Composites Communications 15 (2019) 129–134

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Composites Communications
journal homepage: www.elsevier.com/locate/coco

Short Communication

Thermal behavior of PC-ABS based graphene filled polymer nanocomposite T

synthesized by FDM process
Vijay Tambrallimatha, R. Keshavamurthyb,*, Saravanabavan Dc, Praveennath G. Koppadb,
G.S. Pradeep Kumard
a
Automobile Engineering, Dayananda Sagar College of Engineering, Bangalore, 560078, India
b
Mechanical Engineering, Dayananda Sagar College of Engineering, Bangalore, 560078, India
c
Mechanical Engineering, Dayananda Sagar University, Bangalore, 560078, India
d
Department of Mechanical and Automobile Engineering, Christ (Deemed to be University), Bangalore, 560074, India

ARTICLE INFO ABSTRACT

Keywords: Property enhancement of polymers could be achieved through blending of two or more polymers and via ad-
Graphene dition of filler materials to meet the application requirements. In the present investigation Polycarbonate (PC)
Nanocomposite and Acrylonitrile Butadiene Styrene (ABS), the two polymers were blended together and Graphene platelets as
Electron microscopy nanofiller was added in the ratio of 0.2, 0.4, 0.6 and 0.8 wt% respectively. Polymer blend and graphene platelets
Differential scanning calorimetry
were mixed at appropriate temperature and extruded out in the form of filament of 1.75 mm diameter. Filament
was used as a feed material for Fused Deposition Modelling (FDM) to develop the test samples. The nano-
composites developed using FDM were subjected to differential Scanning Calorimetry (DSC) and
Thermogravimetric Analysis (TGA) to study the effect of graphene platelets. Addition of graphene platelets
resulted in significant increase in Young's modulus with highest value of 4.038 GPa obtained for nanocomposite
with 0.8% graphene content. Thermal analysis showed that addition of graphene platelets increases the glass
transition temperature and reduces the mass with increase in temperature.

1. Introduction nanomaterial adds to increased surface to volume ratio and dispersion

The tailored made materials with requisite properties could be
achieved by amalgamation of polymers individually [1]. The mixing of
materials has to be chosen appropriately in a way to enhance the de-
sired properties. Acrylonitrile Butadiene Styrene (ABS) is widely used
polymer for its easy availability, toughness, processablity and luster.
However, the heat distortion temperature is in the range of 100 °C to
110 °C which would easily change the properties of the desired spe-
cimen. The mechanical properties of ABS is also lesser than other
polymers [2,3]. On the otherhand, Polycarbonate (PC), a versatile re-
liable material with high impact strength, dimensional stability and
toughness, is widely used polymer for high strength applications [3,4].
Addition of small amount of ABS to PC makes it a composite polymer of
combined properties with higher strength and easy processability. The
properties of the PC-ABS blend; higher processability than ABS and
greater strength than PC make it sort after material in Fused Deposition
Modelling (FDM) [5,6]. To refine the properties, adding certain mate-
rials of varied size from micro to nano boosts the applicability and
functionality of the developed micro or nanocomposite. Usage of
is also well established in the polymer network [7]. With numerous
advantages of using nanoparticles as filler in polymer composites adds
to its applicability in vast dimension of industries ranging from auto-
mobile, aerospace, packaging and construction. Graphene, with 2d
lattice structure having very high thermal conductivity, electrical con-
ductivity and mechanical properties, is utmost suited filler material.
Owing to their outstanding properties graphene is used to reinforce
metal, ceramic and polymer matrix materials [8–10]. Fused Deposition
Modelling (FDM) is comparatively a new, advanced, sustainable and
green technology in the prospects of manufacturing sector. The core
idea of this method of building up a material is basically to reduce
down the material wastage and construct the required material of any
complex geometry in a layer by layer format [11,12]. The utilization of
efficient materials through Additive manufacturing (AM) needs to gain
a rapid momentum. The exponential advancements by researchers to
use these parts for functional applications is increasing to the level of
utilization of structural supports in architectural design mainstream
and chassis manufacturing for automobiles. However, the main scale
application of polymers in load bearing industries and as a functional

*
Corresponding author.
E-mail address: keshavamurthy.r@gmail.com (R. Keshavamurthy).

https://doi.org/10.1016/j.coco.2019.07.009
Received 10 May 2019; Received in revised form 24 July 2019; Accepted 25 July 2019
Available online 26 July 2019
2452-2139/ © 2019 Published by Elsevier Ltd.
V. Tambrallimath, et al.
Fig. 1. (a) SEM and (b) EDAX pattern of graphene platelets.
part still remains a void. This drawback has led the utilization of 3D
printed polymer parts only to the scope of prototype. Hence, exploita-
tion of new materials is possible by using composite polymer materials
that enhances the overall mechanical and thermal properties of the
fabricated parts.
Identification of deviation in properties of mechanical and thermal
behavior in polymer nanocomposite is being established through the
weight percent addition of reinforcement to the matrix. Ning et al. [13].
have made a comparative study of tensile and flexural properties with
variation of carbon fiber content from 0 to 15% reinforced in ABS to
analyse the effects. Similarly Tekinalp et al. [14]. have made a com-
parative study of tensile and modulus behavior between conventional
manufacturing and FDM over different fiber loading. Tensile properties
incremental values were noted with increase in fiber content for both
conventional and FDM parts. Uniform dispersion and orientation was
achieved in FDM. However, for 40% loading, clogging of nozzle was
observed for parts manufactured through FDM. Vijay et al. [15]. have
studied the characterization behavior of graphene in PC-ABS matrix, by
varying its content from 0.01 vol% to 0.25 vol%. Microstructure stu-
dies, dimensional accuracy and density measurements were carried out
to analyse the impact of parameters on increased volume percentage of
graphene. Similarly, the same author determined the variation in
thermal conductivity by increased addition of copper particles to ABS
matrix. Copper particles were added in 2.5 and 5 wt% and were com-
pared for thermal conductivity of nanocomposite developed by FDM. It
was noted that an increase in copper content increased the thermal
conductivity of the polymer nanocomposite [16]. The study conducted
by Aw et al. [17]. showed that with the addition of filler content the
tensile strength of the polymer nanocomposite increase until 11 wt%.
Further, addition of nanoparticle reduced the tensile strength and sto-
rage modulus. Dul et al. [18]. through their experimentation have
found that increase thermal stability of the developed part would in-
crease up to certain addition of nanoparticle and would reduce in its
value for further addition of the nanoparticle. Most of these works
demonstrated that weight percentage of reinforcement significantly
influenced the various properties of nanocomposites. As for as me-
chanical properties are concerned multistep method of determining the
Young's modulus was one among many methods developed, that gave
similar results with experimentation. Nafiseh Nikfar et al. [19]. devel-
oped a model that is related to aspect ratio of nanoparticle and per-
colation threshold. The graph of these two parameters determines the
mechanical properties of the developed polymer nanocomposite. The
lower values of threshold predict lower tensile modulus and strength. It
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Composites Communications 15 (2019) 129–134
was noted that increase in threshold reduced the mechanical properties
with improper interphase formation and vice versa. Kovacs model
which is limited to few applications is further developed by considering
the tunnel and interphase regions to be separate. The determination of
resistance of tunnelling and interphase, percolation threshold are cal-
culated using simple equations. The experimental values were in
agreement with model values, further it was predicted that, long, thin
and straight CNTs improve the conductivity to greater extent [20]. In
the light of the above, present study focuses on development of PC-ABS
nanocomposites with different weight percentage of graphene. Young's
modulus of nanocomposites was obtained by conducting tensile tests as
per ASTM E8M-15a standard. Influence of graphene platelets content
on thermal characteristics (DSC and TGA), were studied by varying its
content from 0.2 wt% to 0.8 wt% in steps of 0.2 wt%.
2. Materials and methods
2.1. Preparation of nanocomposite
The polymer PC and ABS in the form of pellets was procured from
M/s Polyshakti Polymers, Bangalore, India. Fig. 1 shows the field-
emission scanning electron microscope (FESEM) micrograph and EDAX
of multi-layered graphene platelets procured from M/s Adnano Private
Limited, India. The pellets of PC-ABS were mixed in the ratio of 70:30.
Utilizing the oven, the pellets were dried at a temperature of 110 °C for
about 2 h to remove the moisture content. The dried pellets were mixed
in the blender and then added to the compounding machine with a
specification of 30 mm twin screw co-rotating lab screw extruder with a
rotational speed of 105 rpm at GLS Polymers, Bangalore.
Five variation of specimens were developed and given the name S1,
S2, S3, S4 and S5, where S1 is a mixture of PC-ABS, S2 corresponds to
PC-ABS+0.2 wt% Graphene, S3 corresponds to PC-ABS + 0.4 wt%
Graphene, S4 is PC-ABS + 0.6 wt% Graphene and S5 corresponds to
PC-ABS + 0.8 wt% Graphene. The compounding temperature was
varied in the range 200 °C to 240 °C and extruded with a filament
diameter of 1.75 ± 0.05 mm. Fig. 2 shows the photograph of extruded
filaments with different graphene platelet content.
2.2. Fused deposition modelling (FDM)
The development of material in layer wise was carried out in the
process of FDM. The nozzle is used to lay the filament in X and Y di-
rection and the platform on which the product is to be developed moves
V. Tambrallimath, et al.
Fig. 2. Photograph of filaments of various graphene proportions.
along z direction [21]. The optimization of process parameters depicts
the efficient behavioural property of the developed product. Lay up
angle, orientation, layer thickness and speeds of nozzle are the para-
meter which could be controlled for optimal performance. Variation of
each parameter will effectively vary the desired properties of final na-
nocomposite [22]. Praman 3D printer, 300 mm3, enclosed chamber
from Global 3D labs, Bangalore was used for the printing specimens.
Tensile test as per ASTM E8M-15a standard was performed on the de-
veloped nanocomposites to obtain Young's modulus. All samples were
subjected to differential scanning calorimetry (DSC) to determine the α
Fig. 3. (a) Dispersion of graphene in PC-ABS and EDAX (b) Graphene nanopartilce in PC-ABS.
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Composites Communications 15 (2019) 129–134
transition of molecular chain from amorphous form to glassy form with
increase in temperature [23]. Sample of 8 g was used under the influ-
ence of Nitrogen gas in enclosed container for determination of Tg. The
heating-cooling-heating cycles were measured with an increment of
10 °C/min from 27 °C to 308 °C. Further, thermal properties were
analysed using thermogravimetric analyzer. 11 gm of each sample was
used for the determination of variation in weight loss with constant
heat rate. The temperature range chosen for this study was 30 °C to
570 °C.
3. Results and discussion
3.1. Microstructure and Young's modulus
Fig. 3 (a) shows FESEM images of PC-ABS-graphene nanocomposite
which depicts fairly homogenous dispersion of graphene platelets
throughout PC-ABS matrix. The presence of graphene platelet in na-
nocomposite was confirmed by performing EDAX which showed carbon
as major peak. The bonding between the graphene platelets and PC-ABS
matrix was found to be good with no interfacial defects.
Table 1 shows the Young's modulus of nanocomposites with dif-
ferent graphene platelet content. From Table 1 it is quite clear that the
addition of graphene platelet led to increase in the Young's modulus of
PC-ABS matrix. For instance the unreinforced PC-ABS showed Young's
V. Tambrallimath, et al. Composites Communications 15 (2019) 129–134

Table 1 forces and other chemical bonds that are formed due to interaction
Young's Modulus for different samples. between two phases. These aggregates can be summed up to be cluster
Sample Modulus (E, GPa) of sturdy particles and agglomerates are loosely held particles which
could be detached with application of load. It is also noted that ag-
PC-ABS 2.531 gregation/agglomeration leads to reduction in Young's modulus.
PC-ABS+0.2 wt% Graphene 2.800
However, these two characteristics alone would not be able to decide
PC-ABS+0.4 wt% Graphene 3.230
PC-ABS+0.6 wt% Graphene 3.818
the optimal parameters of polymers, dispersion of nanoparticles and
PC-ABS+0.8 wt% Graphene 4.038 interaction between the two constituents plays an important role [26].

3.2. Differential scanning calorimetry (DSC)

In order to study the important property changes in developed

Fig. 4. Graph of heat flow vs temperature.
Table 2
DSC values for the samples at various Tg.
Sample Peaks
PC
PC-ABS 107.2 °C
PC-ABS+0.2 wt% Graphene 110.5 °C
PC-ABS+0.4 wt% Graphene 111.2 °C
PC-ABS+0.6 wt% Graphene 111.7 °C
PC-ABS+0.8 wt% Graphene 113.4 °C
modulus of 2.531 GPa while with the addition of 0.2% graphene pla-
telet the Young's modulus increased to 2.8 GPa. With the increase in
graphene platelet content the Young's modulus increased and reached a
maximum value of 4.038 GPa for 0.8% graphene platelet. The increase
in Young's modulus for nanocomposite with 0.8% graphene platelet as
compared to unreinforced PC-ABS is about 59.54%. One can observe
that the increase is quite significant indicating better interfacial
bonding between the two constituents of nanocomposites. Here better
blending, extrusion and FDM techniques helped in good dispersion and
interfacial bonding between graphene platelet and PC-ABS matrix. This
is very important aspect from load transfer point of view as good in-
terfacial bonding ensures efficient load transfer from PC-ABS matrix to
graphene platelets. These results are well supported by previously
published research. For instance Zare et al. [24] showed that the en-
hanced mechanical performance can be well established by proper
mechanism of stress transfer through polymer to nanoparticles, which
could be achieved by good adhesion between the two phases. Young's
modulus clearly indicates the increment in thermal and mechanical
properties which is indicative of fine level of interaction and formation
of interphase between the nanoparticle and polymer matrix. Addition of
nanoparticles has its own advantages in comparison to micro fillers.
Addition of nanofiller (< 5 wt%) will greatly enhance the mechanical,
physical, thermal and barrier properties of the polymer nanocomposite
[25].
Generally, addition of nanoparticles in polymers results in forma-
tion of aggregates/agglomerates due to the presence of van der Waals
material during thermal transition and the effect of graphene platelets
on thermal behavior, differential scanning calorimetry (DSC) studies
were conducted. Thermal properties such as glass transition tempera-
ture (Tg) and melting temperature (Tm) were determined using DSC
thermograms. In particular the DSC studies of PC-ABS and its nano-
composites hold high significance since ABS being amorphous polymer
which is characterized by its Tg. Fig. 4 shows the DSC curves for PC-ABS
blend and its nanocomposite filaments with different concentration of
graphene platelets. The values of peak temperature are indicated in
Table 2. It can be observed from the curves that both PC-ABS blend and
its nanocomposites showed two transitions. In case of PC-ABS blend,
first peak was observed at 107.2 °C which corresponds to glass transi-
tion temperature for ABS. Second peak corresponding to glass transition
temperature of PC was observed at 136.5 °C. In line with the present
results, Uzma et al. [27] observed two transition temperature signals at
111.67 °C and 159.16 °C for ABS and PC respectively. On the other
hand, transition temperature points at 100.30 °C and 127.57 °C was
observed for ABS and PC respectively for PC-ABS blend by Yazdi and
Sullivan [28]. From both the work is it is observed that the Tg is highly
dependent on heating and cooling rates. Further, with addition of
ABS graphene from 0.2 to 0.8 wt% in the steps of 0.2 wt% to the PC-ABS
blend, considerable increase in transition temperature was noticed. For
136.5 °C
138.3 °C PC/ABS blend with 0.2% of graphene, two transition peaks at 110.5 °C
139.8 °C and 138.3 °C were observed. Similarly, for highest content of graphene
140.6 °C of 0.8%, the transition peaks were observed at 113.4 °C and 146.9 °C.
146.9 °C The peak occurring at first transition temperature in all curves re-
presents polystyrene which is mainly due to the styrene which is major
copolymer in ABS. Considerable increase in Tg for nanocomposites
implies that graphene was able to increase the service temperature by
restricting the mobility of polymer chains. The constraining effect in-
dicates sufficient miscibility between the PC-ABS blend and graphene
platelets. The extent of crosslinking between PC-ABS and graphene is
found to increase with the increase in graphene content which is quite
evident from increase in Tg. The increase in Tg indicates restriction of
mobility of polymer chains by uniformly dispersed graphene platelets.
Unlike in some cases where increase in filler content leads to clustering
thereby decreasing the Tg of nanocomposites [29,30]. In addition to this
the inclusion of graphene in PC-ABS blend nanocomposites requires
additional heat from the heating system as compared to blend thereby
increasing the transition temperature. Similar observations were re-
ported by Pastorini and Nunes [31], where they found that the mica
restricted the mobility of ABS matrix.
3.3. Thermogravimetric analysis (TGA)
The thermal stability of PC-ABS blend and its nanocomposites
consisting of varying graphene platelets content were studied using
thermal gravimetric analysis (TGA). The TGA curves as shown in Fig. 5
indicates that both PC-ABS blend and its nanocomposites follow single-
step degradation with a rapid mass loss in the temperature range of
416–575 °C. Tabulated values of TGA analysis is shown in Table 3. TGA
curve for PC-ABS blend showed 89.8% of mass drop at 416 °C while
remaining mass drop observed around 548 °C. Rapid mass loss at 416 °C
corresponds to the decomposition of styrene acrylonitrile which is a

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V. Tambrallimath, et al. Composites Communications 15 (2019) 129–134

Fig. 5. Graph of glass transition vs temperature.

Table 3 ABS matrix enhanced the Young's modulus significantly. Glass transi-
TGA analysis for reduction in mass. tion studied with respect to temperature showed two transitions tem-
Sample Mass reduction perature for ABS and PC respectively which increases with increase in
the graphene volume. With addition of 0.8 wt% of graphene in PC-ABS
Degradation Decomposition glass transition temperature increased by 5.7% and 7.6% for ABS and
Temperature Temperature PC respectively. A decrease in thermal degradation by 3.8% is recorded
PC-ABS 416 °C 548 °C for 0.8 wt% graphene addition in PC-ABS, where thermal decomposi-
PC-ABS+0.2 wt% Graphene 420.9 °C 558.5 °C tion was increased by 4.9%. The incremental values suggest the addi-
PC-ABS+0.4 wt% Graphene 424.3 °C 562.4 °C tion of graphene has enhanced the thermal stability.
PC-ABS+0.6 wt% Graphene 428.7 °C 567.8 °C
PC-ABS+0.8 wt% Graphene 432 °C 575.1 °C
Appendix A. Supplementary data

major copolymer of ABS. On the other hand, the graphene platelet re-
inforced PC-ABS nanocomposites revealed improvement in thermal
stability of nanocomposites. The thermal stability was found to improve
by 4.9–16.1 °C when compared with PC-ABS blend with graphene. For
PC/ABS blend with 0.2% of graphene, the degradation initiated at
420.9 °C with 90.5% mass drop followed by decomposition at 558.5 °C.
Here the improvement in thermal stability was about 4.9 °C which is
minimal when compared to rest of the nanocomposites. The highest
improvement of about 16.1 °C was seen in nanocomposite with 0.8% of
graphene platelet. The initial degradation was seen at 432 °C and de-
composition was observed at 575.1 °C indicating highest thermal sta-
bility. Along with the thermal stability, the maximum degradation
temperature of PC-ABS blend was shifted to higher value after in-
corporation of graphene platelets. Overall, trend depicted increase in
thermal stability with the increase in graphene platelets in PC-ABS
nanocomposites. Graphene with good interfacial bonding with PC-ABS
matrix showed high degree of crosslinking due to which bond breaking
in nanocomposites was much tougher than that of PC-ABS blend
without graphene. Due to high thermal stability of graphene alone, the
heat release rate in case of nanocomposites was much lesser than that of
PC-ABS blend. Along with this the uniformly dispersed graphene serves
an outstanding insulator and physical barrier for transport of volatile
products during decomposition. This claim is well supported by the
similar observations made by research works comprising of ABS and/or
graphene [32–34].
4. Conclusions
Novel graphene platelet reinforced PC-ABS nanocomposites were
successfully developed by FDM technique. This technique helped in
good dispersion and improved interfacial bonding between the two
constituents of nanocomposite. Addition of graphene platelets to PC-
Supplementary data to this article can be found online at https://
doi.org/10.1016/j.coco.2019.07.009.
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