Journal of Reinforced Plastics and Composites OnlineFirst, published on October 14, 2009 as doi:10.

1177/0731684409341761

Effect of Chemical Modification of Jute

Fabrics on the Performance of Urethane
Acrylate-based Composites

HAYDARUZZAMAN A. H. KHAN AND M. A. HOSSAIN

Department of Physics, Jahangirnagar University, Savar, Dhaka, Bangladesh

MUBARAK A. KHAN* AND RUHUL A. KHAN

Radiation and Polymer Chemistry Laboratory, Institute of Nuclear
Science and Technology, Bangladesh Atomic Energy Commission
P.O. Box 3787, Dhaka, Bangladesh

ABSTRACT: Jute fabric-reinforced urethane acrylate-based composites were prepared using

urethane acrylate oligomer (M-1200) in methanol solvent along with photoinitiator (Darocur-
1173) followed by ultraviolet (UV) radiation. Different formulations were prepared by varying
oligomer in the solvent by 50–90% (by weight). Jute fabrics treated with 70% oligomer, 28%
methanol, and 2% photoinitiator followed by UV radiation showed the best mechanical properties
of the resulting composites. For further improvement of the mechanical properties of the
composites, jute fabrics were first treated with different percentages of methylmethacrylate
(MMA) in methanol with photoinitiator and cured under UV radiation and then again the
composites were fabricated by the oligomer. Urea was incorporated into the MMA formulation and
was found to have the potential to improve the mechanical properties of the composites.

KEY WORDS: jute, composite, oligomer, UV radiation, mechanical properties.

INTRODUCTION

HE GROWING INTEREST in using natural fibers as a reinforcement in urethane acrylate-

T based thermoset composites is mainly due to advantages such as lower cost, acceptable
specific properties, lower density, ease of preparation, lower energy requirements for
processing, biodegradability, wide availability, and relative nonabrasiveness over
traditional reinforcing fibers such as glass and carbon. Among all the natural fiber-
reinforcing materials, jute appears to be a promising material because it is relatively
inexpensive, nonabrasive, has low density, high strength and modulus than plastic [1], and
is a good substitute for conventional fibers in many situations and commercially available
in tropical countries. Among commodity thermosettings, urethane acrylate possesses
outstanding properties like good surface hardness, scratch resistance, and excellent
electrical properties. Hence, there is a particular interest for using it as a reinforcing fiber
in thermosetting composites. Natural fiber composite is of great demand in the whole

*Author to whom correspondence should be addressed. E-mail: makhan.inst@gmail.com

Journal of REINFORCED PLASTICS AND COMPOSITES, Vol. 00, No. 00/2009 1

0731-6844/09/00 0001–10 $10.00/0 DOI: 10.1177/0731684409341761
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2 H.A.H. KHAN ET AL.

world for environmental and ecological concern [2]. As a material of construction, jute
urethane acrylate composite can play a vital role in every industry. Jute urethane acrylate
composite can be used as particleboard, ceiling, blocks for building construction, and
furniture. The commercial production of jute urethane acrylate composite can be used to
reduce the import of particle board and cement. Moreover jute is cheaper than most
natural fibers like sisal, flax, hemp, etc. so it is possible to export jute urethane acrylate
composite to coontries abroad. However, some limitations in using natural fibers in
composites are the lower allowable processing temperatures, incompatibility between
the hydrophilic natural fibers and hydrophobic polymers, and high moisture absorption of
the fibers and the resulting swelling of the manufactured composite [3]. Thermoplastics
used in such composites consist of polyethylene (high and low density), polypropylene,
polyvinyl chloride, and polystyrene. On the other hand, kenaf, jute, sisal, coir, flax,
banana, wood flour, rice hulls, newsprint, pulp, and cellulose fibers are the main natural
fibers used as reinforcement [4–14]. Considering the prospects of jute urethane acrylate
composite, a great emphasis on its use is needed. In order to compete with the synthetic
fiber-reinforced composite, the mechanical properties of jute urethane acrylate composite
should be improved. This research work deals with the improvement of the mechanical
properties of jute urethane acrylate composite. The high strength of jute fibers has not
been extensively exploited in reinforced composites. This is, at least partially, because they
are hygroscopic and due to their low wettability by resins. These characteristics result
mainly due to the presence of hydroxyl groups and other polar groups in several
constituents of the fiber, mainly cellulose and lignin. Therefore, to enhance the use of jute
and other vegetal fibers, a broader system of investigations is necessary to search for
chemical modifiers and physical treatments that would alter these undesirable
characteristics. Several processes, such as chemical treatments [15], photochemical
treatments [16,17] have been developed to modify fiber surfaces. Improved physico-
mechanical properties of natural fibers with different impregnating solutions under UV
radiation have been reported [18]. Coupling agents such as methyl methacrylate (MMA)
usually improve the degree of cross-linking in the interface region and offer a perfect
bonding result. Coupling agents are effective in modifying the natural fiber/matrix
interface. The present study deals with the fabrication of jute fabric-reinforced urethane-
based thermoset composites. It further studies the effect of surface modification of jute by
the monomer (MMA) on the improvement of mechanical and degradable properties of the
composites.

EXPERIMENTAL

Materials

Bleached jute fabrics (Tossa jute) were collected from Bangladesh Jute Research
Institute (BJRI), Dhaka, Bangladesh. Oligomer urethane acrylate (M-1200), monomer
methylmethacrylate (MMA), and solvent methanol were purchased from Merck,
Germany. Urea and photoinitiator were procured from Sigma-Aldrich, Germany.

Methods

Jute fabrics were cut into small pieces (12  15 cm2) and dried in an oven at 1008C for
about 30 min to remove moisture. A number of formulations were prepared with different
Urethane Acrylate-based Composites 3

Table 1. Composition of different formulations based on oligomer.

Formulations (w/w %)
Materials F1 F2 F3 F4 F5

Oligomer 50 60 70 80 90
Methanol 48 38 28 18 8
Photoinitiator 2 2 2 2 2

Table 2. Composition of different formulations based

on methyl methacrylate.

Formulations (w/w %)
Materials M1 M2 M3 M4 M5

Methyl methacrylate 10 20 30 40 50
Methanol 88 78 68 58 48
Photoinitiator 2 2 2 2 2

proportions of oligomer (50–90 wt%) in methanol and 2% photoinitiator (Darocur-1173)

as shown in Table 1. The solution was mixed in a glass beaker and heated at 1008C for
20 min. Dried jute fabrics were soaked in the prepared solutions by hand lay-up technique.
Soaked jute fabrics were then directly irradiated under UV light of 2-KW intensity (254–
313 nm, model Me-200 UV, IST Technique, Germany). The conveyor speed was 4 m/min.
The irradiated samples after 24 h of radiation were subjected to various characterization
processes. Five layers of UV-treated jute fabrics were placed between the platens of the
heat press machine and heated at 1408C for 5 min under a pressure of 4 tons using Carver
Laboratory press (model 2518). Then the composites were cooled to room temperature
using another press, cut to the desired size, and kept in a polythene bag within desiccators.
Again, in order to improve the property of jute fabrics, different proportions of MMA
(10–50%) were mixed in methanol with photoinitiator as shown in Table 2. Jute fabrics
were soaked in these solutions and coated with optimized oligomer by hand lay-up
technique and then cured under UV radiation. Urea of different concentrations (0.5–2%)
was added to the optimized solution (30% MMA) and cured under UV radiation. The
tensile properties of the composites were determined using an UTM testing machine
(model H50 KS-0404, Hounsfield Series S, UK). The load capacity was 5000 N; efficiency
was within 1%. The crosshead speed was 10 mm/min and gauge length was 20 mm. For
bending property measurement, the crosshead speed was 10 mm/min and span distance
was 40 mm. Tensile strength and three-point bending tests were carried out following DIN
53455 and DIN 53452 standards methods, respectively.

RESULTS AND DISCUSSION

Effect of Jute Content on the Mechanical Properties of the Composite

The effect of jute content on the mechanical properties of jute oligomer composites was
measured and the results are presented in Figures 1 and 2. Tensile strength (TS) and
bending strength (BS) of the composites were found to increase on increasing the
percentage of jute content in the composite (Figure 1). The highest TS and the BS at
4 H.A.H. KHAN ET AL.

55 wt% jute content composites were found to be 46.7 MPa and 47.3 MPa, respectively.
Tensile modulus (TM) and bending modulus (BM) of the composites also followed the
same trend like TS and BS and is shown in Figure 2. The highest TM and the BM of the
composites (55% jute) were found to be 1.16 GPa and 1.31 GPa, respectively. So, it is clear
that 55% jute-content composites showed the best mechanical properties and this was

50

45
TS and BS (MPa)

40

35

30

TS BS
25
30 35 40 45 50 55 60
Jute content (wt%)

Figure 1. Variation of tensile and bending strength against jute content.

1.7

1.3
TM and BM (GPa)

0.9

0.5

TM BM

0.1
30 35 40 45 50 55 60
Jute content (wt%)

Figure 2. Variation of tensile and bending modulus against jute content.

Urethane Acrylate-based Composites 5

considered as the optimized content of jute. The influence of jute content on mechanical
properties of composites may be explained by the homogeneity of fiber in composite and
wettability of the urethane matrix. Owing to the lower level of fiber in the matrix, non-
homogeneity of the fiber is observed in the composite material. As a result, proper load
transfer is not possible by the composites. Fiber–matrix adhesion is the key to a strong
interface. Optimum adhesion between fiber and matrix can be achieved by maximizing
wetting tension. Wetting tension can be maximized by maximizing the physical
interactions at the molecular level between matrix and fiber and spontaneous wetting of
the fiber surface with liquid matrix in order to maximize the flow density at the interface
[19]. At high levels of fiber content, poor wettability of matrix and improper orientation
of fiber is found in the matrix material. This may cause decrease in the mechanical
properties of the composite above 55% jute.

Mechanical Properties of the Urethane-based Composites: Effect of UV Radiation

Jute-reinforced urethane-based composites were treated with different intensities

(termed as number of UV pass) of UV radiation and the results are shown in Figures 3
and 4. Best mechanical properties were obtained when jute fabrics were coated with the
formulation F3 (Table 1) and cured under UV radiation at 8th pass. Mechanical properties
of the composite, such as 14 and 17% increase in TS and BS, 15 and 4% increase in TM
and BM were found under 8th UV pass relative to untreated urethane acrylate-based
composites. Surface modification of jute fabrics by UV treatment usually increased the
polarities of fiber surface, which increased the fiber wettability as well as composite
strength. An intense UV radiation results in a decrease of mechanical properties, a reduced
degree of polymerization is observed, and two opposing phenomena such as photo-
crosslinking and photo-degradation take place simultaneously when UV radiation is used
as a method of surface pretreatment [20–24].

60

55
TS and BS (MPa)

50

45

TS BS
40
0 4 8 12 16
No. of UV passes

Figure 3. Tensile and bending strength of irradiated composites against number of UV passes.
6 H.A.H. KHAN ET AL.

Effect of Monomer (MMA) on the Performance of the Composites

In this investigation, jute fabrics were first soaked (10 min) in different MMA solutions
(10–50%) and the formulation is given in Table 2. Soaked jute fabrics were cured under
UV radiation at different intensities (6–18 passes) expressed by the number of passes. The
results of polymer loading (PL) are shown in Figure 5 against the number of the UV pass

1.6

1.4
TM and BM (GPa)

1.2

TM BM
1
0 4 8 12 16
No. of UV passes

Figure 4. Tensile and bending modulus of irradiated composites against number of UV passes.

13
Polymer loading (%)

10

4
3 6 9 12 15 18 21
No. of UV passes

10% 20% 30% 40% 50%

Figure 5. Polymer loading against number of passes of UV radiation as a function of different concentrations.
Urethane Acrylate-based Composites 7

with respect to different monomer concentrations. It was observed that PL values

increased with radiation intensities up to the 12th pass; after attaining a maximum value,
PL values decreased with increase in the number of the UV pass. The decrease of PL values
after attainment of the maximum could be caused by the photo-degradation of higher UV
radiation dose [21]. The highest PL value (11.67%) was obtained at 30% MMA solution
and at 12th UV pass. Percentages of PL increase with MMA up to 30%, but more than
30% monomer concentration reduces the PL of jute fabrics with MMA. For a particular
polymerization reaction, the extent of polymerization increases with monomer concentra-
tion up to a certain limit. After the maximum value of PL, it decreases with increase in
monomer concentration. At higher MMA concentration, the radical–radical recombina-
tion reaction among growing MMA molecules leading to poly-MMA may be dominant.
Thus, the reaction between MMA and jute cellulose is diminished. At low concentrations,
the PL value is less because the monomer promotes rapid free-radical propagation reaction
with the help of photoinitiator leading to network polymer structure through graft
copolymerization reaction via their double bonds [22]. As MMA concentration increased,
the amount of residual concentration is also increased resulting in faster rate of formation
of three-dimensional (3D) network structure causing restricted mobility. Another factor
could be that the swelling of the cellulose backbone with MeOH is insufficient due to low
MeOH concentration. As a result, monomer molecules are incapable of penetrating the
cellulose molecules in the presence of low solvent concentrations. This may cause a smaller
number of reacting sites at the cellulose backbone and thus continue to reduce the active
sites as MeOH concentration decreases with higher MMA concentration.
The changes in the TS of the treated composites are depicted in Figure 6 against the
number of UV passes as a function of different monomer concentrations. TS increases
with irradiation dose up to the 12th pass and then decreases as the irradiation doses are
increased beyond the 12th UV pass. It is also observed that TS values increase with MMA

65
10% 20% 30%
40% 50%
Tensile strength (MPa)

60

55

50
3 6 9 12 15 18 21
No. of UV passes

Figure 6. Tensile strength of the treated composites against number of UV passes as a function of different
concentrations.
8 H.A.H. KHAN ET AL.

1.6
10% 20% 30%
40% 50%

1.5

Tensile modulus (GPa) 1.4

1.3

1.2
3 6 9 12 15 18 21
No. of UV passes

Figure 7. Tensile modulus of the treated composites against number of UV passes as a function of different
concentrations.

concentrations up to 30%, but above 30% MMA, the TS decreases with UV radiation
exposure. Samples treated with 50% MMA attained 55.37 MPa which is very low
compared to 30% MMA. The highest TS (62.9 MPa) is obtained by the sample treated
with 30% MMA. It may be noted that the increase of TS with increasing the number of the
UV passes may be due to the inter-crosslinking between the neighboring cellulose
molecules that occurs under UV exposure. It is observed that TS value of the composite
increases up to a certain limit and then decreases due to the two opposing phenomena such
as photo-crosslinking and photo-degradation that take place simultaneously under UV
radiation. In lower doses, free radicals are stabilized by combination reaction; as a result,
photo-crosslinking occurs. The higher the number of active sites generated on the
polymeric substrate, the greater the grafting efficiency. But at higher radiation, the main
chain may be broken and polymer may be degraded into fragments; as a result, TS and BS
decrease with increasing UV dose. The enhancement of TM of the treated sample is
depicted in Figure 7 against the number of UV passes with respect to different MMA
concentrations. The TM value of the composite for 30% MMA solution at 12th pass of
UV radiation is about 1.51 GPa which is the highest among all the concentrations
investigated. The TM decreased with the increase of UV radiation doses after the 12th UV
pass. TM increases with UV radiation, and the 12th UV pass shows the maximum values
in almost cases. A fairly similar trend in TS increment was also observed in Figure 6, in
which 30% shows the maximum TS.

Effect of Urea on the Composites

To investigate the effect of urea as an additive on the mechanical properties of urethane-

based composite, a minute amount of urea was added into the optimized solution (30%
MMA). Urea was used at different concentrations (0.5–2%) in MMA þ MeOH solution
and it was observed that among all the concentrations, 1% urea produced the best results.
Urethane Acrylate-based Composites 9

Table 3. Effect of urea on TS and TM of 30% MMA treated jute fabric oligomer composites.

Concentrations of urea (w/w)

Mechanical properties
0.5% 1% 2%
No. of UV
passes TS (MPa) TM (GPa) TS (MPa) TM (GPa) TS (MPa) TM (GPa)

4 63.23  0.42 1.27  0.034 64.31  0.35 1.48  0.021 62.77  0.27 1.36  0.029
6 65.12  0.43 1.43  0.023 65.78  0.39 1.57  0.034 63.68  0.47 1.47  0.027
8 66.77  0.36 1.62  0.029 68.35  0.44 1.69  0.025 65.12  0.31 1.58  0.023
10 64.89  0.21 1.58  0.021 66.17  0.28 1.62  0.021 63.15  0.42 1.49  0.019
12 62.79  0.52 1.49  0.031 63.14  0.35 1.55  0.035 61.29  0.34 1.42  0.032

Enhanced properties of the composites (TS ¼ 68.4 MPa and TM ¼ 1.69 GPa) were
achieved with 1% urea at 8th pass of UV radiation, which was increased the TS and
TM by about 46 and 50% respectively compared to untreated composite. The results of TS
and TM are presented in Table 3. Urea possesses 4C ¼ O group adjacent to a nitrogen
atom having a lone pair of electrons which are activated to form a bridge between the
monomer and the cellulose through the additive. Oxygen has more affinity toward
electrons; thus, the electron clouds are densely populated around the oxygen atom of
4C ¼ O groups, thereby pulling more electrons toward the oxygen from the urea of the
nitrogen atom or its vicinity, creating some favorable conditions for the augmentation of
the monomer and the additive units with the cellulose backbone polymer of the substrate
[23]. Urea is an inclusion compound whose properties would assist partitioning by
complexing with monomer. This can lead to an increase in monomer concentration at a
grafting site and thus enhance reactivity at that site.

CONCLUSIONS

Jute fabric-reinforced urethane oligomer based thermoset composites were successfully

prepared by conventional hand lay-up method. The mechanical properties revealed that
the composites possessed promising values. In order to improve the mechanical properties,
jute fabrics were treated with the monomer (MMA) followed by UV curing and their
mechanical properties were evaluated. The highest TS and TM of the composites (jute
fabrics were treated with 30% MMA at 12th pass of UV radiation) were found to be
62.95 MPa and 1.51 GPa respectively, which was increased by about 35 and 34%
compared to the untreated composite. Again, urea of different concentrations (0.5–2%)
was added to the optimized solution (30% MMA) and cured under UV radiation and the
mechanical properties of the resulting composites (1% urea treated) increased the TS by
about 46% and TM by about 50% at a certain intensity of UV radiation. It can be
concluded that both the monomer (MMA) and the minute amount of urea (1%) have a
positive impact on the mechanical property enhancement of the urethane-based
composites.

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