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4 Please provide city name for the manufacturers ‘Thye
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 Article
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mechanical properties of DOI: 10.1177/0892705712475006

jtc.sagepub.com

polypropylene/recycled
acrylonitrile butadiene
rubber/rice husk powder
composites modified
with silane and acetic
AQ 1 anhydride compound
S. Ragunathan1, H. Ismail1 and K. Hussin2

Abstract
Polypropylene (PP)/recycled acrylonitrile butadiene rubber (NBRr)/rice husk powder
(RHP) composites were fabricated with silane and acetic anhydride (Ac) treatment
agent. The in situ formed RHP-filled PP/NBRr composites were prepared by melt mixing
technique. The mechanical properties of both the treatment methods were investigated
with Instron mechanical analysis and Fourier transform infrared. The results indicated
that Ac treatment was found to exhibit better mechanical properties of RHP-filled PP/
NBRr composites treated with silane. This was due to good compatibility and stronger
interaction between anhydride moieties with PP/NBRr.

Keywords
Mechanical properties, polypropylene, acrylonitrile butadiene rubber, rice husk powder,
acetic anhydride, silane

1
School of Materials and Mineral Resources Engineering, Universiti Sains Malaysia, Nibong Tebal, Penang,
Malaysia
2
School of Environmental Engineering, Universiti Malaysia Perlis, Arau, Perlis, Malaysia

Corresponding author:
H. Ismail, School of Materials and Mineral Resources Engineering, Universiti Sains Malaysia, 14300 Nibong
Tebal, Penang, Malaysia.
Email: hanafi@eng.usm.my

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 2 Journal of Thermoplastic Composite Materials 00(0)

Introduction
In recent years, the incorporation of lignocellulosic materials as reinforcing agents or as
fillers in polymer composites has received an increased attention. The addition of fillers
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.1–4 The main
advantage of lignocellulosic materials upon mineral fillers is their environmental
friendliness. In general, polymer waste is disposed in large landfills causing serious
problems in the environment, while biodegradable materials are envisaged to be an
excellent alternative to tackle this problem by reducing the waste volume. Considerable
amount of studies has been carried out on utilizing natural fillers such as sago, sisal, short
silk fibre, oil palm empty fruit bunch, rice husk ash, jute fibre, rubber wood powder, jute,
hemp, sisal, cotton stalk, kenaf, sugarcane banana fibres and other cellulosic fibres as
reinforcement materials in various waste polymeric materials.4,5 Consequently, it has not
been surprising that the use of lignocellulosic materials in the production of composites
has gained significant importance in various manufacturing fields and industries.5–8
The major disadvantage encountered during the incorporation of natural lig-
nocellulosic materials into polymers is the lack of good interfacial adhesion between the
two components, which results in poor properties of the resulting material.9 The polar
hydroxyl groups on the surface of the lignocellulosic materials have difficulty in forming
a well-bonded interface with a non-polar matrix, as the hydrogen bonds tend to prevent
the wetting of the filler surfaces. Besides, the incorporation of lignocellulosic materials
in a synthetic polymer is often associated with agglomeration as a result of insufficient
dispersion, caused by the tendency of the fillers to 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 materials
are used as fillers, such as esterification,10–18 silane treatment,19,20 graft co-poly-
merization,21 use of compatibilizers,22 plasma treatment23 and treatment with other
chemicals.24 These methods are usually based on the use of reagents that contain
functional groups that are capable of bonding to the hydroxyl groups of the lig-
nocellulosic material, while maintaining good compatibility with the matrix. Interfacial
compatibilization improves the stress transfer between the two components and leads to
the improvement of mechanical and physical properties of the produced composites.
Esterification by means of acetylation and silane treatment is the common chemical
modification procedure that has been studied the most.10–20 However, so far no work has
been reported on mechanical comparison of rice husk powder (RHP) acetylation using
acetic anhydride (Ac) and silane treatment using -aminopropyltrimethoxysilane ( -
APS) for the purpose of manufacturing RHP-filled polypropylene (PP)/recycled acrylo-
AQ 2 nitrile butadiene rubber (NBRr) composites.

2
 Ragunathan et al. 3

AQ 4 Table 1. Materials specification and description.

Material Description Source

Polypropylene (PP) Code: 331; MFI: 14 g/10 min at Titan Pro Polymers (M) Sdn.
230 C; density: 0.9 g cm3 Bhd., Johor, Malaysia
Recycled acrylonitrile Content: 33% of acrylonitrile; Juara One Resources Sdn. Bhd.,
butadiene rubber (NBRr) density: 1.015 g cm3 Penang, Malaysia
Rice husk powder (RHP) Cellulose 35%; hemicellulose Thye Heng Chan Enterprise Sdn.
25%; lignin 20%; ash 17%; Bhd.
density:1.4702 g cm3; size:
300–500 mm
Treatment agent Acetic anhydride (Ac); - Alfa Aesar (M) Sdn. Bhd.
aminopropyltrimethoxysilane
( -APS)

MFI: melt flow index.

The aim of the present work is to evaluate and compare the mechanical properties of
RHP filler PP/NBRr composite utilizing Ac and -APS treatment agents in polymer
waste such as NBRr and PP. Processing stabilization torque, mechanical properties,
Fourier transform infrared (FTIR) and morphological properties of both the composites
were investigated and compared.

Experimental
Materials
The materials used for the preparation of RHP-filled PP/NBRr composites are shown in
Table 1. The rice husk powder (RHP) were ground in a table-type pulverizing machine
(Rong Tsong Precision Technology Co., Product id: RT-34) with speed of 2850 r min1,
sieved at 300–500 mm in particle size and dried at 110 C for 24 h in a vacuum oven to
AQ 3 produce RHP of homogeneous fractions.

Ac treatment
The RHP fibre were dipped in glacial acetic acid for 30 min. The acid was drained and
the fibres were dipped in 50% Ac solution and stirred for 1 h, with filler to solution ratio
at 1:25. A few drops of concentrated sulphuric acid were also added as catalyst. The RHP
fibre is finally washed in distilled water for few times and then dried in the vacuum oven
at 80 C for 24 h.

Silane treatment ( -APS)

The -APS treatment reaction for RHP was carried out in a mixture of water and ethanol
(40/60, vol, respectively). -APS of 3 g was first introduced into 1000 mL of water/
ethanol mixture and was allowed to stand for 1 h. The pH of the solution was maintained

3
 4 Journal of Thermoplastic Composite Materials 00(0)

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 70 70 70 70 70 70 70 70 70
NBRr 30 30 30 30 30 30 30 30 30
RHP – 5 10 15 30 – – – –
Ac-treated RHP – – – – – 5 10 15 30
-APS-treated RHP 5 10 15 30

PP: polypropylene; NBRr: recycled acrylonitrile butadiene rubber; RHP: rice husk powder; -APS:
aminopropyltrimethoxysilane; Ac: acetic anhydride.

at 4 by the addition of acetic acid. Then, 10 g of RHP was added into the solutions and
continuously stirred for 1.5 h. The treated RHP was filtered, dried by air and then by
vacuum oven at 80 C for 24 h.

Processing and sample preparation

PP was mixed with NBRr and RHP at various loading (0, 10, 15, 20 and 30 phr). RHP
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 r min1. PP was soaked in Ac and -
APS for the RHP-treated composite to allow possible in situ grafting of PP and anhy-
AQ 5 dride/carbon chain of -APS by heat during mixing. However, for control sample, PP
was first charged directly into the mixer and melted for 4 min, NBRr was added at the
4th minute, and the RHP was added at 6th minute. The mixture was allowed to further
mix for another 3 min to obtain the stabilization torque. The total mixing time was
9 min for all samples. The recycled NBRr powder was dried for 24 h at 80 C under
vacuum prior to melt mixing in an internal mixer. The compounded samples were com-
pression moulded in a Go-Tech compression moulding machine. For test sample fab-
rication, the composites were pre-heated for 7 min at 180 C, compressed at 1000 psi
for 2 min and then cooled for 2 min into 1 mm thickness sheets. Moulded samples were
then cut into dumbbell shapes with a Wallace die cutter S6/1/6.A according to ASTM
AQ 6 D638.

Tensile test
The tensile properties were measured using an Instron 3366 machine with a cross head
AQ 7 speed of 5 mm min1 at 25 + 3 C, according to ASTM D638. Tensile strength, tensile
modulus and elongation at break (EB) of the each sample were obtained from the average
of five specimens with their corresponding SDs.

4
 Ragunathan et al. 5

Figure 1. Effect of Ac and -APS treatment on the torque–time curves of the RHP-filled PP/NBRr
composites. PP: polypropylene; NBRr: recycled acrylonitrile butadiene rubber; RHP: rice husk
powder; -APS: aminopropyltrimethoxysilane.

FTIR spectroscopic analysis

FTIR spectroscopic analysis of the composites was carried out using Perkin Elmer
AQ 8 Spectrometer 2000 FTIR. Scanned range was predetermined at 400–4000 cm1. All the
samples including control, -APS and Ac-treated RHP filler were characterized individu-
ally by FTIR to confirm the chemical reaction between RHP filler and PP/NBRr matrices.

Fractography studies
The failure mode of the fractured tensile specimens was examined using field emission
scanning electron microscope (Zeiss Supra 36VP-24-58). Scanning electron micro-
graphs were taken at various magnifications. Prior to the scanning electron microscopic
observation, 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 during
examinations.

Results and discussion

Torque development
Comparisons were made in Figure 1 between torque–time curves of untreated RHP with
-APS-treated RHP and Ac-treated RHP-filled PP/NBRr composites at 15 phr of RHP.

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6 Journal of Thermoplastic Composite Materials 00(0)

Figure 2. Effect of Ac and -APS on the stabilization torque of RHP-filled PP/NBRr composites.
PP: polypropylene; NBRr: recycled acrylonitrile butadiene rubber; RHP: rice husk powder; -APS:
aminopropyltrimethoxysilane.

The peak A for -APS-treated RHP-filled PP/NBRr composite is lower than the peak B
for Ac-treated RHP-filled PP/NBRr composite due to lubricant action of -APS. How-
ever, all curves become completely homogenous and stabilized at the end of 6 min mix-
ing time.
The stabilization torque of both -APS-treated RHP and Ac-treated RHP-filled PP/
NBRr composites increased with increasing filler content, with Ac showing higher torque
than -APS (Figure 1). The results explained that both Ac and -APS provided high
viscosity to the composites due to the interaction between functional group of the compa-
tibilizer and coupling agent with RHP or PP/NBRr matrix. Meanwhile, higher stabilization
torque of the Ac treated with RHP might be due to better interaction between RHP and PP/
NBRr matrix, thus increasing the total viscosity of the composites (Figure 2).

Tensile properties
Figures 3 to 5 show the tensile properties of RHP-filled PP/NBRr composites as a func-
tion of filler content together with Ac and -APS contribution. The tensile properties can
be translated to a degree of reinforcement provided by the filler to the composites.2,3
Tensile strength of control sample (PP/NBRr/RHP) is shown in Figure 3. It can be seen
that the tensile strength continuously decreased with increasing RHP filler content. The
decrease in the tensile strength may be due to poor dispersion of the filler in the matrix,
increase in the interfacial defects or debonding between the filler and the matrix4–8 and
filler moisture uptake.

6
Ragunathan et al. 7

Figure 3. Effect of Ac, -APS and filler content on tensile strength of RHP-filled PP/NBRr com-
posites. PP: polypropylene; NBRr: recycled acrylonitrile butadiene rubber; RHP: rice husk powder;
-APS: aminopropyltrimethoxysilane.

Since the RHP is highly hydrophilic in nature, its strong inter-filler hydrogen bonding
allows them to cling together, thus resisting dispersion of the filler, leading to weak inter-
facial bonding with consequent problems such as poor stress transfer, small void spaces,
debonding in the resulting composites and picked up moisture during storage, processing
and testing.8
In order to reduce the surface hydrophilicity, the filler surface is treated with Ac and
-APS. At a similar content, the tensile strength for both the treated PP/NBRr/RHP
composites increased and also showed higher strength than control composites with 42–
50% improvement in Ac and 25–35% in -APS. At similar filler loading, incorporation
of Ac into RHP-filled composites has the highest tensile strength. This improvement was
due to the interaction through chemical bonds between anhydride moiety of the Ac and
the hydroxyl groups in the filler, which would form covalent bonds and ester linkages,
thus improving fibre–matrix bonding.
The general mechanism of reaction between filler’s surface with functional group of
the treatment agent is shown in Figure 4. Since the filler–matrix bonding is improved, the
PP long chains become compatible with the NBRr. The presence of anhydride groups
lowered the surface tension of the filler and increases its wettability with the PP/NBRr
matrix. Furthermore, the sufficient numbers of anhydride moiety allow better diffusion
into the matrix polymer, which indicates easier entanglement with the polymer matrix.
Without anhydride, the only adhesion mechanism is inter-diffusion. With the strengthening

7
8 Journal of Thermoplastic Composite Materials 00(0)

Figure 4. General mechanism of the reaction between fibre’s surface with functional group of the
treatment agent (Ac).

Figure 5. General bond mechanism of silane coupling agent to fibre’s surface.

of interfacial interaction between RHP and PP/NBRr matrix by anhydride, the resultant effi-
cient stress transfer from the PP/NBRr matrix to the fibre leads to enhance in tensile strength.
Compared with untreated PP/NBRr/RHP composites, application of -APS did
resulted in some increment in the tensile strength for all filler content but decreased with
increasing RHP filler content (Figure 3). The result indicates that the use of -APS as

8
Ragunathan et al. 9

Figure 6. Effect of Ac and -APS filler content on EB of RHP-filled PP/NBRr composites. PP:
polypropylene; NBRr: recycled acrylonitrile butadiene rubber; RHP: rice husk powder; -APS:
aminopropyltrimethoxysilane; EB: elongation at break.

coupling agent was proven to be effective in enhancing dispersion, adhesion and com-
patibility of systems consisting of hydrophilic filler and hydrophobic matrix through
modification of polymer–filler interface.24 Figure 5 illustrates the reaction mechanism
that occurs in three steps. First, the alkoxy group in the coupling agent undergoes a
hydrolysis process. Water for the hydrolysis may come from the surface humidity of the
filler (in the case of the silane treatment). Next, the group reacts with the hydroxyl of the
filler surface by hydrogen bond formation. Then, Si–O cross links are formed between
the filler surface and the adjacent functional groups in a condensation reaction with the
elimination of water.
EB of untreated composite and Ac-/ -APS-treated RHP-filled PP/NBRr compo-
sites is shown in Figure 4. EB is maximum for untreated composites up to 5 phr
of filler content, but then decreased steadily at higher filler content. The presence
of -APS and Ac further decreased even though at the lowest filler content. For both
the cases, once the composites become harder and stiffer, the EB is certainly low-
ered. The improved adhesion in the presence of bonding agent restricts the mobility
of polymer segments, which finally results in a reduction in elongation.18 Similar
behaviour has also been reported by many researchers.19–23 They found that the
decrease in EB at lower filler content may be due to low EB of the filler and this
restricts the polymer molecules flowing past between each other. Incorporation of
Ac yield composites with the EB of compatibilized composites lower than that of

9
 10 Journal of Thermoplastic Composite Materials 00(0)

Figure 7. Effect of Ac and -APS treatment on Young’s modulus of RHP-filled PP/NBRr compo-
sites. PP: polypropylene; NBRr: recycled acrylonitrile butadiene rubber; RHP: rice husk powder; -
APS: aminopropyltrimethoxysilane.

-APS-treated composites and untreated composites. The lower EB of the compati-

bilized composites was associated with its higher stiffness as well as dramatic
increase in Young’s modulus due to the rigidity of the composites. The increase
AQ 9 in stiffness upon addition of Ac made the composites more brittle (Figure 6).
In both cases, untreated composite and Ac-treated/ -APS-treated RHP-filled PP/
NBRr composites (Figure 7), increasing filler content resulted in enhanced Young’s
modulus since it represents the stiffness of the composites. The enhanced modulus is
easily understood because filler in fibrous form may carry more tensile load with
increasing filler content. Besides, filler is much stiffer than polymer matrix and
as a result, it adds stiffness to the composites. For overall trend, a better modulus
of about 20–33% was observed at all filler content when Ac was added when com-
pared with their counter parts. First, this improvement could be related to better
adhesion between the fibre and the matrix by chemical interactions. Better adhesion
yields more restriction to deformation capacity of the matrix in the elastic zone and
increasing modulus. According to Zhang et al.,25 the addition of anhydride groups
even at low levels (1–2%) increases the nucleation capacity of fillers for PP and
alters the crystal morphology of PP around the fillers. Consequently, surface crystal-
lization dominates over bulk crystallization and a transcrystalline can be formed
around the fillers. From that it can be seen that the effects of crystallites have much
higher modulus compared with the amorphous regions and resulted in increase in the
modulus.

10
Ragunathan et al. 11

Figure 8. FTIR spectra corresponding to the RHP-filled PP/NBRr composites with or without Ac
and -APS. PP: polypropylene; NBRr: recycled acrylonitrile butadiene rubber; RHP: rice husk pow-
der; -APS: aminopropyltrimethoxysilane; FTIR: Fourier transform infrared.

Result from FTIR analysis can confirm that the improvement in tensile results was
due to the irreversible chemical bonding of the silane onto the cellulose surface through
surface modification with Ac and -APS with the PP/NBRr matrices. Figure 8 presents
FTIR spectra corresponding to the RHP-filled PP/NBRr composites before and after
incorporation of Ac and -APS. All spectra show different bands at around 3200–
3500, 1740 and 1635 cm1, which are associated with the stretching vibrations of the
OH, C¼O and C¼C groups, respectively. Rice husk is mostly composed of cellulose,
hemicellulose, lignins and some pectins. The C–OH of the cellulose backbone (C–O sec-
ondary and C–O primary alcohols) corresponded to the 1056 and 1030 cm1 peaks,
respectively.
As for Ac, an increase in the band at 1260 cm1 corresponding to the ester (CO–O)
group formation and a vibration band at 1740 cm1 corresponding to the carbonyl groups
(C¼O) related to the ester functions for Ac-treated RHP is observed. Similar finding was
observed by Bessadok et al.26 on Alfa fibres modified by chemical treatments with Ac.
As for -APS, the broad intense bands around 1162 and 1105 cm1 were assigned to
the stretching of the –Si–O–cellulose and –Si–O–Si– bonds, respectively. The large band
around 1047 cm1, present in the spectrum of the untreated composite, was attributed to
–Si–OH groups. This band disappeared after the surface modification and was replaced
by a wide band around 1020 cm1, which is a characteristic of –Si–O–Si– moiety.27

11
12 Journal of Thermoplastic Composite Materials 00(0)

Figure 9. (a) Micrograph of tensile fracture surfaces of control untreated RHP-filled PP/NBRr
composites at a magnification of 100 and at different filler contents (5 phr). (b) Micrograph of
tensile fracture surfaces of control untreated RHP-filled PP/NBRr composites at a magnification
of 100 and at different filler contents (15 phr). (c) Micrograph of tensile fracture surfaces of con-
trol untreated RHP-filled PP/NBRr composites at a magnification of 100 and at different filler
contents (30 phr). PP: polypropylene; NBRr: recycled acrylonitrile butadiene rubber; RHP: rice
husk powder.

Morphological properties
Scanning electron microscopy was used to examine the fracture surface of the
composites after tensile testing of the samples. In Figures 9 to 11, the fractured
surfaces of untreated RHP, Ac-treated RHP and -APS-treated RHP-filled PP/
NBRr composites are shown, respectively. Observations indicate poor adhesion
between filler and matrix for all samples especially at higher filler content. In
Figures 10(b) and (c) and 11(b) and (c), it is also possible to observe same patterns
from RHP fillers, which were so weakly bonded to the matrix because of higher
filler content. They have been detached from the matrix during fracture, which
shows decrease in the strength of the composites. If the micrographs of the Ac-
treated RHP with -APS-treated RHP at same filler content were compared, it can

12
Ragunathan et al. 13

Figure 10. (a) Micrograph of tensile fracture surfaces of Ac-treated RHP-filled PP/NBRr compo-
sites at a magnification of 100 and at different filler contents (5 phr). (b) Micrograph of tensile
fracture surfaces of Ac-treated RHP-filled PP/NBRr composites at a magnification of 100 and
at different filler contents (15 phr). (c) Micrograph of tensile fracture surfaces of Ac-treated
RHP-filled PP/NBRr composites at a magnification of 100 and at different filler contents (30 phr).
PP: polypropylene; NBRr: recycled acrylonitrile butadiene rubber; RHP: rice husk powder.

be seen that there are more ductile composites morphology with less filler detach-
ment sites for the Ac-treated composites indicating better adhesion between filler
and matrix compared with the -APS-treated composites. It is also possible to
observe a crack running through the filler for the compatibilized composites.

Conclusion
The following conclusions can be drawn based on the results presented in this work.

1. The processing torque and tensile modulus increased with increasing RHP filler con-
tent for all composites, which were attributed to the brittle nature of RHP filler.
2. Both RHP-treated composites exhibit higher processing stabilization torque,
tensile strength, tensile modulus and EB compared with control (untreated RHP)
composites due to enhance interfacial bonding between RHP filler and PP/NBRr
matrices.

13
14 Journal of Thermoplastic Composite Materials 00(0)

Figure 11. (a) Micrograph of tensile fracture surfaces of -APS-treated RHP-filled PP/NBRr com-
posites at a magnification of 100 and at different filler contents (5 phr). (b) Micrograph of tensile
fracture surfaces of -APS-treated RHP-filled PP/NBRr composites at a magnification of 100 and
at different filler contents (15 phr). (c) Micrograph of tensile fracture surfaces of -APS-treated
RHP-filled PP/NBRr composites at a magnification of 100 and at different filler contents (30 phr).
PP: polypropylene; NBRr: recycled acrylonitrile butadiene rubber; RHP: rice husk powder; -APS:
aminopropyltrimethoxysilane.

3. Ac treatment in comparison with silane ( -APS) treatment was found to exhibit bet-
ter mechanical properties for RHP-filled PP/NBRr composites. This may be due to
the enhanced adhesion between RHP filler and PP/NBRr matrix as shown in the
scanning electron micrographs.

Funding
This research received no specific grant from any funding agency in the public, commer-
cial, or not-for-profit sectors.

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