Review Article

Journal of Thermoplastic Composite

Materials
Cellulose triacetate 1–15
ª The Author(s) 2019
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polystyrene composite DOI: 10.1177/0892705719847249

journals.sagepub.com/home/jtc

Usman Saeed , Uthman Dawood

and Arshad Mahmood Ali

Abstract
The increase in demand for natural fibers in development of the composites has grown
rapidly due to the cost-effectiveness, low density, biodegradability, and renewability.
The lack of appropriate interfacial bonding between the cellulose fibers and the
thermoplastic matrix is one of the disadvantages faced during their application. Also,
the properties of composite made of thermoplastic polystyrene (PS) and cellulose
acetate fibers are not compatible due to the poor wettability and interfacial adhesion.
In the study presented, PS reinforced with cellulose triacetate is being prepared by
melt blending in a twin-screw extruder with the induction of fusabond (FB). The
influence of the cellulose acetate and FB content on PS composite is being investigated
using thermogravimetric analysis, tensile test, dynamic mechanical analysis, scanning
electron microscopy, and X-ray photoelectron spectroscopy. The addition of FB
enhances interfacial adhesion demonstrated by the improvement in storage modulus,
reduction in damping peak value, and the increase in thermal stability of the composite.
The inclusion of FB not only increases the % elongation but also improves the impact
strength of the cellulose triacetate-reinforced PS composite under dynamic loading.
Moreover, the interaction between PS with cellulose triacetate fiber is indicated by the
results of X-ray photospectroscopy and fracture surface morphology. The results
show that the addition of FB is suitable for use in cellulose fiber-reinforced PS com-
posite for packaging, automotive, and biomedical applications.

Keywords
Polystyrene, cellulose triacetate, Fusabond MB E100D, thermomechanical properties,
X-ray photo spectroscopy

Chemical and Materials Engineering Department, Faculty of Engineering, King Abdulaziz University, Jeddah,
Saudi Arabia

Corresponding author:
Usman Saeed, Chemical and Materials Engineering Department, Faculty of Engineering, King Abdulaziz
University, Jeddah 21441, Saudi Arabia.
Email: [email protected]
2 Journal of Thermoplastic Composite Materials XX(X)

Introduction
The natural fibers are becoming a preferential material choice when it comes to the
reinforcement materials for thermoplastic composites. The natural fibers can be cellu-
lose, bamboo, palm, pine, jute, and sisal. The natural fibers are superior to synthetic
fibers because they are biodegradable and the products made by the natural fiber are
sustainable. Cellulose can be sourced naturally from wood or lint attached to cotton
seeds. Cellulose is made of repeating glucose units that have the chemical formula
C6H7O2 (OH)3.1 Also, cellulose is found plentifully in nature as it occurs in all plant cell
walls (i.e. flax, hemp, kenaf, and ramie) and can also be synthesized by some bacteria
(i.e. gluconacetobacter, agrobacterium, pseudomonas, rhizobium, and sarcin).2,3 The
products made with cellulose fiber-reinforced thermoplastic composites can have
improved specific strength as they have low density and stiffness.4,5 Moreover, the
toughness and strength of manufactured goods will be better than their predecessors.
Also, the cellulose fibers are cost-effective, adaptable, and biodegradable. The cellulose
fiber minimizes the wear of machinery in comparison to synthetic fiber6 and the use of
cellulose fiber in the products minimizes the health hazards. Moreover, the two types of
nano reinforcements that can be obtained from plant cellulose are nanofibrillated cel-
lulose (NFC) and nanocrystalline cellulose (NCC). Several studies center on bionano-
composites, which uses natural fiber due to their abundance and potential for substituting
carbon fiber and glass fiber in the future.7 NCCs serve as a suitable renewable alternative
for bionanocomposites due to its nanoscale cellulose fiber composition, high strength
and stiffness, low weight, biodegradability, and application in the development of
nanocomposite material.8,9
The cellulose has remarkable reinforcing properties due to its abundant hydroxyl
group within the large surface area, but the absence of appropriate interfacial bonding
between the cellulose fibers and the thermoplastic matrix is a major disadvantage.10,11
The reason behind the weak interfacial bonding is the hydrophobic nature of ther-
moplastic matrix and hydrophilic characteristic of cellulose fiber. The incompatibility
of cellulose fiber and thermoplastic matrix causes the adhesion to be weaker and the
dispersion of the fiber to be inhomogeneous. The composite generated have inferior
quality and properties because of inhomogeneous dispersion, which results in the
agglomeration of fibers.10
The use of coupling agent can improve the interfacial adhesion between the cellulose
and the matrix. In addition, the presence of a coupling agent will also help the transfer of
load in between the matrix and fiber uniformly.11 Furthermore, the enhancement in
properties with the help of coupling agent occurs because of immobilization of the
matrix chain and improvement in bonding.
The thermal analysis is helpful in establishing a better understanding of the thermal
stability and structure of the intended material. The thermal analysis will also be useful
in studying the moisture content, weight loss, and volatility as these factors effect on the
degradation and processing condition of the composite. The decomposition of natural
fiber occurs in two or three stages under the process of weight loss, which is performed in
the controlled temperature between 25 C and 800 C.12-15
Saeed et al. 3

The dynamic mechanical analysis (DMA) can be also be used to examine the outcome
of temperature on the mechanical properties of the composite. The study of viscoelas-
ticity of the intended composite will help to predict the behavior of composite under
dynamic stress. Dong and Gauvin16 used DMA study and have reported extensively on
the viscoelastic characteristics of interfacial region of the carbon fiber-reinforced epoxy
composite. Guo and Ashida17 have described the dynamic moduli (G0 and G00 ) and loss
tangent (tan d) of polyethylene terepthalate fiber-reinforced thermoplastic elastomer by
utilizing DMA. Hwang et al.18 inspected the orientation, aspect ratio, and interlaminar
stress of the fiber on the damping behavior of the composite.
Hwang et al.18 accounted for dynamic viscoelastic characteristics of low-density
polyethylene composites reinforced with short sisal fibers and pineapple fibers.
George and Mohanty et al.19,20 examined the variability in the damping modulus (G0 ,
G00 ) and tan d by combining coupling agent with jute fiber and high-density poly-
ethylene (HDPE) polymer. Huang and Zhang21 investigated the interaction of HDPE
and wood particles by considering the dynamic and mechanical properties. The result
of Huang and Zhang showed that when the agglomeration of wood particles is
decreased, the storage modulus is enhanced.
The aim of the intended study is to explore the performance of cellulose triacetate
fiber (CF)-reinforced polystyrene (PS) composite. The study was conducted by inves-
tigating thermal, mechanical, and dynamic mechanical properties. The Fusabond MB100
D (FB) is being used as a coupling agent in the CF-reinforced PS composite.

Experiment
Preparation
PS (Petrochemical (M) Sdn. Bhd., Pasir Gudang, Johor, Malaysia) was extruded
with CFs (Arabian Japanese Company, LLC, KSA) and FB E MB 100 D (Dupont,
Michigan, USA) in variable concentrations. The FB E MB 100 D is maleic
anhydride-grafted HDPE, which contains high graft level and can also be used as an
interfacial modifier to enhance the adhesion. The pellets of PS were initially dried in
a vacuum oven at a temperature of 60 C for 12 h to remove moisture before pro-
cessing through the twin-screw extruder. The CF had average fiber length, which
was within 0.3  LW  0.4 mm and diameter of 10 mm. The fiber length and
diameter were determined by measuring the length of 250 fibers. The PS was
reinforced with four concentrations of 10, 20, 30, and 40% wt of cellulose triacetate
with the induction of FB MB-100D (3–5 wt.%) as a coupling agent. The extruder
was operated at 180 C with a screw speed of 90 rev min1. The PS/CF/FB com-
posites were blended for 30 min. Finally, the PS composites were injection molded
at 150 C and pressed into the test specimen die for 10 min.

Characterization
The thermal stability of cellulose triacetate-reinforced PS composite was characterized
using TGA Q50 (TA Instruments, Newcastle, USA) having an accuracy of +1 C. The
4 Journal of Thermoplastic Composite Materials XX(X)

alumina pan was used to contain 10 mg samples of composite, and the samples were
heated from 20 C to 600 C at a heating rate of 10 C min1 under nitrogen atmosphere.
The DMA 242 (Netszch, Germany) was used to determine the loss modulus G0 ,
storage modulus G00 , and loss factor (tan d) of the specimens as a function of temperature
using dual cantilever having specimen dimensions of 40  12  5 mm3. The mea-
surements were performed at a frequency of 1 Hz, a strain rate of 0.1% with the heating
rate of 2 C min1, and the temperature range from 20 C to 100 C.
The tensile tests were carried out with the use of Instron Tensile Testing machine
(Instron, Norwood, USA) of 50 kN with load accuracy of 0.05%. The prepared
samples were loaded at a constant 5 mm min1 crosshead speed and 0.50-N preload.
The three samples having the geometry of ASTM D638 type IV for each compo-
sition were tested at 25 C.
The Charpy test was performed with JB W300 J impact testing machine (Test lab,
Poland). The potential impact energy, raise angle, and impact speed of the testing
machine were 150 + 1 J, 150 and 5.2 m s1, respectively. According to ASTM D256,
the dimensions of samples were 10  10  55 mm3 having a notch size of 2 mm.
The morphology of the fracture surface of the PS/CF/FB composites was observed
with a JEOL JSM-7600F field-emission scanning electron microscope (Peabody, Mas-
sachusetts, USA) at an accelerating voltage of 10 kV.
The XPS measurements were made on an XR 50 spectrometer (SPECS GmbH,
Germany) operating at a base pressure of 1  10 8 mbar. A dual-anode non-
monochromatic magnesium Ka X-ray source was used to irradiate the sample surface
with 13.5 kV and 150 W. The sample was positioned at a take-off angle of 90 between
the sample surface and the direction of photoelectrons. The XPS data were acquired
utilizing a PHOIBOS 150 MCD-9 hemispherical energy analyzer operating in fixed
analyzer transmission mode with an accuracy of +1% mass concentration. During all
characterization technique, each sample was tested three times to verify the results of PS/
CF/FB composite.

Results and discussion

The thermal decomposition of neat PS and PS/CF composite at the temperature range of
30–600 C are presented in Figure 1(a). The decomposition and degradation of neat PS
initiated at 343 C also shows the complete thermal depolymerisation at 462 C. The first
weight loss appears between 330 C and 370 C with the addition of 10% CF, which is
related to heat vaporization of water. Meanwhile, the thermal depolymerization of PS
and degradation of CF causes the second drop of weight, which starts at 377 C and
finishes at 468 C.20 The introduction of 20%, 30%, and 40% CF in PS provides ana-
logous behavior with a slight deviation in temperature, as shown in Figure 1(a) and
Table 1. The outcome of experimental data demonstrates that the gradual addition of CF
in PS has insignificant consequences on the thermal decomposition temperature. The
thermal decomposition of PS/20%CF with the addition of 3% and 5% FB is shown in
Figure 1(b) as an example. The figure shows that the first weight drop happens at 331 C.
Meanwhile, the main degradation starts at 379 C and comes to an end at 474 C. The
Saeed et al. 5

Figure 1. (a) TG curves of PS/CF (b) TG/DTG curves of PS, PS/CF, and PS/CF/FB.
TG: thermogravimetric; PS: polystyrene; CF: cellulose acetate fiber; FB: Fusabond.

Table 1. Results of the TG analysis.

Fisrt transition Second transition

PS/ Peak Peak Residual

cellulose/ temperature Weight temperature Weight weight %
FB Ti ( C) Tf ( C) ( C) loss (%) Ti ( C) Tf ( C) ( C) loss (%) (550 C)

100/0/0 343.86 462.88 423.67 99.76 — — — — 0.23

90/10/0 330.80 370 347.34 18.80 377.20 468.86 426.06 78.20 2.56
80/20/0 331.81 370.89 347.37 18.90 376.39 469.13 423.06 78.43 2.66
70/30/0 331.54 368.37 347.43 19.10 378.46 469.73 424.72 76.09 3.02
60/40/0 331.19 368.13 347.60 19.30 381.77 472.50 427.55 76.91 3.78
87/10/3 331.60 369.45 347.01 19.30 379.61 468.39 424.53 77.67 3.29
77/20/3 331.45 370.15 348.65 22.20 379.09 469.86 425.13 73.45 3.69
67/30/3 331.71 370.54 348.20 22.30 379.42 470.10 424.3 74.67 4.08
57/40/3 331.47 370.49 348.15 22.30 382.62 473.78 424.97 74.72 4.34
85/10/5 331.61 369.97 348.59 19.60 378.19 469.02 425.55 74.45 4.01
75/20/5 331.37 370.13 348.49 22.30 378.47 470.59 424.62 73.68 4.66
65/30/5 331.75 369.56 348.76 22.40 379.42 471.70 425.77 72.93 5.52
55/40/5 331.87 370.67 348.79 22.50 383.61 474.78 425.43 71.97 5.94

TG: thermogravimetric; PS: polystyrene; CF: cellulose acetate fiber; FB: Fusabond.

exploration demonstrates that the thermal stability of PS/CF composite is not influenced
by the addition of FB.
The derivative thermogravimetry (DTG) curves of neat polyester and 20% CF with
3% and 5% FB is also shown in Figure 1(b) as an example. The DTG data show minor
temperature dissimilarities of neat PS, PS/CF, and PS/CF/FB composite when compared
to TG data. The shoulder peak appears at 330 and 370 C when CF is being added. The
appearance of shoulder peaks demonstrates the dehydration of CF. The prominent DTG
6 Journal of Thermoplastic Composite Materials XX(X)

peak of PS/CF and PS/CF/FB appears when the maximum thermal degradation occurs at
374 C and finishes at 474 C The appearance of prominent peaks with slight variation
indicates that CF and FB have minor influence on the stability of polyester. At the same
time, it is being noted that the decomposition of CF and depolymerization of PS
molecular chains coincides with the appearance of the prominent peaks.
The investigation of PS thermogravimetric scans in the range from 30 C to 300 C
shows a weight loss of 0%. Moreover, the degradation of PS appears in the temperature
range between 343 C and 462 C demonstrating a weight loss of 99.76%. This weight
loss of 99.76%, as shown in Table 1, can be coincided with the thermal cracking of the
hydrocarbon chains of PS. The addition of 10%CF to 40%CF presents a weight loss of
18–22%, respectively, and can be correlated with the first transition of temperature in
PS/CF composites. The significant weight loss of 72–78% occurs between 377 C and
474 C with the addition of 10%, 20%, 30%, and 40% CF, as shown in Table 1. The
weight loss can be linked to the second temperature transition peak, which leaves behind
a residue of 2.5–3.78% of ash content. Furthermore, the main reason for the stability of
CF is the presence of hydrogen bond, which makes it possible for thermal energy to be
distributed equally.21 Also, it can be witnessed that the addition of CF in the PS prevents
the complete degradation of the PS matrix at a temperature of 550 C. The prevention of
complete decomposition can be attributed to ash content when the fiber content is
increased. In addition, it is observed that the residue content increases from 3.78% to
5.94% when FB is introduced in the PS/CF composite, as shown in Table 1. The FB has
an insignificant effect on the thermal behavior of the PS/CF composite even when the
ash content is in considerable quantity. The thermal decomposition temperatures and
weight losses of PS, PS/NFC and PS/CF/FB composites are presented in Table 1.
Figure 2(a) shows the value of the storage modulus (G0 ) of the PS/CF/FB composites
as a function of temperature. The storage modulus of the PS matrix is enhanced with the
inclusion of CF. The rise in modulus is due to the increase in the stiffness of the matrix
because of the reinforcement facilitated by the fibers.22,23 The sharp decline in the
modulus of PS/CF composite occurs with the rise in temperature of the glass transition
section. The decrease in the modulus can coincide with the molecular mobility of
polymer chains above the glass transition temperature (Tg).23 In the meantime, the
outcomes show that CFs have reinforced the neat PS. This reinforcement can be noticed
by studying the difference between the glassy and the rubbery state of the storage
modulus G0 when compared with neat PS and PS/CF composites. The consequences of
the use of the coupling agent on the storage modulus of PS/30%CF composite with 3 and
5% FB is also shown in Figure 2(a). The storage modulus is higher and increases with the
increase of FB in PS/CF composite. The FB introduces the interfacial adhesion between
the CF and the PS matrix, attributing to the improvement of the storage modulus of the
CF/PS composite. Also, the molecular mobility in the interfacial region is reduced when
FB improves the fiber matrix adhesion. The lower molecular weight of FB100D allows
effective diffusion in the polymer matrix, which causes the most needed entanglement
within the PS matrix.24 The maleic anhydride in the FB introduces significant interfacial
attraction because the FB forms the bonds between the hydroxyl in the CF and the maleic
anhydride in FB. The improved adhesion results in the increase of storage modulus as the
Saeed et al. 7

Figure 2. (a) Storage modulus of PS/CF/FB, (b) loss modulus of PS/CF/FB, (c) tan d of PS/CF, and
(d) tan d of PS/CF and PS/CF/FB.
PS: polystyrene; CF: cellulose acetate fiber; FB: Fusabond.

CF and PS matrix becomes more compatible. Moreover, the analogous behavior has
been noticed with all concentrations of PS/CF composite when the FB is added. The
maximum value of storage modulus is shown in Table 2.
The loss modulus, G00 , as a function of the temperature for the PS/CF composite is
shown in Figure 2(b). The inclusion of CF resulted in the expansion of the G00 peak when
compared to the PS matrix peak. The loss modulus curve as a result of the free movement
of the polymer chains reaches a maximum value and decreases for the higher tem-
peratures. The increase in loss modulus peak height with varying CF content is likely to
have occurred due to the inhibition of the relaxation process within the PS/CF composite.
The relaxation occurs due to the enhancement in the number of chain segments and the
presence of free volume upon fiber addition.25,26 Also, the decrease in the G00 decreases
the internal friction which results in the increase in dissipation energy.19 Additionally,
the presence of CF adds to free mobility of polymeric molecules which helps to enhance
the flexibility of composite.23 The PS/30%CF composite with the addition of 3% and
5%FB results in the higher value of G00 is shown in Figure 2(b) as an example. The higher
value of G00 is related to maleic anhydride presence in FB, which develops the bond
between the PS matrix and the CF. The existence of bonds increases the height of loss
8 Journal of Thermoplastic Composite Materials XX(X)

Table 2. Storage modulus, E0 , tan d, Tg, and A of PS/CF/FB.

PS/CF/FB (wt%) Storage modulus (MPa) tan d peak height Tg ( C) A

100/0/0 1141 2.23 121.9 —

90/10/0 1301 1.97 121.6 0.21
80/20/0 1536 1.76 121.2 0.38
70/30/0 1430 1.65 122.4 0.42
60/40/0 1374 1.44 120.5 0.46
87/10/3 1312 1.91 121.3 0.45
77/20/3 1355 1.84 121.2 0.59
67/30/3 1345 1.52 122.3 0.65
57/40/3 1458 1.34 122.6 0.74
85/10/5 1445 1.79 122.4 0.68
75/20/5 1433 1.68 122.3 0.71
65/30/5 1317 1.18 122.4 0.75
55/40/5 1429 1.07 122.8 0.81

PS: polystyrene; CF: cellulose acetate fiber; FB: Fusabond; Tg: glass transition temperature; A: adhesion factor.

modulus peak and increases the viscous response with the relaxation mechanism of the
PS/CF composite.
The mechanical damping, tan d, values of the PS/CF are lower than the neat PS, as
shown in Figure 2(c). The values show that the tan d value decreases as the con-
centration of CF fibers increases in the composite. The reduction in the tan d occurs
due to the restriction in movement of the PS molecules caused by the presence of stiff
fiber.27 Moreover, the improvement in the interfacial adhesion occurs due to the
addition of FB, which shrinks the tan d peak height to 1.07 of PS/CF/FB, as shown in
Figure 2(d) and Table 2. The reduction in the tan d peak increases the molecular
relaxation and facilitates the PS/CF composite to absorb a higher amount of energy.
The improvement in absorption behavior is being introduced because of the strong
interfacial adhesion causing less dissipation of energy in the composite. The Tg values
obtained from tan d peak for the PS, PS/CF, and PS/CF/FB are presented in Table 2.
The Tg values of the PS matrix show a slight variation when the CF and FB is
incorporated. The variation may be attributed to the restriction imposed by the fibers
on the molecular motion in the PS matrix.
The relative damping of the composite and polymer matrix can be used to estimate the
adhesion factor A by considering the volume fraction of fiber as shown in equation (1):28
1 tan dC
A¼ 1 ð1Þ
ð1  Vf Þ tan dp

where tan dc and tan dp are the relative damping of composite and polymer and Vf is the
volume fraction of the fiber. The value of A decreases with the addition of FB, as shown
in Table 2. The lower level of adhesion factor A is related to the strong adhesion. The
lower value of A occurs due to the reduction in tan d c. However, the decrease in tan dc
Saeed et al. 9

Figure 3. (a) Tensile behavior of PS/CF composite and (b) tensile behavior of 77% PS/20%CF/
3%FB and 75%PS/20%CF/5%FB.
PS: polystyrene; CF: cellulose acetate fiber; FB: Fusabond.

Table 3. Mechanical properties of PS/CF/FB.

Tensile strength Elastic modulus Impact toughness

PS/CF/FB (MPa) (GPa) %Elongation (kJ m2)

100/0/0 17.63 + 0.20 0.93 + 0.02 94 + 3.2 5.37 + 0.05

90/10/0 19.19 + 0.25 0.96 + 0.03 87 + 5.1 5.26 + 0.07
80/20/0 21.41 + 0.27 1.04 + 0.05 72 + 7.1 4.16 + 0.10
70/30/0 23.68 + 0.19 1.07 + 0.09 68 + 4.1 3.62 + 0.12
60/40/0 25.13 + 0.25 1.09 + 0.01 59 + 2.4 3.14 + 0.06
87/10/3 19.12 + 0.10 0.99 + 0.02 97 + 4.0 5.91 + 0.10
77/20/3 20.5 + 0.23 1.07 + 0.01 86 + 3.5 4.75 + 0.09
67/30/3 22.30 + 0.32 1.13 + 0.03 75 + 3.8 3.97 + 0.08
57/40/3 24.40 + 0.11 1.26 + 0.04 66 + 4.4 3.55 + 0.11
85/10/5 19.01 + 0.09 1.00 + 0.02 102 + 3.3 5.98 + 0.11
75/20/5 20.17 + 0.22 1.14 + 0.01 92 + 4.3 5.12 + 0.04
65/30/5 21.90 + 0.17 1.19 + 0.06 81 + 2.7 4.17 + 0.06
55/40/5 24.05 + 0.16 1.31 + 0.05 71 + 6.1 3.73 + 0.08

PS: polystyrene; CF: cellulose acetate fiber; FB: Fusabond.

happens due to the reduction in the molecular mobility in the vicinity of fiber, which
enhances the interaction between the PS matrix and the CF.
The stress (s) and strain (e) behavior of PS with the addition of cellulose fiber and FB
are presented in Figure 3(a) and (b) with the summary of results in Table 3. The tensile
strength and elastic modulus of neat PS are 17.63 MPA and 0.9 GPa. The increase of CF
content increases the elastic modulus up to 20% and tensile strength up to 21% but
decreases the %elongation of PS. The elastic modulus and strength gradually increase
with the addition of CF content probably because of the steady enhancement of rigidity
10 Journal of Thermoplastic Composite Materials XX(X)

in the PS matrix, as shown in Figure 3(a) and (b). The decrease in the %elongation upto
20% with the increasing CF loading can be attributed to the rigid behavior of the PS
matrix, as shown in Table 3. In addition, the FB coupling agent strongly impacts on the
mechanical characteristics, as shown in Figure 3(b) and Table 3. The decline in the
strength with FB in PS/CF composite is 18–25%. This characteristic might be credited
to the reaction that occurs between the OH group of CF and the anhydride group of the
FB. Also, the %elongation increases up to 20% with the addition of the coupling agent.
The use of FB increases the dispersion of CF in the PS matrix reducing the fiber–fiber
interactions. The reduced fiber–fiber interaction allows the matrix to transfer the
applied stresses to the fiber. Similarly, the improvement in the interfacial adhesion
enhances the stress transfer from the PS matrix to the stiffer CF increasing, in turn, the
elastic modulus.
Table 3 shows the impact strength of PS with the increasing content of CF and FB.
The impact strength of neat PS is 5.69 kJ m2. The impact strength of PS/CF composite
is lower than the neat PS indicating the decline in toughness. Furthermore, Table 3 shows
that the impact strength of PS/CF composite reduces up to 48%. The reduction in impact
strength might be due to the stiffness of the CF that restricts the mobility of the polymer
chains and also due to the poor interfacial interaction between the CF and the PS
polymer. On the other hand, the rise in the impact strength has been observed up to 20–
34% with the addition of FB in comparison to PS/CF composite. The improvement in the
impact strength of PS/CF/FB composites occurs due to the better adhesion between
polymer blends and CF bonding. The enhanced adhesion implies that the composite with
the addition of FB is tougher than PS/CF under dynamic loading. The improved impact
energy with the addition of FB corresponds to the reduction of tan d peak and low value
of adhesion factor A, as shown in Figure 2 and Table 2.
The tensile fracture surface of PS/CF (80/20) composite is shown in Figure 4. Figure
4(a) shows the CF pulled out and the voids on the surface indicating the poor interfacial
adhesion between the PS matrix and the CF. Meanwhile, the fracture of PS/CF/FB (75/
20/5) presents the rough and uneven surface due to load transfer from the PS matrix to
the CF. Also, the decrease in the number of voids suggests the improvement in the
interfacial affinity and adhesion between the CF and the PS matrix, as shown in Figure
4(b). Furthermore, Figure 4(c) shows the twist in the single fiber presenting the fracture
of PS/CF/FB composite due to load transfer in the fiber. The load transfer in the fibers
occurs due to the improvement in the interfacial affinity and adhesion by the addition
of FB MB E 100 D as a coupling agent. The addition of FB introduces a considerable
amount of compatibility between the PS and the cellulose fiber, which is being pre-
sented by the increased storage modulus and enhanced mechanical properties of the
PS/CF/FB composites.
The XPS high-resolution scan was conducted on the C1 s and O1 s regions of the
specimen to determine the types of carbon–oxygen bonds. The XPS peaks of PS, PS/CF,
and PS/CF/FB with the variable intensities of the functional groups corresponding to C1
s and O1 s region are shown Figure 5. The binding energy and corresponding bond type
with their atomic concentrations are shown in Table 3. The PS is formed by covalent
bonding of carbon, hydrogen, and oxygen. Except for hydrogen, the C–H, C–C, C-–O–H,
Saeed et al. 11

Figure 4. SEM micrograph of (a) fracture surface of PS/20%CF, (b) fracture surface of PS/20%CF/
5%FB, and (c) fracture of single fiber in PS/20%CF/5%FB.
SEM: scanning electron microscopy; PS: polystyrene; CF: cellulose acetate fiber; FB: Fusabond.

and C–O–C bonds are presented in the PS with their peak positions and mass% con-
centration, as shown in Figure 5(a) and Table 4. The addition of CF to the PS increases
the concentration of carbon–oxygen bond in the PS/CF composite, as it is shown in
Figure 5(b). The increase is expected since the major component of CF has a large
percentage of carbon–oxygen in their chemical structure than the PS,29 which is shown
by the slight rise of atomic concentration in C–O–C¼O and C–C from 0.324 at.% to
0.653 at.%. Meanwhile, the rise in C–O–C¼O is observed from 0.427 mass% to 0.859
mass%. Nicole et al.29 presented the peak of C–C to C–H at 285.0 eV, which corresponds
to the bonding of the polymer matrix with the CF. The FB E MB100D (maleic anhy-
drides high-density polyethylene) contains C–O–H and C–O–C bonds. The C–O–H and
C–O–C structure increases the graft reactivity of the carbon–oxygen bond in the polymer
matrix.30,31 The availability of the hydroxyl bond leads to a generation of an interaction
between the PS matrix and the CF, which enhances the properties of composites.
However, the rise in graft reactivity creates the cross-linking or strong adhesion at the
interface due to the rise of shoulder peaks in C1 s region, as it is illustrated in Figure 5(c).
The trend exhibits the variation in the concentration of C–O–H/C–O–C bonds from
4.326 mass% to 5.365 mass % leading to an increase in the O/C ratio, which is attributed
to the addition of FB, as shown in the Table 4. Moreover, the decrease in concentrations
of C–H and C–C bonds occurred from 91.598 mass % to 90.984 mass % due to the
addition of FB in PS/CF composite. Nevertheless, it is assumed that the molecular chain
12 Journal of Thermoplastic Composite Materials XX(X)

Figure 5. XPS peaks in C1 s and O1 s region (a) PS, (b) PS/CF composites, and (c) PS/CF/FB
composite.
XPS: X-ray photospectroscopy; PS: polystyrene; CF: cellulose acetate fiber; FB: Fusabond.

Table 4. XPS peaks with binding energy and bond type of O1 s, C1 s, and N1 s regions with mass%
concentration.

PS PS/CF PS/CF/FB

Mass % Mass % Mass %

Bond type BE (eV) concentration BE (eV) concentration BE (ev) concentration

O 1s 532.17 6.883 532.53 4.07 532.48 4.781

C 1s 284.82 92.9 248.83 95.92 248.78 95.219
N1s 400.17 0.21 — — — —
O 1s_1_C¼O, O–C¼O 531.48 2.467 — — — —
O 1s_2_C–O–H, C–O–C 532.25 3.557 532.36 3.649 532.41 5.786
O 1s_3_C–O–C¼O 533.5 0.427 533.91 0.859 533.88 0.995
C 1s_1_C–H–C–C 284.81 87.796 284.8 91.598 284.8 90.854
C 1s_2_C–O–H, C–O–C 286.19 4.11 286.2 4.326 286.37 5.365
N1s 400.17 0.21 — — — —

XPS: X-ray photospectroscopy; PS: polystyrene; CF: cellulose acetate fiber; FB: Fusabond; BE: binding energy.
Saeed et al. 13

of FB E MB 100D is shorter than PS and cellulose fibers. These shorter length molecular
chains have distinct feature, which make the use of FB limited in improving the inter-
facial adhesion.26 The limited improvement of PS/CF/FB composite is being confirmed
by the enhancement in the impact energy and decrease in damping tan d peak.

Conclusion
The effect of FB is being successfully studied on the PS/CF composite, which was
produced by the twin extruder. The TG thermograms of the PS/CF composite present the
negligible effect of FB. Also, the increase in the modulus and the decrease in tan d with
the addition of FB improves the molecular relaxation of the examined PS/CF composite.
The reduction in the tan d peak increases the molecular relaxation and facilitates the PS/
CF composite to absorb a higher amount of energy. Furthermore, the impact energy
decreases with the incorporation of CF due to the rigidity of the fiber, which leads to
insignificant interfacial strength. Meanwhile, the addition of FB in PS/CF increases the
impact strength and % elongation revealing the interfacial strengthening between the PS
matrix and the CF. The analysis of impact energy shows that the addition of 3% and 5%
FB integrates higher impact energy, which increases the toughness of the PS/CF com-
posite. Moreover, it was observed that the C–O–H and C–O–C bonds, which are present
in FB assist in forming a conjugated structure. Finally, the interfacial adhesion between
the PS and CF is confirmed by the presence of cross-linking and interfacial bonding. The
PS/CF/FB composite fabricated in this study is intended to be used in the packaging,
automotive, and biomedical applications.

Acknowledgement
The authors would like to extend their gratitude for the King Abdulaziz University
Jeddah for supporting this research project.

Funding
The author(s) received no financial support for the research, authorship, and/or
publication of this article.

ORCID iD
Usman Saeed https://orcid.org/0000-0002-2380-7881

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