder (PP=NBRr=RHP) composites.
Polym. Plast. Technol. Eng. 2010, 49, 13231328.
25. Bessadok, A.; Roudesli, S.; Marais, S.; Follain, N.; Lebrun, L. Alfa
bres for unsaturated polyester composites reinforcement: Effects of
chemical treatments on mechanical and permeation properties.
Compos. Pt. A 2009, 40, 184195.
26. Bledzki, A.K.; Reihmane, S.; Gassan, J. Properties and modication
methods for vegetable bers for natural ber composites. Appl.
Polym. Sci. 59, 13291336.
27. Razavi, N.M.; Jafarzadeh, D.F.; Oromiehie, A.; Langroudi, A.E. Mechanical properties and water absorption behaviour of chopped rice husk
lled polypropylene composites. Iran. Polym. J. 2006, 15, 757766.

28. Ismail, H.; Ragunathan, S.; Hussin, K. Tensile properties, swelling,

and water absorption behavior of rice-husk-powder-lled polypropylene=(recycled acrylonitrile-butadiene rubber) composites. Vinyl
Addit. Technol. 2011, 17 (3), 190197.
29. Hong, C.K.; Hwang, I.; Kim, N.; Park, D.H.; Hwang, B.S.; Nah, C.
Mechanical properties of silanized jute-polypropylene composites.
J. Indust. Eng. Chem. 2008, 14, 7176.
30. Olsen, D.J. Effectiveness of maleated polypropylenes as coupling
agents for wood our=polypropylene composites. The 49th Annual
Technical Conference Antec Society of Plastics Engineers,
Montreal, Canada. 1991, 62, 18861891.
31. Arbelaiz, A.; Fernandez, B.; Ramos, J.A.; Retegi, A.; Llano-Ponte,
R.; Mondragon, I. Mechanical properties of short ax bre bundle=
polypropylene composites: Inuence of matrix=bre modication,
bre content, water uptake and recycling. Comp. Sci. Technol.
2005, 65, 1582159.
32. Jebrane, M.; Harper D.; Labbe, N.; Sebe, G. Comparative determination of the grafting distribution and viscoelastic properties of wood
blocks acetylated by vinyl acetate or acetic anhydride carbohydrates
polyms. 2011, 84 (4), 13141320.

525

530

535

Q6
540

Q7