Enhancement of Processability

of Rice Husk Filled High-density

Polyethylene Composite Profiles

S. PANTHAPULAKKAL, S. LAW AND M. SAIN*

Centre for Biocomposites and Biomaterials Processing
Faculty of Forestry, University of Toronto, Canada

ABSTRACT: The effect of coupling agent and processing aid on the performance
properties of rice husk filled high-density polyethylene (HDPE) composites
was studied. Composite profiles of HDPE filled with 65% rice husk were extruded
using a single screw extruder with die dimensions of 3
8 mm. Processability
and performance properties of the composites were highly dependent on the
concentration of the coupling agent and processing aid in the composite formulation.
Attempt was made to optimize the composite formulation with respect to both
coupling agent and processing aid to attain optimum mechanical and water
absorption properties with an optimum extrusion rate. Incorporation of a terpolymer
(ethylene–acrylic ester–maleic anhydride) based coupling agent enhanced the
properties of the composites with a significant reduction in the extrusion rate.
Addition of processing aid enhanced the extrusion rate and showed a negative
impact on the performance properties. Composites with a coupling agent to
processing aid ratio of 0.73 : 0.59 by weight showed an optimum combination of
performance properties and extrusion rate.

KEY WORDS: biocomposites, rice husk, extruded profiles, HDPE, coupling agents,
processing aids.

INTRODUCTION

OW-COST NATURAL FIBER reinforced thermoplastic composites are

L gaining importance in building, automobile, and other consumer
applications. This is because of their inherent advantages such as low
cost, renewability, biodegradability, low specific gravity, abundance,
high specific strength, and nonabrasiveness [1–5]. Underutilized agricultural

*Author to whom correspondence should be addressed. E-mail: m.sain@utoronto.ca

Journal of THERMOPLASTIC COMPOSITE MATERIALS, Vol. 18—September 2005 445

0892-7057/05/05 0445–14 $10.00/0 DOI: 10.1177/0892705705054398
ß 2005 Sage Publications
446 S. PANTHAPULAKKAL ET AL.

residues and/or by-products of agricultural product processing are rich

resources of lignocellulosic materials, some examples of which include rice,
wheat and corn straw, corncobs, and rice husk [6–8]. Only a minor quantity
of these materials is reserved for animal feed or production of energy and a
major portion is burned in the field creating environmental pollution.
Conversion of these materials into useful industrial products leads to
a win–win situation economically by creating jobs, and ecologically by
alleviating waste disposal problems.
Rice husk is a waste product from the rice mill and consists of 35%
cellulose, 25% hemicellulose, and 20% lignin by weight [9]. The higher
content of silica (94%) in rice husk ash encourages the use of rice husk ash
as inorganic reinforcement for plastics and rubbers [10–13]. However,
only limited number of studies have been reported on rice husk reinforced
plastic composites [14–16]. Like any other lignocellulosic fiber in reinforced
plastic composites, the major concern with using rice husk is the relatively
poor compatibility with hydrophobic thermoplastics, which leads to poor
mechanical properties. Coupling agents are generally used to modify the
fiber–matrix interface and thereby enhance the fiber–matrix adhesion.
Extensive research work has been carried out on interface modification in
natural fiber reinforced composites using external coupling agents [17–23].
In an earlier paper we have reported the effect of various coupling agents on
the performance properties and processability of extruded rice husk filled
high-density polyethylene composite (HDPE) profiles [24].
Press molding, injection molding, and extrusion are the most commonly
used processing techniques for natural fiber reinforced thermoplastic
composites. Enhancement of processability of natural fiber reinforced
thermoplastics is an important issue, as the addition of interphase
modifiers reduces the flow properties of the composites considerably by
increasing the interaction between the fiber and the matrix [24]. On the
other hand, incorporation of processing aid improves processability by
reducing the viscosity of the molten composite. Processability enhance-
ment, while retaining and/or improving the performance properties, is
more economical and can be an added advantage for the natural fiber
composite industry. In the present study, an effort was made to
understand the combined effect of processing aid and coupling agent on
the processability of natural fiber thermoplastic composites. Special
emphasis was given to the effects of the coupling agent and the
processing aid on the mechanical and water absorption properties,
density, and processability of the extruded rice husk filled HDPE
composite profiles. Scanning electron microscopy (SEM) of the fracture
surfaces of the composites was also examined to study the fiber–matrix
interaction.
Enhancement of Processability of HDPE Composite Profiles 447

EXPERIMENTAL

Materials Used

High-density polyethylene (HDPE 5502) from Atofina with a density of

0.954 g/cc and melt flow index of 0.2 g/10 min was used as the matrix. Rice
husk with a density of 1.2 g/cc (80% þ 60 mesh and 20% þ 120 mesh)
obtained from CBI building products was used as the filler. A coupling
agent used was supplied by Atofina, which is a terpolymer based on
ethylene–acrylic ester–maleic anhydride with a molecular weight (Mw) of
120,000 g/mol and with a maleic anhydride content of 3.1%. The structure
of the coupling agent is shown in Figure 1. Metallic stearate based
processing aid (Struktol TPW 104) used in this study was obtained from
Struktol.

Test Specimen Preparation by Extrusion

The formulation of the composites is shown in Table 1. The compounds

were formulated based on 65 : 35 ratio of rice husk to PE (composite A)
and with different ratios of coupling agent and processing aid as detailed in
Table 1. The ratio of coupling agent to processing aid was selected according
to the earlier research done in our laboratory. The amount of coupling agent
and processing aid used in the formulation was based on the total weight of
the composite and was deducted from the PE content. Ingredients were
blended in a high-intensity kinetic mixer (manufactured by Werner and
Pfleiderer Gelimat) at 3200 rpm. with a tip speed of 23 m/s and were
discharged at a pre-set temperature of 185 C. After compounding,
the melted compounds were allowed to cool to room temperature
and then granulated using a C.W. Brabender Granulator (Model S-10-9).

Figure 1. Structure of the coupling agent.

448 S. PANTHAPULAKKAL ET AL.

Table 1. Composition of the compositesa.

Process additives

Composite no. Coupling agent (wt%) Processing aid (wt%)

A 0 0
B 2.5 0
C 0 2
D 0.73 0.59
E 0.73 3.41
F 4.27 0.59
G 4.27 3.41
H 5 2
I 2.5 4
J 2.5 2
a
Base recipe: 65 wt% of rice husk and 35 wt% of HDPE.

The granulated compounds were extruded into strips using a 3/4 in. single
screw extruder with die dimensions of 3
8 mm. Length to diameter (L/D)
ratio and compression ratio of the extruder were 25 : 1 and 3 : 1 respectively.
The respective temperatures for the four different processing zones from the
hopper to horizontal die of the extruder were set as 160/165/170/123 C and
the screw speed was maintained at 4 rpm.

Testing of Extruded Profiles

The test specimens were cut from the profiles as per test specifications.
Their tensile and flexural properties were measured on a standard
computerized testing machine (Sintech Model 20). The tensile properties
were measured in accordance with the ASTM D638 procedure using six
specimens at a cross head rate of 12.5 mm/min. The flexural properties were
measured on six specimens in accordance with the procedure in ASTM
D790 (Method 1, Procedure B) using the aforementioned machine in the
three point bending mode at a cross head speed of 12.5 mm/min and a span
width of 50.8 mm. Izod impact tests followed ASTM D256 procedure using
a pendulum type impact machine and six specimens were tested to obtain a
reliable average and standard deviations. All the mechanical properties were
performed at room temperature.
Water absorption after 2 h of boiling in water and the corresponding
thickness swelling was determined in accordance with ASTM D570. Density
of the profiles was determined according to ASTM D792. Extrusion rate
was measured by measuring the length of the extruded profiles at 5 min
intervals.
Enhancement of Processability of HDPE Composite Profiles 449

Morphological Study

Morphology of tensile fracture surfaces of the composites was examined

using a scanning electron microscope (model Hitachi S-2500) to understand
the matrix interaction in the presence of process additives. The fracture end
of the composites was mounted on aluminium stubs and sputter coated with
a thin layer of gold to avoid electrostatic charge during examination.

RESULTS AND DISCUSSION

Mechanical Properties

Mechanical properties obtained for 65% rice husk filled HDPE

composites with and without coupling agent and processing aid are
shown in Figures 2–4. Figure 2 shows tensile and flexural strength of the
composites A–C. The control sample A (composite without any process
additive) exhibited low tensile and flexural strength, which could be due to
the poor interaction between the hydrophilic rice husk and hydrophobic PE.
The addition of 2.5% of the coupling agent (composite B) enhanced the
tensile and flexural strength by 54.8 and 20%, respectively. This indicates
that the terpolymer based coupling agent improves the interaction, like any

Figure 2. Tensile and flexural strength of the composites with and without process additives.
450 S. PANTHAPULAKKAL ET AL.

Figure 3. Tensile and flexural modulus of the composites with and without process additives.

Figure 4. Izod impact strength of the composites with and without process additives.

other maleated polyolefin, between the rice husk and HDPE. This results in
an efficient stress transfer from the matrix to the fiber. Although tensile and
flexural strength of the composites are enhanced with the coupling agent,
respective moduli of the composites are not altered much by the coupling
agent (Figure 3). On the other hand, the addition of processing aid reduced
the strength and stiffness of the composites (composite C) significantly.
Enhancement of Processability of HDPE Composite Profiles 451

Percentage reduction in the tensile and flexural strength and moduli are 26,
38, 27, and 35% respectively. The drop in both strength and stiffness may be
attributed to the plasticizing effect produced by the processing aid in the
matrix and also to the reduction in the adhesion between the filler and
the matrix in the presence of processing aid. An optimum bonding between
fiber and matrix is needed for good impact strength. Izod impact strength
(un-notched) of the composites (Figure 4) showed significant improvement
with coupling agent, but no noticeable change with processing aid.
Un-notched impact strength reflects the energy required for the initiation
and the propagation of the initiated crack. The improvement in the impact
strength in the presence of coupling agent may be due to the ability of the
interface, formed in the composite, to absorb and redistribute the energy
before the crack initiation.
Tensile fracture surface of the composites with and without coupling
agent and processing aid are shown in Figures 5–7. Figure 6 shows better
interaction between rice husk and HDPE in the presence of coupling agent
than the composite without process additives, where debonding of the fiber
from the matrix is visible (Figure 5). The composite with processing aid
(Figure 7) showed more exposed filler surface and holes in the matrix similar

Figure 5. SEM photomicrographs of rice husk filled HDPE composite (A) profile.
452 S. PANTHAPULAKKAL ET AL.

Figure 6. SEM photomicrographs of rice husk filled HDPE composite (B) with coupling
agent.

Figure 7. SEM photomicrographs of rice husk filled HDPE composite (C) with
processing aid.
Enhancement of Processability of HDPE Composite Profiles 453

to the composite without process additives, which is due to the poor

interaction between the rice husk and HDPE.

Water Absorption Properties

Lignocellulosic fillers are highly susceptible to attack by water, which may

lead to reduction in their performance. Dalvag et al. reported a reduction in
the strength of 30% wood flour filled polypropylene and HDPE after water
absorption and also reported that addition of coupling agent decreases
the reduction in strength [22]. Water absorption and the corresponding
thickness swelling of the control and the composite with coupling agent and
processing aid after boiling in water for 2 h are shown in Figure 8. As
foreseen, addition of coupling agent decreased the water absorption (41%)
and the related change in the dimension (26%) of the composite samples.
The enhanced resistance to water absorption is due to the improved
interaction between rice husk and HDPE, which prevents the water uptake
by the lignocellulosic filler. In contrary, addition of processing aid showed
increased water absorption (11%) and thickness swelling (19%) of the
composite, which also demonstrates the reduced interaction between rice
husk and HDPE in the presence of processing aid.

Figure 8. Water absorption and thickness swelling of the composites with and without
process additives.
454 S. PANTHAPULAKKAL ET AL.

Table 2. Density and extrusion rate of the composites A–Ca.

Composite no. Density (g/cc) Extrusion rate (cm/5 min)

A 1.16 (0.01) 59.1 (1.8)
B 1.18 (0.03) 51.0 (0.5)
C 1.12 (0.05) 72.8 (1.5)
a
Standard deviations are given in parentheses.

Processability and Density

Density and extrusion rate of the rice husk filled HDPE extruded profiles
are summarized in Table 2. It is clear from the table that density of the
composites are not altered much by the presence of coupling agents and
processing aid, whereas extrusion rate of the composites are very much
dependent on the process additives. The extrusion rate of the composite with
coupling agent (B) showed a reduction of 13% over the control. This is due
to the improved bonding between the rice husk and HDPE, resulting in
an increased resistance of the composite to flow under shear. Addition of
processing aid enhanced the extrusion rate significantly (23%) and is
because of the significant reduction in the viscosity of the composite under
shear due to the decreased interaction between the filler and the matrix.
These results indicate that a good balance of properties and extrusion rate
can be achieved by proper selection of coupling agent and processing aid
ratio.

Optimization of Coupling Agent and Processing Aid

Table 3 summarizes the mean and the standard deviation of the

mechanical properties of 65% rice husk filled HDPE composites with
different ratios of coupling agent and processing aid. Tensile, flexural, and
un-notched impact strength of the composites increased by the addition
of coupling agent, while the respective moduli were unaffected by the
addition of coupling agent. The strength and stiffness of the composites
decreased with the addition of processing aid and the effect was more
pronounced at higher ratios of processing aid to coupling agent. This is
attributed to the reduction in the interaction between the filler and the
matrix imparted by the processing aid. However, at a very high ratio of
coupling agent to processing aid (Composite F, as noted in Table 3), the
interaction enhanced by the coupling agent counterbalances the effect of
processing aid, thus leading to an ultimate improvement in the tensile and
flexural strength. Composite formulations, which showed an enhancement
Enhancement of Processability of HDPE Composite Profiles 455

Table 3. Mechanical properties of the rice husk filled HDPE compositesa.

Ratio of Un-notched
coupling agent Tensile Tensile Flexural Flexural izod impact
Composite to processing strength modulus strength modulus strength
no. aid (MPa) (GPa) (MPa) (GPa) (J/m)
A 0/0 13.5 2.39 33.5 2.90 38
(0.8) (0.13) (1.3) (0.13) (5)
B 2.5/0 20.9 2.42 40.2 2.81 80
(0.7) (0.13) (2.0) (0.15) (11)
C 0/2 9.9 1.73 20.8 1.88 37
(0.6) (0.14) (2.1) (0.33) (5)
D 0.73/0.59 16.2 2.26 32.3 2.65 52
(0.6) (0.07) (0.8) (0.06) (7)
E 0.73/3.41 9.0 1.65 18.1 1.71 30
(1.1) (0.11) (2.4) (0.17) (7)
F 4.27/0.59 19.5 2.35 38.6 2.75 77
(0.5) (0.10) (2.2) (0.17) (7)
G 4.27/3.41 10.0 1.79 19.2 1.98 32
(0.4) (0.08) (1.2) (0.14) (2)
H 5/2 16.7 2.20 33.4 2.60 68
(0.6) (0.10) (1.2) (0.12) (13)
I 2.5/4 8.9 1.64 17.6 1.88 27
(0.4) (0.15) (0.4) (0.06) (4)
J 2.5/2 12.7 1.81 25.6 2.10 47
(0.5) (0.13) (1.5) (0.21) (7)
a
Standard deviations are given in parentheses.

in tensile and un-notched impact strength without significantly altering

the tensile and flexural moduli of the control compound, contained
coupling agent to processing aid ratios of 0.73/0.59, 4.27/0.59, and 5/2
respectively.
Water absorption properties and the corresponding thickness swelling,
density, and extrusion rate of the composites A and D–J are summarized
in Table 4. The presence of the processing aid in the composites, adversely
affected the water absorption and the thickness swelling of the composites,
while the presence of the coupling agent enhanced the resistance to absorb
water and the resulting deformation. This was also due to the difference in
the function of the two process additives; the coupling agent enhances the
interaction between rice husk and HDPE, whereas the processing aid
reduces the interaction between the same. Composite formulations, which
show an improvement in the resistance to water absorption and the
corresponding thickness swelling with an enhanced tensile and impact
strength properties contained coupling agent to processing aid ratios of
0.73/0.59, 4.27/0.59, and 5/2 respectively.
456 S. PANTHAPULAKKAL ET AL.

Table 4. Water absorption properties, density, and extrusion rate of the rice
husk filled HDPE compositesa.

Ratio of Water Thickness

coupling agent absorption swelling Extrusion
Composite to processing after 2 h boiling after 2 h boiling Density rate
no. aid in water (%) in water (%) (g/cc) (cm/5 min)
A 0/0 8.3 6.2 1.16 59.1
(2.6) (1.8) (0.01) (1.8)
D 0.73/0.59 6.5 4.4 1.16 61.1
(1.5) (0.9) (0.03) (0.6)
E 0.73/3.41 16.1 9.6 1.10 73.6
(6.4) (5.1) (0.04) (1.9)
F 4.27/0.59 4.2 4.4 1.16 53.2
(1.3) (0.5) (0.03) (0.5)
G 4.27/3.41 6.4 4.8 1.08 60.0
(1.0) (1.2) (0.03) (1.7)
H 5/2 5.1 5.0 1.20 57.7
(1.9) (0.5) (0.02) (0.7)
I 2.5/5 7.5 5.9 1.11 61.8
(2.9) (0.7) (0.03) (1.8)
J 2.5/2 5.6 4.4 1.10 55.3
(0.8) (1.1) (0.04) (0.8)
a
Standard deviations are given in parentheses.

The density of the composites was not influenced much by the process
additive, whereas the extrusion rate of the composites were positively
affected by processing aid and negatively affected by the coupling agent.
Composites with improved or similar extrusion rates and at the same
time exhibiting improved mechanical properties contained a coupling
agent to processing aid ratio of 0.73/0.59. It was clear from the above
that the composite containing a coupling agent to processing aid ratio
of 0.73/0.59 showed an improvement in properties with enhanced
processability.

CONCLUSIONS

The performance properties of the rice husk filled HDPE composite

profiles with different loadings of coupling agent and processing aid were
studied and the conclusions drawn from this study are as follows:
1. Terpolymer based coupling agent enhanced the tensile strength, flexural
strength, and resistance to water absorption properties of the composites
with a reduction in the processability.
Enhancement of Processability of HDPE Composite Profiles 457

2. The addition of processing aid resulted in a reduction in the strength and

stiffness of the composites and the effect is at a higher content of
processing aid in the formulation.
3. The extrusion rate of the composites improved by the incorporation of
processing aid.
4. Processing aid adversely affected water absorption resistance of the
composite.
5. The density of the composites was found to be independent of the
coupling agent and processing aid.
6. Composites containing coupling agent to processing aid ratio of
0.73 : 0.59 provided optimum properties with an enhanced processability
of the composites.

ACKNOWLEDGMENTS

The authors would like to acknowledge MMO-Enabling, Atofina, and

CBI Building Products for the financial and in-kind support for this
project.

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