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Journal of Industrial and Engineering Chemistry 14 (2008) 71–76

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Mechanical properties of silanized jute–polypropylene composites

C.K. Hong a, I. Hwang b, N. Kim b, D.H. Park c, B.S. Hwang d, C. Nah b,*
a
School of Applied Chemical Engineering, Chonnam National University, Gwangju 500-757, Republic of Korea
b
Division of New Materials Engineering, Chonbuk National University, Jeonju 561-756, Republic of Korea
c
Department of Electronic Materials Engineering, Wonkwang University, Iksan 570-749, Republic of Korea
d
Materials Processing Department, Korea Institute of Machine & Materials, Changwon 641-831, Republic of Korea
Received 8 May 2007; accepted 2 July 2007

Abstract
An affordable composite was prepared from jute fibers and polypropylene (PP) in this study. Jute fibers are echo-friendly, low-density materials
yielding considerably lightweight composites with highly specific properties. The surfaces of the jute fibers were silanized to increase the
interfacial adhesion between the jute fiber and the polymer matrix. During the fracture process of the silanized composites, the jute fibers were
broken without complete pullout; much of the PP matrix still coated the fibers, indicating the enhanced degree of adhesion. The tensile and dynamic
mechanical properties of the jute–PP composites were enhanced by the silane treatment as a result of the improved interfacial adhesion between the
silanized jute fiber and the PP matrix.
# 2007 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights reserved.

Keywords: Fiber–matrix; Jute; Natural fiber

1. Introduction matrices [4]. The hydrophilic nature of natural fibers adversely

Global environmental issues have led to a renewed interest
in bio-based materials, with the focus on renewable raw
materials can be biodegradable or recyclable at reasonable cost.
As a result of the increasing demand for environmentally-
friendly materials and the desire to reduce the cost of traditional
fibers, many natural fiber composites have been developed
[1,2]. Natural fibers like banana, cotton, coir, sisal, and jute
have attracted the attention of scientists and technologists for
applications in consumer goods, low-cost housing, and other
civil structures [3]. Natural fibers exhibit many advantageous
properties for use as reinforcement materials for composites.
They are low-density materials yielding considerably light-
weight composites with highly specific properties. Natural
fibers also offer significant cost advantages and benefits
associated with their processing, relative to synthetic fibers.
Also, they are a highly renewable resource, which reduces the
dependency on petroleum oil.
One difficulty that has prevented a more extended utilization
of natural fibers is the lack of strong adhesion to most polymeric
* Corresponding author. Tel.: +82 63 270 4281; fax: +82 63 270 2341.
E-mail address: cnah@chonbuk.ac.kr (C. Nah).
1226-086X/$ – see front matter # 2007 The Korean Society of Industrial and Engineering Chemistry. Published by Elsevier B.V. All rights reserved.
doi:10.1016/j.jiec.2007.07.002
affects adhesion to a hydrophobic matrix, and as a result, there
may cause a loss of strength. The deficient adhesion leads to a
weak load transfer from the matrix to the fibers, which induces
a low reinforcing effect. The mechanical properties of a fiber-
reinforced polymer composite depend not only on the
properties of constituents but also on the degree of interfacial
adhesion between the fiber and the polymer matrix. Poor
interfacial bonding leads to composites, exhibiting rather poor
durability and toughness. To reduce the hydrophilic character
of cellulose fibers and to improve their adhesion properties, it is
necessary to modify the fiber surface [5]. Several methods used
to modify natural fiber surfaces, such as alkali treatment [6,7],
the use of maleic anhydride copolymers [8,9], pre-impregna-
tion of the fiber [10], and the use of silanes [4,5,11–14], have
been proposed.
Recently, natural fibers have been used to reinforce
traditional thermoplastic polymers for automotive applications
[15]. Polypropylene has often been used as the matrix material.
Among the natural fiber-reinforcing materials, jute appears
quite promising because it is relatively inexpensive and
commercially available in a required form. It has higher
strength and modulus than plastic [16] and is a good substitute
for conventional fibers in many applications. In this study, the
chemical surface modification of jute fibers was carried out
72 C.K. Hong et al. / Journal of Industrial and Engineering Chemistry 14 (2008) 71–76
using a silane-coupling agent in a methanol/water medium to
improve its suitability as a reinforcing material. The use of
silanes as coupling agents in reinforced polymer composites of
natural fibers is analogous to that of synthetic fibers [13]. The
reinforcing capability of the modified jute fiber on the
polypropylene (PP) composites was investigated. The silanized
jute–PP composites were characterized using various experi-
mental techniques.
2. Experimental
2.1. Materials
The natural fiber used in this experiment was Bangladesh
jute fiber with a length of 70 mm. The commercial-grade
polypropylene (PP, J-170 homo polypropylene; MI = 28.0 g/
10 min; Honam Petrochemical Corp.) was selected as a
polymer matrix. As a coupling agent, g-glycidoxypropyl
trimethoxy silane (Z-6040, Dow Corning), shown in Fig. 1,
was used.
2.2. Fiber surface treatment
Short jute fibers (ca. 3 mm long) were added into a mixture
of methanol/water (90/10, w/w) and stirred for 12 h at room
temperature to clean the fibers by removing starch and waxes
from the surface. The fibers were then filtered and dried in an
oven at 80 8C for 12 h. For the fiber surface treatment, 2 wt%
silane was dissolved in a methanol/water mixture at room
temperature and the pH of the solution adjusted to 4 with the
addition of acetic acid, according to the procedure reported
previously by Gassan and Bledzki [8]. Silanes are more stable if
they are applied from a slightly acid solution. After the
continuous stirring of the solution for 10 min, the dried jute
fibers were immersed in the solution and stirred for 24 h at room
temperature. The jute fibers were then filtered and dried at
80 8C for 12 h.
2.3. Compounding
Jute–PP composites of various fiber concentrations (1, 5, 10,
and 15 wt%) were prepared using a laboratory internal mixer
(Haake Mess-Technik GMBH, Germany). To prepare the
composites, the chamber temperature was set at 180 8C. Half of
the PP was first added into the mixer for ca. 3 min. After the PP
had melted, jute fibers were mixed with the molten PP for
3 min, and then the rest of PP was added and mixed for 4 min.
The composites were pressed shortly after they were removed
from the internal mixer and cut into pieces using scissors. An
injection-molding machine (SPF-100, Hyundai Precision &
Fig. 1. Structure of the silane-coupling agent.
Industry Co., Ltd.) was used to prepare the specimens for the
mechanical tests.
2.4. Characterization
The silane modification of jute fiber was identified using a
Fourier transform infrared spectrometer (FTIR, Abb Bomem
MB100). A JEOL Scanning Electron Microscope (SEM, JSM-
5900) was used to characterize the fracture surfaces of the
untreated and silane-treated composites, and its effect on the
composite properties. An Instron UTM 8872 instrument was
used for the tensile property measurements, according to
ASTM D638. All tests were performed at room temperature
with a crosshead speed of 5 mm/min. The dynamic mechanical
properties of the jute–PP composites were measured using a
dynamic mechanical analyzer (DMA938, TA Instruments)
operated at a heating rate of 5 8C/min and a frequency of 10 Hz.
The dimensions of each sample were 50.0  12.3  3.0 mm.
3. Results and discussion
3.1. Silane treatment
The surface of the jute fibers was modified using an
organofunctional silane to promote adhesion with the PP
matrix. The primary component of jute fiber is cellulose, which
contains numerous hydroxyl groups that are strongly hydro-
philic [17]. In general, the use of coupling agents, such as
silanes, significantly improves the mechanical properties of the
composites. The possible reaction mechanism of the silane
treatment is shown in Fig. 2.
Firstly, the methoxyl groups in the silane are hydrolyzed to
hydroxyl groups (silantriol) in methanol/water solutions
[12,13]. Water is responsible for the hydrolysis of the methoxyl
groups. Secondly, the silanol groups created in the first step
react with hydroxyl groups on the surface of jute cellulose.
There is a possibility of a direct condensation reaction between
the silanol groups (Si–OH) and hydroxyl groups on the jute
fiber. This reaction would create a covalent bond between jute
cellulose and the silanol group (jute–O–Si). The remaining
silanol groups are capable of hydrogen bonding or condensing
with adjacent silanol groups (Si–O–Si). Finally, the hydro-
phobic part of the silane on the jute surface could chemically
bond or interact through van der Waals forces with the PP
matrix. The chemical bonding at the fiber–matrix interfaces is
critically important to understanding the interfacial strength in
natural fiber-reinforced polymer composites.
Fig. 3 shows the FTIR spectra of untreated and silanized jute
fibers in the region 1700–700 cm1. Both untreated and
silanized jute fibers were characterized by FTIR spectroscopy
to confirm the chemical reaction between the silane and the jute
cellulose. The silanized jute fiber reveals an absorption peak at
ca. 800 cm1 that could be assigned to a Si–O–Si bond [11,12].
A peak found at ca. 850 cm1 in the spectrum of the silanized
jute corresponds to a Si–cellulose bond and a new peak at ca.
930 cm1 could be due to asymmetric stretching of Si–O–Si or
cellulose–O–Si bonds [13,18]. These features could be due to
 C.K. Hong et al. / Journal of Industrial and Engineering Chemistry 14 (2008) 71–76
Fig. 2. Reaction mechanism of a silane-treated jute–PP composite.
some silane reactions with jute fibers occurring through direct
condensation reactions between the hydrolyzed silane and the
hydroxyl groups of the jute cellulose. The peak near 1060 cm1
of the treated fiber is related to residual unhydrolyzed Si–O–
CH3 groups; their small intensity suggests that most of the
silane had been hydrolyzed [5]. Also, the spectrum of the
silanized jute fiber shows a peak at ca. 1190 cm1 assigned to
the cellulose–Si–O or Si–O–Si linkages [5]. Such an absorption
Fig. 3. FTIR spectra from 1700 to 700 cm1 of untreated and silanized jute
fibers.
73
band for cellulose–O–Si assures condensation reactions had
occurred between the cellulose of the jute fibers and the silanol
group, and the band for Si–O–Si is an indication of
intermolecular condensation having occurred between adjacent
silanol groups deposited on the fibers [13].
3.2. SEM analysis of fracture surfaces
SEM micrographs of the fracture surfaces of the untreated
and silanized jute–PP composites with 15 wt% jute fibers are
shown in Fig. 4. The surface of the untreated fiber is quite
smooth and there is no evidence or trace of any matrix resin
adhering to the jute fiber. Considerable fiber pullout is also
visible in the fracture surface of the untreated composite.
However, in the case of the silanized fiber, jute fibers were
broken without complete pullout during the fracture process
and there was much PP matrix still coating the fibers. It was also
noted that the fiber failed by tearing, but no complete interfacial
failure was observed, indicating that adhesion between the
silanized jute fiber and the PP matrix was quite good for
reinforcing. The silane treatment of the jute fiber modified its
surface properties and increased the fiber–matrix interaction.
Generally, the mechanical properties of composites depend on
the properties of the matrix and the fiber, and the bond strength,
among other factors.
3.3. Tensile properties
The tensile properties were investigated to observe the
reinforcement effects of the untreated and silanized jute fibers.
74 C.K. Hong et al. / Journal of Industrial and Engineering Chemistry 14 (2008) 71–76
Fig. 4. SEM micrographs of 15 wt% jute–PP composites: (a) untreated and (b) silanized.
Fig. 5 shows the tensile modulus of the untreated and silanized
jute–PP composites at various jute fiber concentrations. The
modulus of the composites increased with increasing the jute
content.
However, the optimum fiber content would vary with the
nature of the fiber and matrix, the fiber aspect ratio, and the
fiber–matrix adhesion [7]. It is also evident that the tensile
modulus of the jute–PP composite was increased slightly by
silane treatment of the jute fiber, excepting the case of the
5 wt% jute content. The increase in modulus of the silanized
composite was most likely caused by improved adhesion
between the jute fiber and the PP matrix. Improved adhesion
between jute and PP makes it possible for stress transfer to
occur from the weaker plastic matrix to the stronger jute fiber
during loading, thereby improving the strength of the
composites [12]. The improved interfacial adhesion could be
due to some chemical bonding between the hydrophobic part of
the silane on the jute surface and the PP matrix or van der Waals
forces between them. Moreover, covalent bonding between jute
cellulose and the PP matrix could also improve adhesion
between the phases.
Fig. 6 shows the stress–strain curves of PP plastic and the
untreated and silanized jute–PP composites containing 1 and
Fig. 5. Tensile moduli of untreated and silanized jute–PP composites.
15 wt% jute. The curves indicate that silane treatment of the
jute fiber yielded a stronger and more ductile composite
material by improving the interfacial adhesion. In the case of
the untreated composite containing 1 wt% fiber, the tensile
properties deteriorated as a result of poor interfacial adhesion
between the hydrophilic jute fibers and the hydrophobic PP
matrix. To obtain natural fiber composites with satisfactory
mechanical properties, strong interfacial adhesion and effective
wetting of the fiber by the matrix are required [19]. Increasing
the fiber content resulted in the improvement in stiffness of the
composites.
3.4. Thermomechanical properties
Dynamic mechanical measurements over a wide temperature
range are useful for understanding the viscoelastic behavior and
provide valuable insight into the relationship between the
structures and properties of composite materials. The storage
modulus is useful in assessing the molecular basis of the
mechanical properties of a material because it is very sensitive to
structural changes, such as fiber–matrix interfacial bonding [20].
Fig. 7 shows the storage modulus of pure PP and the untreated
and silanized jute–PP composites containing 15 wt% jute fiber as
Fig. 6. Stress–strain curves of PP, untreated and silanized jute–PP composites
with 1 and 15 wt% fiber contents.
 C.K. Hong et al. / Journal of Industrial and Engineering Chemistry 14 (2008) 71–76 75

Fig. 7. Storage modulus, E0 , of PP, untreated and silanized jute–PP composites Fig. 8. Loss modulus, E00 , of PP and the untreated and silanized jute–PP
with 15 wt% fiber content. composites containing 15 wt% fiber.

a function of temperature. The values of the storage modulus

dropped as the temperature increased. The storage modulus
improved significantly with the addition of jute fiber to pure PP
over the whole range of testing temperatures as a result of the
reinforcement imparted by the fiber, which allowed stress
transfer to occur at the interface. A much enhanced storage
modulus of the composites was obtained for the silanized jute.
This situation can be explained as a result of improved
interfacial adhesion or chemical bonding between silanized jute
cellulose and the PP matrix. Table 1 lists the increments in
storage modulus of jute–PP composites with various jute fiber
contents at three different temperatures. The storage modulus of
the silanized composites were more improved than those of the
untreated composites and the increment of the storage modulus
increased with increasing temperature. The storage modulus
gives an idea of the stiffness behavior and load-bearing capability Fig. 9. tan d of PP and the untreated and silanized jute–PP composites contain-
of a composite material. Therefore, it is expected that the ing 15 wt% fiber.
silanized jute–PP composites would have greater load-bearing
ability than would pure PP and the untreated composites. which is sometimes considered as the glass transition
Fig. 8 presents the loss modulus of PP and the untreated and temperature (Tg) of the material [21]. The loss modulus peak
silanized jute–PP composites containing 15 wt% jute fiber as a of pure PP appeared at ca. 11 8C; it increased to 15 8C with
function of temperature. The silanized jute composite produced addition of jute fiber. In the silanized jute–PP composite, the peak
higher values of loss modulus than did the pure PP and untreated shifted to higher temperature. This result is due to immobiliza-
jute composites. The loss modulus is proportional to the amount tion of the polymer molecules near the surface of the jute fibers
of energy that dissipated as heat by the material. The loss because of the improved interfacial adhesion, which increased
modulus peak is attributed to the mobility of the resin molecules, the glass transition temperature of the composites [6,21].

Table 1
Storage modulus of jute–PP composites with various jute fiber contents at three different temperatures
Fiber content (wt%) Storage modulus (GPa)
0 8C 60 8C 120 8C
Untreated Silanized Untreated Silanized Untreated Silanized
0 2.07 0.71 0.19
1 2.23 (7.7%) 2.50 (20.7%) 0.74 (4.0%) 0.94 (32.4%) 0.22 (17.3%) 0.31 (63.2%)
5 2.45 (18.4%) 2.54 (22.7%) 1.01 (42.7%) 1.08 (52.1%) 0.36 (91.9%) 0.38 (100.0%)
10 2.81 (35.7%) 3.16 (52.6%) 1.24 (75.1%) 1.63 (129.6%) 0.52 (181.1%) 0.67 (252.6%)
15 3.20 (54.6%) 3.65 (76.3%) 1.53 (116.1%) 1.87 (163.4%) 0.65 (249.2%) 0.79 (315.8%)
The value in parenthesis represents the increment of storage modulus relative to that of pure PP.
76 C.K. Hong et al. / Journal of Industrial and Engineering Chemistry 14 (2008) 71–76
The values of tan d, the ratio of viscous to elastic properties,
of PP and the untreated and silanized jute–PP composites
containing 15 wt% jute fiber are shown in Fig. 9 as a function of
temperature. The value of tan d, the damping energy ratio, is an
indication of the molecular motions existing in the materials. In
a composite, molecular motion at the interface contributes to
damping of the composites [13]. The lowering of tan d values
suggests the restraining effect of the fibers on the matrix
mobility [22]. This restriction is enhanced with silane treatment
of the jute fiber. The improved interfacial adhesion tends to
reduce the mobility of the molecular chain at the interface and
reduces tan d values accordingly.
4. Conclusions
In this study, the surface of jute fiber was modified using an
organofunctional silane to promote adhesion with a PP matrix,
and the reinforcing capability of the modified jute fibers on the
PP composites was investigated. Silane treatment of the jute
fibers increased the fiber–matrix interaction through a
condensation reaction between hydrolyzed silane and hydroxyl
groups of jute cellulose. During the fracture process of silanized
composites, the jute fibers were broken without complete
pullout and there much of the PP matrix remained surrounding
the fibers. Silane treatment increased the tensile properties of
the jute–PP composites, caused by improved adhesion between
the silanized jute fiber and the PP matrix. The silanized jute
composites exhibited greater dynamic mechanical properties
than did the untreated jute composites.
Acknowledgments
This study was supported partly by the Korea Electrical
Engineering & Science Research Institute (R-2005-7-100) and
sponsored by the Ministry of Commerce, Industry, and Energy.
CN thanks Dr. Hwang of the KIMM at Changwon for financial
support.
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