Composites: Part B 68 (2015) 200–206

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Composites: Part B
journal homepage: www.elsevier.com/locate/compositesb

Strength improvement in injection-molded jute-fiber-reinforced

polylactide green-composites
Yoshihiko Arao a,⇑, Takayasu Fujiura b, Satoshi Itani c, Tatsuya Tanaka a
a
Doshisha University, Department of Mechanical and Systems Engineering, 1-3 Tataramiyakodani, Kyotanabe, Kyoto, Japan
b
Kobe Steel, Mechanical Engineering Research Laboratory, 1-5-5 Takatsukadai, Kobe, Hyogo, Japan
c
Graduate School of Doshisha University, 1-3 Tataramiyakodani, Kyotanabe, Kyoto, Japan

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

Article history: The mechanical properties of green-composites based on polylactic acid (PLA) with jute fibers were
Received 27 May 2014 investigated. A long fiber pellet was developed to obtain a high aspect ratio of residual fiber after injection
Received in revised form 18 August 2014 molding. Comparative studies were carried out, where shorter fiber pellets were compounded by differ-
Accepted 20 August 2014
ent screw configurations using a twin-screw extruder. To interpret the results of our mechanical tests, the
Available online 6 September 2014
fiber geometry, dispersion state, and fiber fracture surfaces after tensile testing were analyzed. We found
that the composites made of short fiber pellet (which suffer high compound intensity), exhibited optimal
Keywords:
mechanical performance. Although, compounding with a twin-screw extruder decreased the overall
A. Polymer-matrix composites (PMCs)
B. Strength
aspect ratio of residual fibers, we observed that it significantly facilitated both the dispersion of the jute
E. Injection molding yarn to jute bundle and the decohesion of jute bundle to elementary fibers. This fiber separation caused
by high intensity mixing led to efficient load transfer from matrix to fiber, and improvement of interfacial
strength. These findings provide us with an insight into the critical parameters required to develop a high
performing jute/PLA composite.
Ó 2014 Elsevier Ltd. All rights reserved.

1. Introduction the drawbacks of these natural fiber reinforced green-composites

In recent years, the use of natural products has increased due to
its low environmental impact. For example, the energy production
of natural fibers such as jute, flax, and hemp is significantly lower
than that of conventional reinforcement fiber including glass and
carbon. The growth of natural fiber has also contributed to the
reduction of carbon dioxide in the atmosphere. In addition, the
density of natural fibers (1.3–1.5 g/cm3) is much lower than that
of glass (2.5 g/cm3). In fact, natural fiber reinforced composites
have generated wide interest in various engineering fields, partic-
ularly automotive applications, owing to their high specific
strength, durability, lightweight (high modulus/density ratio) and
low cost production [1].
Systems including polypropylene (PP) and natural fibers are
commonly used for such purposes owing to their increased pro-
cessability and cost performance. Recently, the use of biodegrad-
able materials such as polylactic acid (PLA) has gradually
increased due to their apparent ease of disposal [2]. Despite this,
⇑ Corresponding author. Tel.: +81 774 65 6832.
E-mail address: yoshihiko.arao@gmail.com (Y. Arao).
include their cost and poor mechanical properties in comparison
to composites constructed of glass fibers (GF) and PP [3–5]. There-
fore, to extend the use of fully bio-based composites, higher
mechanical performance is required.
GF/PP composites are widely used as secondary structures and
their mechanical properties are dominated by the length of the
fiber [6–9]. The high aspect ratio of these fibers after processing
leads to higher tensile and impact strengths. This is achieved
through the use of long fiber pellets and appropriate injection tech-
niques which result in fiber lengths of >5 mm, exhibiting tensile
strengths of 100 MPa [10]. The glass fibers can reinforce the
matrix efficiently.
In contrast, it is difficult to reinforce the matrix using natural
fibers, as they possess hydrophobic surfaces and anisotropic inter-
nal structures. To address these issues, the surface state of natural
fibers is typically modified by alkalization and/or silanization
treatments [11–16]. Use of maleic anhydride-grafted polypropyl-
ene (MAPP) as a coupling agent can further improve the interfacial
shear strength (IFSS) between a natural fiber and its matrix [17,18].
Earlier studies carried out by Thomason presume that the lower
reinforcement efficiency of natural fiber is due to its anisotropic
feature [19]. Here, the compression residual stress, which

http://dx.doi.org/10.1016/j.compositesb.2014.08.032
1359-8368/Ó 2014 Elsevier Ltd. All rights reserved.
 Y. Arao et al. / Composites: Part B 68 (2015) 200–206
primarily affects the IFSS [20], is lower for natural fibers compared
to GF, owing to a low transverse and shear modulus.
It is clear, that the structure of natural fiber is significantly dif-
ferent from its glass counterpart. The natural fiber is composed of
cellulose as the reinforcement (elementary fibers) and amorphous
polymers as an adhesive. This dominates the mechanical proper-
ties, by aligning the cellulose fibrils next to the fibers’ axis. For
instance, jute fiber bundle (diameter = 25–50 lm), which has a
lower orientation angle than other natural fibers, displays a high
modulus but is brittle in nature [19]. The bundles are produced
through a spinning process and supplied in the form of a twisted
yarn. In contrast, glass fibers are supplied as bundles using a sizing
agent. The fiber structure and product form of natural fiber is com-
pletely different from glass fiber. Recently, long fiber pellet of nat-
ural fiber is developed, similarly to glass fiber [21–23]. However,
the validity of using this technique for natural fiber composite
has not been confirmed yet.
Previous studies on tensile strength of natural fiber/PLA com-
posites are summarized in Table 1. Compression molding can fab-
ricate natural fiber/PLA composites without damaging natural fiber
during processing [24–27]. Lim et al. examined the effects of fiber
loading and surface treatment on the strength of hemp/PLA com-
posite made by compression molding. They found that the com-
posites with 40% volume fraction of alkali treated fiber showed
the best tensile strength. The composites showed much higher
strength compared to neat PLA. The best data of PLA/natural fiber
composites was reported by Plackett et al. [26]. In this study,
non-woven jute fiber mats were stacked with several PLA films
and subjected to compression molding. The key parameter in their
study was the temperature to impregnate the PLA matrix to jute
mat without degrading the matrix and fiber at a constant high tem-
perature. As no fiber damage was observed during this process,
composites with significantly high strengths could be constructed.
However, compression molding technique is time consuming and
unsuitable for mass production.
The preferred manufacturing method for mass products is typ-
ically injection molding. A major advantage of this technique lies in
its high processability, although the fiber is known to degrade dur-
ing the procedure. Previous work by Yang et al. has focused on the
development of long jute fiber pellets and fabrication through
injection molding [21]. Upon addition of the jute fiber, they
observed an increase in the material modulus; however, the tensile
strength was found to decrease. Bax et al. used an injection mold-
ing technique to fabricate Cordenka/PLA and flax/PLA composites,
and remarkably achieved a strength of 58 MPa for the former com-
posite [28], with a maximum impact strength of 72 kJ/m2 (4.5
times higher than what has been observed for pure PLA). They con-
cluded that the addition of Cordenka fiber was capable of modify-
ing the brittleness and low impact properties of PLA. However, the
most favorable results have been reported by Sawpan et al. [14],
where the authors noted an exceptionally high strength value of
75.5 MPa (148%) for PLA combined with 30 wt.% hemp fibers, com-
Table 1
Comparison of the mechanical properties of PLA based green composite fabricated by various process.
Fiber Fiber content (wt.%) Process Stress (MPa)
Flax 30 CM 53
Hemp 40 (volume) CM 54.6
Ramie 30 (volume) CM 66.8
Jute 40 CM 100.5
Jute 35–39 IM 49
Cordenka 30 IM 58
Jute 30 IM 81.9
Jute 50 IM 82.2
Hemp 30 IM 75.5
CM: Compression molding, IM: Injection molding.
201
pared to pure PLA = 51 MPa. By conducting alkali and silane fiber
treatments, they found that the alkali treated reinforced fiber com-
posites displayed improved mechanical properties, owing to the
exceptional fiber/matrix adhesion. The jute/PLA composites
reported by Bledzki et al. and Gunning et al. also illustrated high
mechanical performance [29,30]. Gunning et al. investigated the
effective process condition for PLA based green-composites via
twin-screw extrusion, and found that the composite produced
using lower temperature profiles exhibited superior properties to
those produced at higher temperature, owing to reduce thermal
degradation of natural fiber during compounding. They fabricated
PLA based composite using jute, hemp and lyocell fiber with vari-
ous fiber loading. In their experiment, jute/PLA composite with
50 wt.% fiber loading showed the best mechanical properties. The
tensile strength of jute/PLA afforded 82.2 MPa, which was the max-
imum value, reported for injection molded samples. Although the
average residual fiber length was short (approximately 1 mm),
due to the high compounding intensity applied by a twin-screw
extruder, the composites exhibited enhanced mechanical proper-
ties than what has been reported to date.
The purpose of this study is to develop PLA based green-com-
posite materials that exhibit superior mechanical properties. Par-
ticular emphasis is placed on the material processing steps. By
employing a continuous pultrusion technique, we successfully
demonstrated the fabrication of natural long fiber pellets (LFPs).
To further investigate the characteristics of these LFPs, we com-
pared our results with a short fiber pellet (SFP), constructed using
a twin-screw extruder. Both composites were fabricated by a
method known as injection molding. Tensile and Izod impact tests
were also performed to measure the overall strength. Furthermore,
microscopy techniques were employed to study both the fiber size
and distribution after processing, in order to validate the results
against their mechanical properties.
2. Experimental
2.1. Materials
The TE-8000 PLA, supplied from Unitika Ltd. was used in this
study. A twisted jute yarn (Tex 400) was purchased from Tesac
Co. In order to suppress the hydrolysis during processing, LA-1
(Nisshinbo Chemical Inc.) was added to PLA. In addition, the crys-
tallizing agent, Ecopromote (Nissan Chemical Industries), was used
to increase the crystallinity of PLA composites. The weight ratio of
jute, PLA, LA-1 and crystallization agent was set to 50, 46, 2 and
2 wt.%, respectively.
2.2. Composite processing
LFP (length = 6 mm) was fabricated using a standard long pellet
instrument (Kobe Steel, Ltd.) as reported previously [21,23]. All of
Strength in % Young’s modulus (GPa) Additional information Source
106 8.3 Using extruded pellet [25]
156 8.45 Film stacking + surface treatment [24]
148 – Compound pellet + surface treatment [12]
182 9.4 Film stacking method [26]
80 10.5 Using long fiber pellet [21]
130 4.85 Using compound pellet [28]
129 9.6 Using compound pellet [29]
121 – Optimal compound process [30]
148 8.18 Surface treatment [14]
202 Y. Arao et al. / Composites: Part B 68 (2015) 200–206
additives were compounded in LFP production process. The equip-
ment composed of a twin-screw extruder for plasticization of PLA
and an impregnation head to infuse the molten PLA into a jute
strand. To investigate the effect of LFP on the mechanical property
of our green-composites, we also prepared the SFP as a control. LFP
was added into the twin-screw extruder (ZSK-18, L/D = 40,
Coperion).
With respect to the process in twin-screw extruder, tempera-
ture, screw speed and screw configuration have dominant effect
on the quality of compound. Especially for natural fiber, thermal
degradation occurs above 180 °C, which is around the melting tem-
perature of PLA. To mitigate the thermal degradation of jute fiber
during processing, control temperature was set to 180 °C. In gen-
eral, higher screw speed leads to higher shear force during com-
pounding. Therefore, it facilitates fiber dispersion, on the other
hand it increases the temperature of compound by shear heating.
In fact, the temperature of extruded compound was 10–20 °C
higher than the control temperature (180 °C). To minimize thermal
degradation by shear heating, the screw speed was controlled at
150 rpm.
We employed two different types of configurations for this pur-
pose: (i) the first was composed entirely of a full flight (convey)
element, to reduce the shear stress during compounding, and (ii)
the second was composed of both a full flight and several mixing
elements (SME and ZME, Coperion) to improve the overall fiber
dispersion. In general, kneading element, which can generate high
shear stress during compounding, are often used to improve dis-
persion quality. However, high shear stress by kneading elements
increases temperature of compound. Therefore, in this study we
chose mixing elements instead of kneading elements. Mixing
elements are designed to minimize the amount of dispersive,
shear-intensive mixing, and to facilitate the amount of distributive
mixing by complex flow. The combination of two SME and
one ZME was used as a mixing region, and three of them were
set up for mixing screw.
Subsequently, the LFP and SFP were fed into the injection mold-
ing instrument (PLASTER ET-40V, Toyo Machinery & Metal Co.,
Ltd.). The barrel temperature was controlled at 180 °C. The result-
ing structures were dumb-bell shaped, with a thickness of 8 mm
and a width of 10 mm, at the gauge position. We prepared three
types of specimens depending the type of pellet. The specimens
fabricated using LFP is defined as LFP, SFP by full flight element
as SFP (FF), and SFP by mixing element as SFP (MIX).
2.3. Mechanical testing
Tensile tests were conducted by a universal testing machine
(Autograph AG-1, Shimadzu Co.) based on the Japanese Industrial
Standard (JIS K7161). The cross-head speed was maintained at
1 mm/min and during the tensile test the external strain was mea-
sured using an extensometer (ST10-10, Shimadzu Co.).
The Izod impact strength test (in accordance with JIS K7110)
was carried out at room temperature. The dumb-bell shaped spec-
imens were prepared with a V-notch cut for impact. Both tests
were repeated at least 10 times for each type of specimen. Mor-
phologies of the composites’ tensile fracture surfaces were
observed using a scanning electron microscope (SEM, JSM-
7001FD, JEOL Ltd.), under a 10 kV acceleration voltage. All speci-
mens were coated with platinum prior to examination.
2.4. Distribution of fiber
The overall fiber geometry of the injection molded samples was
investigated after dissolving the PLA specimens in chloroform. The
residual jute fibers were dispersed in water, and observed under an
optical microscope. We observed a broad distribution of jute fibers,
with diameters ranging from a few microns to a few hundred
microns. The fiber sizes were analyzed manually with either a
10  or 30  magnification. Over 1000 measurements of the fiber
length and diameter were collected using the image analysis soft-
ware. Furthermore, high-resolution X-ray micro-tomography
(micro-CT, SkyScan 1172, Bruker Co.) was also employed to exam-
ine both the spatial distribution and orientation of our fibers
within the composite. A large number of images were recorded
while rotating the sample between 0° and 360°, to reconstruct
the entire volume. Image analysis was then conducted at various
cross-sections to resolve these features. The resolution of our anal-
ysis method was further improved by cutting the injection molded
sample down to 6  2  2 mm. With an X-ray beam power of 8 W,
we were able to obtain a spatial resolution of 2.1 lm.
3. Experimental results
3.1. Mechanical properties
Our initial studies were focused on the effect of LA-1 for sup-
pressing the hydrolysis of PLA. We found that in the absence of
LA-1, the addition of 50 wt.% jute fiber to LFP decreased the
strength of PLA from 49.8 MPa to 28 MPa as shown in Table 2.
The presence of water inside the jute fiber and the increased tem-
peratures accelerated the hydrolysis of PLA. In fact, the molecular
weight average (Mw) of PLA was observed to decrease from
170,000 g/mol to 45,000 g/mol, as measured by gel permeation
chromatography (GPC). Addition of 2 wt.% of LA-1 to the jute/PLA
composite increased the Mw to 87,000 g/mol. As a result, jute/PLA
composite with LA-1 showed higher tensile strength compared to
neat PLA. We further investigated the effect of pre-drying of our
jute fiber during LFP fabrication. The effect of pre-drying the fibers
was evident in the improved strength of jute/PLA composite with-
out LA-1. Whereas, in the presence of LA-1, it had negligible effects
and the strength was seen to improve by only 1–3 MPa. It seems
that as long as hydrolysis suppressor is added into PLA, residual
moisture inside jute fiber do not facilitate hydrolysis during the
process. Suppression of PLA hydrolysis was essential in improving
the mechanical properties of jute/PLA composites. It was presumed
that the apparent minimal improvement of tensile strength
[21,25,31] was a result of PLA hydrolysis.
Fig. 1 shows the typical stress–strain curves for PLA and jute/
PLA composites. Note that all of the composites include LA-1. Con-
sidering that hydrolysis of PLA is suppressed, the addition of jute
fiber increased the strength of PLA. The tensile and Izod impact
tests are summarized in Table 2. Standard deviation of the results
are also listed in Table 2. Contrary to the expectation, the use of LFP
did not show the best mechanical performance. The specimens
made of SFP showed not only higher strength but also increased
modulus, compared to jute/PLA composites made of LFP. The SFP
exhibited a significant 182% strength compared to that of pure
PLA. Although the fiber loading and surface treatment, which are
dominant parameters for mechanical performance of natural com-
posites [32], were not optimized, the composites made of SFP
showed the best tensile strength and modulus in injection molded
samples. This improvement was similar to or better than the com-
posite fabricated by compression molding, using aligned jute fiber
mat as shown in Table 1.
In the specimens constructed of SFP, the specimens using SFP
(MIX) gave better mechanical performance than that of SFP (FF).
This indicated that for jute/PLA composites, using the pellet, which
suffered higher compounding intensity, led to exceptional perfor-
mance. This evidence is in contradiction to what has been observed
for reinforced glass or carbon fiber composites. In the case of the
glass fiber, the high shear force during compounding shortens
 Y. Arao et al. / Composites: Part B 68 (2015) 200–206 203

Table 2
Mechanical properties of PLA and jute/PLA composites.

Material Strength (MPa) Strength in % Modulus (GPa) Impact strength (kJ/m)

PLA 49.8 ± 0.53 – 2.8 ± 0.1 2.68 ± 0.27
LFP without La-1 28.0 ± 2.3 56.2 – 3.85 ± 0.49
LFP 65.2 ± 2.2 131 10.3 ± 0.26 4.39 ± 0.76
SFP (FF) 78.6 ± 0.80 158 11.5 ± 0.26 4.57 ± 0.29
SFP (MIX) 90.7 ± 1.3 182 12.3 ± 0.17 4.22 ± 0.15

100 (a) 18
16 LFP
PLA
80
LFP 14 SFP (FF)
SFP (FF)

Frequency (%)
Stress [MPa]

12 SFP (MIX)
60 SFP (MIX)
10

40 8
6
20 4
2
0 0
㻜㻚㻜 㻜㻚㻡 㻝㻚㻜 㻝㻚㻡 㻞㻚㻜 㻞㻚㻡 40 45 50 55 60 65 70 75 80 85 90 95 100 105 110
Strain [%] Fiber diameter (µm)
Fig. 1. Stress–strain curves for injection molded specimens.

(b) 35
the fiber length, and can lead to lower mechanical efficiency of LFP
30
injection molded components. In contrast, high mixing intensity SFP (FF)
improves the reinforcing efficiency of natural fiber. The same ten- 25 SFP (MIX)
Frequency (%)

dency has been confirmed for flax/PP composites reported by

Barkoula et al. [22]. They concluded that the kneader compounded
composite displayed better tensile strength as well as improved
stiffness compared with the composite formed from LFP.
The impact strength also increased by >60% with the addition of
50 wt.% jute fiber. Undoubtedly, the impact strength does not
solely depend on the type of pellet used in injection molding. How-
ever, the standard deviation of impact strength decreased with
increasing compounding intensity of the pellet. This implied that
high dispersion state in PLA matrix decreased the scattering of
the impact. It is well known that the mechanical properties of short
fiber reinforced composites depend on the aspect ratio of fiber, the
IFFS between fiber and matrix, and their dispersion state. There-
fore, to interpret the overall strength improvement of jute/PLA
composite using SFP, it is crucial to obtain these parameters. These
are discussed in the following sub-sections.
3.2. Fiber-size distribution
Using optical imaging, we observed a broad distribution for our
jute fiber diameters ranging from a few to several hundred
microns. For this purpose, two independent settings were used
on the optical microscope: 10 and 30 magnification, to allow
complete characterization of our composites.
Fig. 2 shows the distribution of fiber diameter for injection
molded specimens. In the case of the lower 10 magnification,
only fibers with diameter >40 lm could be identified correctly.
Hence, the higher 30 magnification was used to distinguish smal-
ler dimensions (10–40 lm in size). The typical dimensions of our
jute fibers were between 20 and 50 lm. Multiple fibers with diam-
eters >50 lm, were observed using the 10 magnification. This
indicated two or more fiber, which may have been entangled and
thus were evaluated easily with the lower resolution. Additionally,
we observed that the entangled fiber diameters decreased with
increasing compounding intensity. In the case of the observation
of 30 magnification, the fibers with a diameter of 10–60 lm were
20
15
10
5
0
0 5 10 15 20 25 30 35 40 45 50 55 60
Fiber diameter (µm)
Fig. 2. Distribution of fiber diameter observed by an optical microscope. (a) 10
magnification. (b) 30 magnification.
observed. It means this magnification was suitable to evaluate
the size of single jute fiber. Notably, fibers with diameters
<20 lm were observed consistently with the SFP (MIX) specimen.
This decrease in diameter was attributed to the presence of a high
shear force during the compounding process.
Table 3 presents the average fiber size obtained by microscopic
observation. Here we observed that the aspect ratio of LFP showed
the best value for each specimens, because fibers did not suffer
high shear force through the twin-screw extruder. Particularly,
the aspect ratio for entangled jute bundles (observed by 10 mag-
nification) is considerably lower than that of an individual or ele-
mentary fibers (observed by 30 magnification). It is important
to note that high shear force during compounding decreases not
only the length of fiber (fiber fragmentation) but also the diameter
of fiber (fiber decohesion). Consequently, high intensity com-
pounding can facilitate dispersion of jute yarn and separation of
jute bundle, which can potentially contribute to the increased
aspect ratios observed here. These results also imply that accurate
aspect ratio of natural fibers should be carefully determined,
because they exist as entangled yarn, bundles, or elementary
fibers. It is difficult to evaluate aspect ratio of these fibers (yarn,
bundle, elementary fiber) at the same time.
204 Y. Arao et al. / Composites: Part B 68 (2015) 200–206

Table 3
Average fiber length, diameter and aspect ratio for each magnification.

Length (lm) Diameter (lm) Aspect ratio LFP

A microscope of 10 magnification
LFP 618 68.1 9.4
SFP (FF) 387 71.8 5.6
SFP (MIX) 289 50.5 4.8
A microscope of 30 magnification
y
LFP 614 38.1 17.2
SFP (FF) 383 34.2 12.2
SFP (MIX)
SFP (MIX) 288 23.6 13.3

z x

3.3. Distribution of fiber Fig. 3. Photograph of the specimens after injection molding.

Fig. 3 shows optical images for the appearance of injection

molded samples using LFP and SFP. In the case of LFP, a consider-
able amount of jute fiber bundles were observed. In contrast, when
using SFP no such bundles were detected. The agglomerations of
fiber act as the defect. On the basis of different dispersion states,
it was presumed that the elongation at the break of LFP was lower
than that of SFP (as represented in Fig. 1).
Fig. 4 shows the cross section of the composites observed by X-
ray micro-tomography. Here, a cluster of jute fibers is observed for
LFP, demonstrating an unsuccessful dispersion. Although in the
case of SFP, the clusters are observed to reduce in size, as the com-
pounding step using a twin-screw extruder can lead to the jute
yarn dispersions. Upon examination of the SFP (MIX) images, the
fraction of fiber in the image decreases. It is presumed that
the diameter of fiber decreased less than the spatial resolution of
the observation. From these observations, we obtained two classes
of dispersions: (i) firstly, the large range from an entire yarn to
fiber bundles (referred to as jute fiber in general), and (ii) secondly,
decohesion of fiber bundles to elementary fibers. Notably, such
phenomenon is commonly observed in natural fibers, but is not
in conventional glass or carbon fiber [33,34].
With poor distribution, the entangled fibers indicate a large
fiber to fiber contact area. This association decreases the stress
transfer efficiency from matrix to fibers. It is presumed that a high
shear force applied to SFP (MIX) can reduce the contact by facilitat-
ing the dispersion from a yarn to a bundle, and from a bundle to an
elementary fiber. Hence the Young’s modulus of the SFP (MIX)
obtained was typically superior to other specimens. Furthermore,
we evaluated the orientation factor of each specimens based on
the results of our X-CT images but no apparent differences
could be confirmed. Accordingly, it can be proposed that the

100 µm x y
(a)

100 µm 100 µm

(b) (c)
Fig. 4. X-CT image of jute/PLA composites. The size of the image is 600  600 lm2. The image represents a sample with 50 wt.% fiber such that the PLA matrix is not visible.
The cross-section is perpendicular to flow direction (longitudinal direction). (a) LFP. (b) SFP (FF). (c) SFP (MIX).
 Y. Arao et al. / Composites: Part B 68 (2015) 200–206
Fig. 5. SEM micrographs of the fracture surface after tensile test. (a) LFP. (b) SFP
(MIX).
well-dispersed jute fibers resulting from high shear compounding
can lead to efficient load transfer; hence well-compounded com-
posites show both a high strength and modulus.
3.4. Fracture surface analysis
Fig. 5 shows the fracture surfaces of jute/PLA composites con-
structed using LFP and SFP (MIX). With respect to LFP, numerous
pull-out fibers were observed, indicating low IFSS between the
fiber and matrix. The pull-out fiber not coated by PLA, showed bare
surfaces of jute fibers. In general, the IFSS between natural fibers
and a thermoplastic is extremely low, and brittle fractures of jute
fibers as well as fiber pullout without resin coating have been
observed [11,26,35]. The low IFSS observed between the jute fiber
and PLA can be directly associated to the hydrophilic nature and
anisotropic property of the natural fiber. Furthermore, the jute
yarns used in this study were manufactured with either minerals
or natural oils to increase overall throughput and production effi-
ciency. On this assumption, the oil remaining on the jute fiber sur-
faces was expected to potentially deteriorate the IFSS of the
composites.
The fiber pull-out was also observed in the case of the fractured
surface of SFP (MIX). However, many jute fibers were coated by
PLA in this case. This implied that the IFSS of the composite had
increased for the SFP (MIX) specimen. This was indeed remarkable,
205
allowing us to control the composites’ IFSS, by simply changing the
high shear force applied during compounding.
The initial diameter size before compounding was between 20
and 50 lm. Jute fiber is composed of smaller fibers glued by an
adhesive (amorphous polymer such as lignin). Different from inor-
ganic fibers, the diameter of natural fiber decreases as a result of
the fiber structure. New jute fiber surfaces appeared when the
diameter of the fiber decreased by shearing. In this case, the IFSS
appears to increase because the surface area of the jute fiber with-
out oil also increases.
In the case of natural fibers, the positive effect of improved IFSS
and load transfer efficiency induced by well dispersion can over-
come the negative effect of fiber length reduction. Thus, use of well
compounded pellet in injection molding result in high mechanical
properties. It is presumed that efficient compounding with mini-
mizing thermal degradation of natural fiber lead to the best
mechanical performance of jute/PLA composite (Table 2).
4. Conclusions
We have developed an effective process to improve the
mechanical properties of jute/PLA composites. From our results,
we note that the suppression of hydrolysis is necessary to improve
the overall performance. When PLA without modification against
hydrolysis was used, addition of jute fiber increased the modulus
but lowered the absolute tensile strength. To further improve this
system, we used a LFP at the injection molding step, which
increased the aspect ratio of our jute fibers. However, this could
also lead to excessive aggregation. From our distribution analysis,
we observed well-dispersed fibers when the SFP pellet (which suf-
fered high shear force during compounding) was used in injection
molding. Whereas, the compounding through a twin-screw extru-
der facilitated the dispersion of the jute yarn and decohesive of jute
bundle. These features help improve the IFSS and stress transfer
efficiency for such composites. Hence, the use of a well-com-
pounded pellet in injection molding can significantly improve the
Young’s modulus and the tensile strength of jute/PLA composites.
References
[1] Koronis G, Silva A, Fontul M. Green composites: a review of adequate materials
for automotive applications. Compos Part B 2013;44:120–7.
[2] Sin Lee Tin, Rahmat AR, Rahman WAWA. Polylactic acid: PLA biopolymer
technology and applications. Elsevier; 2013.
[3] Wambua P, Ivens J, Verpoest I. Natural fibres: can they replace glass in fibre
reinforced plastics? Compos Sci Technol 2003;63:1259–64.
[4] Mukherjee T, Kao N. PLA based biopolymer reinforced with natural fibre: a
review. J Polym Environ 2011;19:714–25.
[5] Khan RA, Khan MA, Zaman HU, Pervin S, Khan N, Sultana S, et al. Comparative
studies of mechanical and interfacial properties between jute and E-glass
fiber-reinforced polypropylene composites. J Reinf Plast Compos
2010;29:1078–88.
[6] Thomason JL, Vlug MA. Influence of fibre length and concentration on the
properties of glass fibre-reinforced polypropylene: 1. Tensile and flexural
modulus. Compos Part A 1996;27:477–84.
[7] Thomason JL, Vlug MA, Schipper G, Krikor HGLT. Influence of fibre length and
concentration on the properties of glass fibre-reinforced polypropylene: 3.
Strength and strain at failure. Compos Part A 1996;27:1075–84.
[8] Thomason JL. Influence of fibre length and concentration on the properties of
glass fibre-reinforced polypropylene: 5. Injection moulded long and short fibre
PP. Compos Part A 2002;33:1641–52.
[9] Thomason JL. Influence of fibre length and concentration on the properties of
glass fibre-reinforced polypropylene: 6. The properties of injection moulded
long fibre PP at high fibre content. Compos Part A 2005;36:995–1003.
[10] Inoue A, Morita K, Tanaka T, Arao Y, Sawada Y. Effect of screw designs on fiber
breakage and dispersion of GFRTP in injection molding plasticization. J
Compos Mater, http://dx.doi.org/10.1177/0021998313514872.
[11] Ma H, Joo CW. Structure and mechanical properties of jute–polylactic acid
biodegradable composites. J Compos Mater 2010;45:1451–60.
[12] Yu T, Li S, Yuan H, Li Y. Effect of fiber surface-treatments on the properties of
poly(lactic acid)/ramie composites. Compos Part A 2010;499:505.
206 Y. Arao et al. / Composites: Part B 68 (2015) 200–206
[13] Huda MS, Drzal LT, Mohanty AK, Misra M. Effect of fiber surface-treatments on
the properties of laminated biocomposites from poly(lactic acid) (PLA) and
kenaf fibers. Compos Sci Technol 2008;68:424–32.
[14] Sawpan MA, Pickering KL, Fernyhough A. Improvement of mechanical
performance of industrial hemp fibre reinforced polylactide biocomposites.
Compos Part A 2011;42:310–9.
[15] Goriparthi BK, Suman KNS, Rao NM. Effect of fiber surface treatments on
mechanical and abrasive wear performance of polylactide/jute composites.
Compos Part A 2012;43:1800–8.
[16] Csizmadia R, Faludi G, Renner K, Mo9 czó J, Pukánszky B. PLA/wood
biocomposites: improving composite strength by chemical treatment of
fibers. Compos Part A 2013;53:46–53.
[17] Doan TTL, Gao SL, Mäder E. Jute/polypropylene composites I. Effect of matric
modification. Compos Sci Technol 2006;66:952–63.
[18] Sun ZY, Han HS, Dai GC. Mechanical properties of injection-molded natural
fiber-reinforced polypropylene composites: formulation and compounding
processes. J Reinf Plast Compos 2010;29:637–50.
[19] Thomason JL. Dependence of interfacial strength on the anisotropic fiber
properties of jute reinforced composites. Polym Compos 2010. http://
dx.doi.org/10.1002/pc.20939.
[20] Thomason JL, Yang L. Temperature dependence of the interfacial shear
strength in glass–fibre polypropylene composites. Compos Sci Technol
2011;71:1600–5.
[21] Yang Y, Murakami M, Hamada H. Molding method, thermal and
mechanical properties of jute/PLA injection molding. J Polym Environ 2012;
20:1124–33.
[22] Barkoula NM, Garkhail SK, Peijs T. Effect of compounding and injection
molding on the mechanical properties of flax fiber polypropylene composites. J
Reinf Plast Compos 2010;29:1366–85.
[23] Fujiura T, Okamoto T, Tanaka T, Imaida Y. Improvement of mechanical
properties of long jute fiber reinforced polylactide prepared by injection
molding process. WIT Trans Ecol Environ 2010;138:181–8.
[24] Hu R, Lim J. Fabrication and mechanical properties of completely
biodegradable hemp fiber reinforced polylactic acid composites. J Compos
Mater 2007;41:1655–69.
[25] Oksman K, Skrifvars M, Selin JF. Natural fibres as reinforcement in polylactic
acid (PLA) composites. Compos Sci Technol 2003;63:1317–24.
[26] Plackett D, Andersen TL, Pedersen WB, Nielsen L. Biodegradable composites
based on L-polylactide and jute fibres. Compos Sci Technol 2003;63:1287–96.
[27] Jayaraman K. Manufacturing sisal–polypropylene composites with minimum
fibre degradation. Compos Sci Technol 2003;63:367–74.
[28] Bax B, Müssig J. Impact and tensile properties of PLA/Cordenka and PLA/flax
composites. Compos Sci Technol 2008;68:1601–7.
[29] Bledzki AK, Jaszkiewicz A. Mechanical performance of biocomposites based on
PLA and PHBV reinforced with natural fibres – a comparative study to PP.
Compos Sci Technol 2010;70:1687–96.
[30] Gunning MA, Geever LM, Killion JA, Lyons JG, Higginbotham CL. The effect of
processing conditions for polylactic acid based fibre composites via twin-
screw extrusion. J Reinf Plast Compos 2014;33:648–62.
[31] Oever MJA, Beck B, Müssing J. Agrofibre reinforced poly(lactic acid)
composites: effect of moisture on degradation and mechanical properties.
Compos Part A 2011;41:1628–35.
[32] Ku H, Wang H, Pattarachaiyakoop N, Trada M. A review on the tensile
properties of natural fiber reinforced polymer composites. Compos Part B
2011;42:856–73.
[33] Beaugrand J, Berzin F. Lignocellulosic fiber reinforced composites: Influence of
compounding condition on defibrization and mechanical properties. J Appl
Polym Sci 2013;128:1227–38.
[34] Berzin F, Vergnes B, Beaugrand J. Evolution of lignocellulosic fibre lengths
along the screw profile during twin screw compounding with
polycaprolactone. Compos Part A 2014;59:30–6.
[35] Oksman K, Matherw AP, Långström R, Nyström B, Joseph K. The influence of
fibre microstructure on fiber breakage and mechanical properties of natural
fibre reinforced polypropylene. Compos Sci Technol 2009;69:1847–53.