Thermal Properties of Jute Fiber Reinforced Chemically Functionalized High Density Polyethylene (JF/

CF-HDPE) Composites Developed by Palsule Process

Thermal Properties of Jute Fiber

Reinforced Chemically Functionalized
High Density Polyethylene (JF/CF-
HDPE) Composites Developed by
Palsule Process
Anshu Anjali Singh* and Sanjay Palsule
Department of Polymer & Process Engineering, Indian Institute of Technology-
Roorkee, DPPE IIT-R SRE Campus, Paper Mill Road, Saharanpur 247 001 India

Received: 3 January 2014, Accepted: 17 April 2014

Summary
Jute fiber reinforced chemically functionalized high density polyethylene
composites developed by Palsule process, without using any compatibilizer,
and without any fiber treatment exhibit good thermal stability. The initiation of
degradation of the JF/CF-HDPE composites is at temperatures intermediate
between those of temperatures of initiation of degradation of the fiber and the
matrix. The maximum degradation temperature of all the composite compositions
are higher that of the matrix, and increase with increasing Jute fiber content.
The temperatures of highest rate of degradation of 10/90, 20/80 and 30/70 JF/
CF-HDPE composites are 483°C, 485°C and 488°C respectively, and at 550°C
the composite compositions show the residual mass of 4.3%, 5.8% and 7%
respectively.

Introduction
Natural fiber reinforced polymeric composites are emerging as eco-friendly,
green polymer composites and are offering commercial and engineering
applications along with techno-economic advantages. These natural fiber
polymer composites are also offering environmental advantages, like; materials
based on renewable and biodegradable resources; reduced dependence on

* [email protected]
©Smithers Information Ltd., 2014

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non-renewable sources, reduced pollutant and greenhouse gas emissions

and also carbon-di-oxide sequestration, and enhanced energy recovery [1].
In recent years, natural plant based fibers, for example; jute, coconut,
hemp, sisal, coir etc., have been used as reinforcing materials for polymeric
composites in place of conventional fibers like glass, carbon, aramid, etc.
because natural fibers are renewable, non toxic, cost effective, easily available
and have acceptable specific properties [2]. Several plant based natural
fibers have been used as reinforcement materials for polymeric composite
because of their easy availability, low cost, bio-degradability, renewability,
recyclability, low density, good physical, thermal and mechanical properties
including acceptable specific strength and specific stiffness, reduced tool
wear, non-abrasiveness and non-toxic nature [3].
The main components of a plant fiber are; cellulose, hemicellulose and
lignin; and hence natural fibers are commonly termed as lingo-cellulosic
materials. Jute fibers, obtained from the bast layer of plants, have emerged
as important reinforcing fibers for thermoplastic matrix based composites and
like all other natural fibers, jute fibers are also lingo-cellulosic in nature with
61-71% cellulose, 14-20% hemicelluloses and 12-13% lignin [3, 4]. These
constituents make natural fibers hygroscopic and hydrophilic because of
which they have poor compatibility with hydrophobic polymer matrix in natural
fiber reinforced polymer composites. Consequently, natural fiber reinforced
polymer composites have poor fiber/matrix interfacial adhesion that limits load
transfer from the fiber to the matrix and results in poor mechanical, thermal
and physical properties of the composites. Strong fiber/matrix interfacial
adhesion is necessary in a natural fiber reinforced polymer composite for its
good overall properties and high performance. Following three processes
have been used to improve fiber/matrix interfacial adhesion in natural fiber
reinforced thermoplastic composites: (i) chemical or physical treatment of
natural fibers; (ii) use of compatibilizers or coupling agents; and, (iii) Palsule
process based on the use of chemically functionalized polyolefin as a matrix
(in place of polyolefin).
Several jute fiber reinforced polymer composites have been processed by the
first method of fiber modification by chemical or physical treatment to improve
fiber/matrix interfacial adhesion. For example, to process the composites, jute
fibers have been treated with 2-hydroxyl ethyl methacrylate (HEMA) [5], Silane
[6], Sodium periodate [7], 1,4-butanediol diacrylate (BDDA), ethyl hexyl acrylate
(EHA) and trypropylene glycol diacrylate (TPGDA) [8], oligomeric siloxane [9],
methyl methacrylate (MMA) , polyamide (PA) [10], maleic anhydride grafted
polyethylene [11, 12]. However, in this process of imparting fiber/matrix
interfacial adhesion by fiber surface modification by chemical or physical
treatments, several fibers remain untreated due to aggregation of fibers.

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 Thermal Properties of Jute Fiber Reinforced Chemically Functionalized High Density Polyethylene (JF/
CF-HDPE) Composites Developed by Palsule Process

Such untreated fibers fail to develop proper adhesion with the matrix in the
composite; consequently, the composite materials exhibit limited properties
at heavy loadings and at higher temperatures.
A compatibilizer acts as a coupling agent between the natural fiber and the
polymeric matrix and improves the compatibility and interfacial adhesion
between the fiber and the matrix and thus improves the properties of the
composites. Following the second method of use of compatibilizers or
coupling agents to develop fiber/matrix interfacial adhesion, several jute
fiber reinforced composites have been developed using compatibilizers like,
maleic anhydride grafted polypropylene varying in 1% to 6% concentration,
[13-16], m-TMI grafted polypropylene [17] and several others. In natural fiber
reinforced polymer composites processed by compatibilizers, non-uniform
distribution of compatibilizer across the composite results in poor fiber/matrix
interfacial adhesion and limits the composite properties at heavy loadings and
higher temperatures. Reviews on jute fiber/polyolefin composites developed
by both methods are available [18, 19].
Palsule [20-22] for the first time demonstrated that the use of chemically
functionalized polyolefin, for example, maleic anhydride grafted polyolefin, as
a matrix, in place of polyolefin, eliminates the need of any compatibilizer or any
fiber treatment for processing natural fiber reinforced chemically functionalized
polyolefin composites. This process of using chemically functionalized
polyolefin matrix to develop natural fiber reinforced chemically functionalized
polyolefin composite has now been termed as Palsule process [21, 22].
Natural fiber reinforced chemically functionalized polyolefin composites, for
example banana fiber reinforced chemically functionalized polypropylene
composites [21] and jute fiber reinforced chemically functionalized high density
polyethylene (JF/CF-HDPE) composites [22], developed by Palsule process
have demonstrated good properties due to significantly improved fiber/matrix
interfacial adhesion generated in-situ from interactions between the functional
groups present on the chemically functionalized polyolefin and the functional
groups present on the chemical components of the natural fiber.
Following the studies on structure, morphology and mechanical properties of
jute fiber reinforced chemically functionalized high density polyethylene (JF/
CF-HDPE) composites by Palsule process; this study reports thermal properties
of jute fiber reinforced chemically functionalized high density polyethylene
(JF/CF-HDPE) composites developed by Palsule process. Consequently, high
density polyethylene (HDPE) has not been used as a matrix in this study, but
chemically functionalized high density polyethylene (CF-HDPE), i.e. maleic
anhydride grafted high density polyethylene, has been used as matrix. The
use of CF-HDPE as the matrix does not require any fiber treatment or any
compatibilizers for processing of jute fiber reinforced chemically functionalized

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high density polyethylene (CF-HDPE) composites by Palsule process; as the

CF-HDPE is expected to develop in-situ fiber/matrix interfacial adhesion with
jute fibers due to the presence of maleic anhydride in it. Consequently, the
composites processed in this study have been developed by Palsule process,
without using any compatibilizer and without any chemical/physical treatment
of jute fibers; and this also avoids the problems due to untreated fibers and due
to non-uniform distribution of compatibilizer, like, poor fiber/matrix interfacial
adhesion, that may limit properties of jute fiber/chemically functionalized
polyolefin composites at heavy loadings and higher temperatures.

Experimental

Materials

Matrix Polymer
In this study, high density polyethylene (HDPE) – that requires a compatibilizer
or fiber surface treatment- has not been used as matrix; but chemically
functionalized high density polyethylene (CF-HDPE) with 1.2% maleic anhydride
grafted on it, has been used as matrix for the composites. CF-HDPE was
obtained commercially (OPTIM® E-156, Series 300) from Pluss Polymer Pvt.
Ltd., India. It is available, commercially, as free flowing granules and is off
white to light yellow in appearance. It has a reported density of 0.954 g/cm3,
reported melting temperature (Tm) of 132°C and the melt flow index (MFI) of
4.5 g/10 min (190°C, 2.16 kg).

Reinforcing Fiber
Reinforcing jute fibers, of 0.06 mm average diameter, obtained from local market
in raw form, were chopped to 3-6 mm length and were used, as received,
without any fiber surface treatment. Jute fibers have been termed as JF.

Compounding and Processing of JF/CF-HDPE Composites

Chemically functionalized high density polyethylene (CF-HDPE), and 3-6 mm
short jute fibers (JF) were dried separately in hot air oven at 50°C for one day,
and then at 80°C for 3-4 hours, prior to extrusion to remove the moisture.
Calculated amounts of reinforcing JF and CF-HDPE matrix were mixed
manually with a view to finally obtain 10/90, 20/80 and 30/70 JF/CF-HDPE
composites. Mixtures with appropriate amounts of constituent materials

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 Thermal Properties of Jute Fiber Reinforced Chemically Functionalized High Density Polyethylene (JF/
CF-HDPE) Composites Developed by Palsule Process

were fed into the hopper of the co-rotating twin screw extruder (model JSW
TEX 30α). The screw speed of JSW TEX 30α co-rotating twin screw extruder
was set at 145 rpm and the temperature profile for nine different zones in the
extruder was varied from 155°C to 175°C. In particular, the temperature profiles
of the various zones of the extruder for processing JF/CF-HDPE composites
were – 155°C-155°C-160°C-160°C-165°C-170°C-175°C-175°C-165°C. The
JF/CF-HDPE mixtures, with appropriate amounts of the JF and CF-HDPE,
were compounded in the extruder, and the extruded composite compositions,
termed as 10/90, 20/80 and 30/70 JF/CF-HDPE composites, were cooled in
water. These were then pelletized in a pelletizer to obtain granules that were
dried in hot air oven at 80°C for overnight, and were then used to mold test
specimens for tensile, flexural and Izod impact tests. To process samples
for testing and characterization as per ASTM standards, CF-HDPE matrix
and extruded and pelletized JF/CF-HDPE composite granules were molded
by injection molding machine [Electronica ENDURA 90] with the feed zone
temperature of 145°C and nozzle temperature of 170°C.

Fibre/Matrix Interfacial Adhesion in the JF/CF-HDPE Composites

Jute fiber reinforced chemically functionalized high density polyethylene
composites developed in this study by Palsule process, without using any
compatibilizer, and without any fiber treatment, show good mechanical
properties and also develop in-situ fiber/matrix interfacial adhesion due to
interactions between the functional groups on the fiber and the matrix. Details
of the in-situ fiber/matrix interfacial adhesion and its mechanism and of the
mechanical properties of the JF/CF-HDPE composites have been described
in literature [22].

Thermal Characterization of the Reinforcing Jute Fibers, CF-

HDPE Matrix Polymer and the JF/CF-HDPE Composites
The thermal properties of the CF-HDPE polymer matrix, reinforcing jute
fibers (JF) and the processed JF/CF-HDPE composites were evaluated by a
Thermogravimetric/Differential Thermal Analyzer (TG-DTA SII 6300 EXSTAR).
This instrument gives data for TGA, DTG and DTA and three different graphs
are obtained: (i) Weight change (%) v/s temperature i.e. TGA, (ii) Weight /Time
(μg/min) v/s temperature i.e. DTG, (iii) Heat flux (μV) v/s temperature i.e. DTA
(for melting temperature).
TGA, DTG and DTA are the most widely used thermal methods, TGA being
the most basic and the simplest of all the thermo-analytical method. The

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measurement of the sample may be carried out in presence of inert atmosphere

(nitrogen), at constant heating rate, and the change in weight is recorded as a
function of increasing temperature. Maximum temperature is selected such that
the sample weight is stable at the end. This approach gives important information
about the sample, i.e.; the ash content (residual mass), the temperature of
maximum degradation and the melting temperature. This technique is effective
for quantitative analysis of thermal reactions that are accompanied by mass
changes viz. evaporation, decomposition, dehydration, gas absorption and
desorption and helps in deciding the end use application of the composites.
In this study, CF-HDPE polymer matrix, reinforcing jute fiber and JF/CF-HDPE
composite samples were heated from room temperature to 550ºC at heating
rate 10ºC/min in presence of nitrogen atmosphere.

Results and Discussions

Figure 1a-e shows the TG and the weight loss% of the reinforcing jute fibers,
CF-HDPE polymer matrix and all the compositions of JF/CF-HDPE composites
in nitrogen atmosphere. TGA evaluates mass loss of a material as a function
of temperature. A continuous graph of mass change against temperature is
obtained when a sample is heated at a constant rate. A plot of percent mass
change v/s temperature is referred to as thermogravimetric (TG) curve.

Figure 1a-e. Thermo-gravimetric curves, in nitrogen atmosphere, of (a) Reinforcing

jute fibers (JF), (b) CF-HDPE matrix, and of following JF/CF-HDPE composites – (c)
10/90 JF/CF-HDPE (d) 20/80 JF/CF-HDPE (e) 30/70 JF/CF-HDPE

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Figure 1a and b indicates that the JF starts releasing volatile matter (water)
at around 70°C, CF-HDPE does not release any volatile matter at lower
temperatures; and shows initiation of degradation at around 470°C. Figure 1a
and b also show that the residual mass of CF-HDPE at 550°C is 3% and that
of JF is 16.1%. Figure 1c-e indicates that the 10/90, 20/80 and 30/70 JF/CF-
HDPE composites show initiation of degradation at around 405°C, 380°C and
360°C respectively; and these temperatures are in between the temperatures
of initiation of degradation of JF (70°C) and CF-HDPE (470°C). Figure 1c,d
and e also shows that the residual mass of 10/90, 20/80 and 30/70 JF/CF-
HDPE at 550°C are 4.3%, 5.8% and 7% respectively.
Figures 2a and b show the DTG (relative weight change as a function
of temperature) of JF and CF-HDPE matrix and it was observed that the
temperature of highest rate of degradation of JF is 359°C and that of CF-
HDPE is 480°C. Figures 2c-e indicates that the temperatures of highest rate
of degradation of 10/90, 20/80 and 30/70 JF/CF-HDPE composites are 483°C,
485°C and 488°C respectively.

Figure 2. DTG Curves (relative weight change as function of temperature) of (a) JF and
(b) CF-HDPE

The maximum degradation temperature of all JF/CF-HDPE composite

compositions is higher than the maximum degradation temperature of CF-
HDPE matrix and the maximum degradation temperature of the composites
increases with increase in jute fiber content in composite compositions,
indicating higher thermal stability of all the JF/CF-HDPE composites than
that of the CF-HDPE matrix.

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Figure 2. DTG Curves (relative weight change as function of temperature) in nitrogen

atmosphere of (c) 10/90 JF/CF-HDPE, (d) 20/80 JF/CF-HDPE (e) 30/70 JF/CF-HDPE

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CF-HDPE) Composites Developed by Palsule Process

Melting Temperatures of CF-HDPE Matrix and JF/CF-HDPE

Composites
The melting temperature of the CF-HDPE matrix and all the compositions of
JF/CF-HDPE composites are recorded in the Figure 3 (DTA) and in Table 1.
The peak melting temperature (Tm) of CF-HDPE matrix and of the 10/90, 20/80
and 30/70 JF/CF-HDPE composites evaluated from the DTA curves (Figure 3)
recorded in Table 1 indicate that the melting temperature of the CF-HDPE
is 132.4°C and of the various JF/CF-HDPE composites are in the range of
132.7°C to 135.1°C. This indicates that the Tm of the different compositions
of the JF/CF-HDPE composite are not exactly the same (132.4°C) as that of
the CF-HDPE matrix, but are within the limits of experimental errors, probably,
either because of the measurement limitations of the instrument, or probably
because of some very minor interference of the fiber with the polymer matrix
structure. Thus, there is no appreciable change in the melting temperature
of the JF/CF-HDPE composites, as compared to CF-HDPE matrix, because
in principle, the CF-HDPE is the only component of JF/CF-HDPE composite
that actually melts, and the JF would not melt, but would degrade.

Figure 3. DTA curve indicating melting temperature (Tm) of (a) CF-HDPE matrix, (b)
10/90 JF/CF-HDPE, (c) 20/80 JF/CF-HDPE and (d) 30/70 JF/CF-HDPE composites

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Table 1. Melting temperature of CF-HDPE matrix and of all the

JF/CF-HDPE composites
Material Melting Temperature
Tm (°C)

CF-HDPE 132.4
10/90 JF/CF-HDPE 133.6
20/80 JF/CF-HDPE 132.7
30/70 JF/CF-HDPE 135.1

Conclusions
Good thermal stability is demonstrated by jute fiber reinforced chemically
functionalized high density polyethylene composites developed by Palsule
process, without using any compatibilizer, and without any fiber treatment.
The maximum degradation temperature of all the composite compositions are
higher that of the matrix, and increase with increasing jute fiber content. The
initiation of degradation of the JF/CF-HDPE composites is at temperatures
intermediate between those of temperatures of initiation of degradation of
the fiber and the matrix; and the temperatures of highest rate of degradation
of 10/90, 20/80 and 30/70 JF/CF-HDPE composite compositions are 483°C,
485°C and 488°C respectively, and at 550°C the composite compositions
show the residual mass of 4.3%, 5.8% and 7% respectively.

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