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 Materials Today: Proceedings xxx (xxxx) xxx

Contents lists available at ScienceDirect

Materials Today: Proceedings

journal homepage: www.elsevier.com/locate/matpr

Micromechanical and experimental analysis of mechanical properties

of graphene/CNT epoxy composites
Sumit Nagar a,⇑, Kamal Sharma a, Nitin Kukreja a, Manoj Kumar Shukla b
a
Department of Mechanical Engineering, GLA University, Mathura, UP 281406, India
b
KNPC Jabalpur, Rajiv Gandhi Technical University, Bhopal, India

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

Article history: Amine functionalized multilayer graphene (Af-MLG) and amine functionalized multi wall carbon nano
Received 29 December 2019 tube (CNT) (Af-MWCNT) were fabricated by sonication method, maintaining the ratio of both the nano
Accepted 13 February 2020 fillers as 1:1 and were termed as hybrid fillers due to its composition. The effects of both these fillers
Available online xxxx
on the mechanical properties of epoxy composites were researched upon. Hybrid composite samples
were characterized using Scanning electron microscope (SEM) for morphology study. The mechanical
Keywords: behaviour of graphene reinforced epoxy based composites (Gr/Ep-C) were studied using continuum
Micro-mechanical model
based micromechanical models such as Halpin –Tsai (H-T) and Mori –Tanaka (M
T). The mechanical
Nano composites
Graphene
properties were depicted graphically. The variation in properties have been evaluated with respect to fil-
Mechanical Properties ler weight fraction and aspect ratio using a well defined MATLAB code. The ratio of longitudinal and
transverse modulus to the modulus of matrix was then plotted with weight fraction and aspect ratio.
When weight fraction and aspect ratio were increased from 0 to 10% and 0–1000 for H-T and M-T models
an expected enhancement in the ratio of longitudinal modulus to the modulus of matrix was noticed.
Ó 2020 Elsevier Ltd. All rights reserved.
Selection and of the scientific committee of the 10th International Conference of Materials Processing and
Characterization.

1. Introduction design of more custom-made nano composite structure results in

Nano fillers for the improvement of overall properties have
already proved themselves as the most prominent reinforcing can-
didates of composites. Different types of graphene as reinforcing
agent was used by researchers. Graphene’s role in nanotechnology
can be easily understood because of its extraordinary mechanical
Properties and strength [1,2], high electron mobility and thermal
conductivity [3,4]. By using AFM (atomic force microscopy) Lee
et al. [1] calculated tensile strength of pristine graphene as 130
GPa. They also reported that the strength of single layer Graphene
was more than 200 times that of steel, but stiffness was found out
as 1 TPa. AFM was used to calculate stiffness of single layer gra-
phene by Frank et al. [5] and it was reported to be 0.5 TPa.
In case of Polymer nano composite the reinforcement by nano-
filler improves physical and mechanical properties significantly
[6–8]. Because of low cost, the enhancement of properties and par-
ticularly good ability to get processed, Gr/Ep-C have attracted
tremendous interest among scientists. Because of such effects
⇑ Corresponding author.
E-mail address: sumit12_ab@rediffmail.com (S. Nagar).
very lighter structural components. The Gr/Ep-C have shown
improvements in variety of mechanical properties like mechanical
strength and modulus of elasticity. When the volume fraction was
varied from 0.1 to 6% Wang et al. [9] determined the effect of
spherical graphene nano filler on Young’s modulus. Zarasvand
et al. [10] showed for nano composites containing 0.25, 0.5, 0.75
and 1.0 wt% of graphene nano- fillers the results of H-T microme-
chanical model. Gao et al. [11] proved that the yield strength of
nano composites severely increased by adding a small volume per-
cent of graphene. They noticed a remarkable increment of 92, 128,
and 78% in strength of graphene- Al2024, Al-graphene and Cu-
graphene nano particles based composites, when they have been
added in weight fractions of 0.7, 1.5 and 2.5% respectively. Kim
et al. [12] established the dependency of interfacial interactions
between silica and epoxy matrix, using micro mechanical model
(MM) simulations with the degree of cross linking.
The reinforcement efficiency of Gr/Ep-C especially for mechan-
ical properties, strongly depends upon filler aspect ratio ‘a’, filler
modulus, filler weight fraction and interfacial adhesion. So far lim-
ited researches have been done by considering the effect of filler
(graphene) structural parameters on the mechanical properties of
nano composite.

https://doi.org/10.1016/j.matpr.2020.02.407
2214-7853/Ó 2020 Elsevier Ltd. All rights reserved.
Selection and of the scientific committee of the 10th International Conference of Materials Processing and Characterization.

Please cite this article as: S. Nagar, K. Sharma, N. Kukreja et al., Micromechanical and experimental analysis of mechanical properties of graphene/CNT
epoxy composites, Materials Today: Proceedings, https://doi.org/10.1016/j.matpr.2020.02.407
2 S. Nagar et al. / Materials Today: Proceedings xxx (xxxx) xxx
This particular research is more focused on the strengthening
efficiency of graphene filler based composites using continuum
based MM models and experiment was done on hybrid fillers com-
posed of (Af-MLG) and (Af-MWCNT) and their synergistic effects
were investigated upon. The sample was fabricated keeping ratio
of (Af-MLG) and (Af-MWCNT) nano fillers 1:1 [13,14]. The tensile
strength and tensile modulus were computed using computer
based tensile testing machine. H-T and M-T models were used to
elucidate the effect of nano filler structural parameters on the
strengthening efficiency of Gr/Ep-C and graphene/CNT epoxy com-
posite [15]. To the best knowledge of the authors, the aspect ratio
’a’ of graphene filler was assumed to be constant in many of the
researches, hence more analytical studies were to be needed. Cur-
rent research also focused on higher aspect ratio’s of filler and its
corresponding effect on strengthening efficiency [16]. Further-
more, the effect of varying weight fraction on strengthening effi-
ciency of Gr/Ep-C was also investigated. To provide an ease to
the reader, a comparison between clay and graphene based com-
posites has also been done. MATLAB coding is done for whole ana-
lytical work.
2. Continuum and conventional filler based micromechanical
models
Theoretical and numerical models [17–25] predicted the
strengthening efficiency of Gr/Ep-C composites. Though a number
of mechanics based models have been designed to predict the
properties of filler based composite materials, however the analyt-
ical performance of Halpin-Tsai (H-T) and Mori-Tanaka (M-T) was
incredibly good, especially when they have been applied on nano
filler reinforced composites [23–25]. These MM models were
deployed to observe the effect of nano filler weight fraction (uf ),
aspect ratio (a), stiffness ratio (Ef/Em) on the mechanical properties
of Gr/Ep-C at macroscopic level [26–28]. The schematic illustration
of Gr/Ep-C composite has been shown in Fig. 1.
2.1. Halpin-Tsai (H-T) model
Reasonable information of reinforcement efficiency of compos-
ite materials was provided by H-T theory [18,19]. The three princi-
ple orthogonal directions used to calculate composite stiffness
corresponding to H-T model was shown by Fig. 2(a). The longitudi-
nal and transverse stiffness (E11and E33) of H-T model have been
expressed in Eqs. (1) and (2) respectively:
Fig. 1. Schematic illustration of graphene epoxy composite.
Please cite this article as: S. Nagar, K. Sharma, N. Kukreja et al., Micromechanical and experimental analysis of mechanical properties of graphene/CNT
epoxy composites, Materials Today: Proceedings, https://doi.org/10.1016/j.matpr.2020.02.407
E11 1 þ 2ðl=tf Þguf
¼ ð1Þ
Em 1
guf
E33 1 þ 2guf
¼ ð2Þ
Em 1
guf
Ef =Em
1
g¼

Ef =Em þ 2 l=t f
2.2. Mori-Tanaka (M-T) model
The best prediction for the properties was offered by M-T the-
ory for composites with respect to aspect ratios. Three principle
orthogonal directions used to calculate composite stiffness corre-
sponding to M-T model was depicted by Fig. 2(b). The longitudinal
and the transverse stiffness (E11 and E33) in M-T model have been
expressed in Eqs. (3) and (4) respectively where lis the filler length
and t f is the filler thickness.
E11 1
¼ ð3Þ
Em 1 þ uf ðA1 þ 2tm A2 Þ=A
E33 1
¼ ð4Þ
Em 1 þ uf ½
2tm A3 þ ð1
tm ÞA4 þ ð1 þ tm ÞA5 A=2A
where uf is the filler weight fraction ,tm is the Poisson ratio of the
matrix ,A; A1 ; A2 ; A3 ; A4 ; A5 are calculated from the matrix, filler prop-
erties and components of Eshelby tensor [23], which depend upon
filler aspect ratio (l=t f ) (where land t f are the major and minor diam-
eters of an ellipsoidal disk shaped inclusion) and dimensionless
elastic constant of the matrix.
The values of modulus of elasticity of fibre, modulus of elasticity
of the matrix (Ef and Em) Poisson ratio of filler, Poisson ratio of
matrix (tf and tm ) [26,27] and shear modulus of fibre and shear
modulus of matrix (Gf and Gm) taken in this paper are illustrated
in Table 1.
3. Experimental section
3.1. Material and experimental methods
Af-MLG, and Af-MWCNT fillers are procured from United Nan-
otech Innovations, Bangalore (India).
Epoxy resins commercially available as LY 556 with density
0.241 g/cm3 are purchased from Sakshi Dying and Chemicals, Delhi
(India). Multi layer Af-MLG has surface area 250 m2/g, bulk density
0.241 g/cm3. Af-MWCNT has average length 20 µm, outer diameter
20 nm, , surface area as 320 m2/g [28].
3.2. Fabrication of hybrid composite
The reinforcement of Af-MLG/Af-MWCNT fillers with pure
epoxy was utilized to obtain fabricated hybrid composite. Weight
fractions of fillers taken were 0, 0.25, 0.5, 1 and 2 wt% in 1:1 ratio.
The process followed for sample preparation by sonication method
is shown in the Fig. 3. The sample composition of fillers and matrix
as per sample configuration are shown in Table 2. Af-MLG/Af-
MWCNT fillers was diffused in epoxy resin along with ethanol
and sonicated to obtain proper mixture. Post curing of sample is
performed for 24 h in vacuum oven.
3.3. Characterizations
Tensile properties of hybrid epoxy composite are computed
using tensile test which is performed as per ASTM D 638 code at
 S. Nagar et al. / Materials Today: Proceedings xxx (xxxx) xxx 3

Fig. 2. Three principle orthogonal directions used to calculate nano-composite modulus corresponding to (a) H-T model (b) M-T model.

Table 1 modulus (E11 =Em ). As shown in Fig. 4(a) and (b), it was indicated
Elastic properties of fiber and matrix. by the test results that E11 =Em effectively enhanced as ‘a’ increases
Fiber and Matrix properties Ef and Em (GPa) tf and tm Gf and Gm (GPa)
(for different values of uf ) for both synergistically combined gra-
phene/CNT epoxy composite and graphene epoxy composite even
Fiber (Graphene) 1000 0.19 493
Matrix (Epoxy) 10.5 0.33 1.2
in high aspect ratio ranges, eventually reduces the possibilities of
fracture. A similar trend was also observed with an increase of
uf (for different values of ’a’) for both synergistically combined gra-
room temperature at a displacement rate of 5 mm/min. Morphol- phene/CNT epoxy composite and graphene epoxy composite i.e.
ogy of fractured images obtained after tensile test are further ana- increment then becoming constant at high aspect ratios. These
lyzed using Scanning electron microscope (SEM) enhancement in the properties may be due to the reason that as
aspect ratio increases, the tendency of filler getting embedded in
4. Results and discussion the matrix simultaneously increases, result of which an overall
improvement in strengthening efficiency. This can also be further
4.1. Comparison with Halpin-Tsai and Mori-Tanaka models justified with the fact that the elastic modulus of filler was always
higher as compared to matrix. The comparison between synergis-
Micromechanical models and their constitutive equations were tically combined graphene/CNT epoxy composite and graphene
used to examine the effect of uf , a and Ef =Em on longitudinal epoxy composite signifies that the strengthening efficiency of

Fig. 3. Fabrication process of hybrid composite.

Please cite this article as: S. Nagar, K. Sharma, N. Kukreja et al., Micromechanical and experimental analysis of mechanical properties of graphene/CNT
epoxy composites, Materials Today: Proceedings, https://doi.org/10.1016/j.matpr.2020.02.407
4 S. Nagar et al. / Materials Today: Proceedings xxx (xxxx) xxx

Table 2
Sample code and composition of hybrid composite.

Sample code Epoxy resin (Wt%) Filler (Wt%) Filler composition

Af-MLG Af-MWCNT
A 100 0 0 0
B: 99.75 0.25 0.125 0.125
C 99.50 0.50 0.25 0.25
D 99 1 0.50 0.50
E 98 2 1 1

Fig. 4. Variation of longitudinal modulus E11 observed using H-T model with (a) aspect ratio (a), and (b) Weight fraction of filler (uf ).

Please cite this article as: S. Nagar, K. Sharma, N. Kukreja et al., Micromechanical and experimental analysis of mechanical properties of graphene/CNT
epoxy composites, Materials Today: Proceedings, https://doi.org/10.1016/j.matpr.2020.02.407
 S. Nagar et al. / Materials Today: Proceedings xxx (xxxx) xxx 5

graphene/CNT epoxy composite is more than graphene epoxy com-

posite due to the synergistic effect of both graphene and CNT.
Fig. 5 illustrated the variation of (E11 =Em ) with respect to (Ef =Em )
at different values of aspect ratio (a) for synergistically combined
graphene/CNT epoxy composite and graphene epoxy composite.
It was clear from the graph that at initial stages the (E11/Em)
increases as (Ef =Em ) increases but after reaching a threshold value
no effect of adding the fiber was seen. This may be attributed to the
fact that if the fibre weight fraction increases beyond a certain
limit, the percentage of matrix phase was reduced and possibly
delamination occurs.
Fig. 6 (a) and (b) shows the variation in longitudinal modulus
with respect to ’a’ and ’uf ’ using M-T model and its constitutive
equations for synergistically combined graphene/CNT epoxy com-
posite and graphene epoxy composite. It was observed that E11/
Em increases very slowly, this may be justified by the inclusion of
Poisson’s ratio in M-T model. This results in contraction of the
nano-composite in the directions transverse to the direction of ten-
sile loading. M-T model demonstrated more traditional results as
compared to H-T model, because of the filler shape assumed in
Fig. 5. Variation of longitudinal modulus E11 observed using H-T model with
both the models. In M-T model fibers and disks have been consid-
modulus of elasticity Ef of fiber.

Fig. 6. Variation of longitudinal modulus E11 observed using M-T model with (a) aspect ratio (a), and (b) Weight fraction of filler (uf ).

Please cite this article as: S. Nagar, K. Sharma, N. Kukreja et al., Micromechanical and experimental analysis of mechanical properties of graphene/CNT
epoxy composites, Materials Today: Proceedings, https://doi.org/10.1016/j.matpr.2020.02.407
6 S. Nagar et al. / Materials Today: Proceedings xxx (xxxx) xxx

ered as ellipsoidal particles whereas in H-T model constitutive

Fig. 7. Variation of transverse modulus E33 observed using H-T and M-T models
with respect to Weight fraction of filler (uf ).
equations fibre was treated as fibre and disks as platelet [29].
The variation of transverse modulus to modulus of matrix
E33 =Em with respect to uf has been shown in Fig. 7. Both the models
produced nearby same trend because aspect ratio ’a’ was not con-
sidered in the constitutive equations of models.
In order to validate the results obtained from the present
research, they have been compared with Weon et al. [29]. For bet-
ter understanding the aspect ratio’s of nano fillers were taken same
as considered by Weon et al. [29]. An improvement of about 2–11%
was noticed in longitudinal modulus of nano composite for same
aspect ratio’s and weight fraction this may be attributed to the dif-
ferent fillers along with different matrix used in micromechanical
models, as illustrated in Table 3.
The results obtained in the current research were finally com-
pared with Weon et al. [29] as shown in Fig. 8. The strengthening
efficiency of nano-composite using disk type graphene nano-filler
showed better results as compared to polyamide 6-clay filler used
by Weon et al. [29]. This may be due to the variation in aspect ratio
of both the nano-fillers.

Table 3
Comparison of results obtained in current research with Weon et al. [29].

a u% E11 =Em [29] (V 1 ) E11 =Em for SL (Single Layer) Percentage (%) " Difference jV 1
V 2 j
V 1 þV 2  100
Gr/Ep-C (V 2 ) 2

87 4 7.7279 7.9476 2.8031

6 10.9839 11.4373 4.0443
8 14.1710 14.9377 5.2678
10 17.2914 18.4489 6.4772
132 4 10.8809 11.3249 3.9989
6 15.4522 16.3675 5.7530
8 19.8012 21.3325 7.4454
10 23.9439 26.2217 9.0811
180 4 14.0413 14.7916 5.2044
6 19.8038 21.3339 7.4389
8 25.1362 27.6564 9.5475
10 30.0851 33.7700 11.5414

Fig. 8. Comparison of results obtained in current research with Weon et al. [29].

Please cite this article as: S. Nagar, K. Sharma, N. Kukreja et al., Micromechanical and experimental analysis of mechanical properties of graphene/CNT
epoxy composites, Materials Today: Proceedings, https://doi.org/10.1016/j.matpr.2020.02.407
 S. Nagar et al. / Materials Today: Proceedings xxx (xxxx) xxx 7

4.2. Experimental Characterization, morphology and mechanical

characterization

4.2.1. Mechanical characterization

Fig. 9. Tensile strength and tensile modulus of composite found experimentally.
On each composite sample codes Mechanical test is performed
and the performance of fabricated composites were taken as aver-
age values of results for analysis purpose. The tensile stress beha-
viour of hybrid composites experimentally is shown in Fig. 9.
Tensile strength and modulus of hybrid composite is indicated in
Figs. 10 and 11 found by H-T and M-T models respectively. Tensile
strength increment was obvious continuously up-to 0.5 wt% filler
concentration; however above 0.5 wt% a decrease in tensile prop-
erties is observed. An improvement of 52% in tensile strength has
been observed for hybrid composite with filler loading 0.5 wt%,
in comparison to pure epoxy composite. Similarly, tensile modulus
increases by 19.1% when filler loading is 0.25 wt%, in comparison
to pure epoxy composite. Thus sample code C with 0.5 wt% filler
loading exhibits optimum results in terms of tensile properties.

Fig. 10. Tensile strength and tensile modulus of composite by Halpin-Tsai method.

Fig. 11. Tensile strength and tensile modulus of composite by Mori Tanaka method.

Please cite this article as: S. Nagar, K. Sharma, N. Kukreja et al., Micromechanical and experimental analysis of mechanical properties of graphene/CNT
epoxy composites, Materials Today: Proceedings, https://doi.org/10.1016/j.matpr.2020.02.407
8 S. Nagar et al. / Materials Today: Proceedings xxx (xxxx) xxx
Fig. 12. SEM Images of Af-MLG/Af-MWCNT hybrid epoxy composite with nano-filler wt% (a) 0 (b) 0.25 (c) 0.50 (d) 1 (e) 2.
However, above 0.5 wt% of filler reinforcement, a decrease in
tensile modulus value is revealed due to lower dispersion of filler
which increases fillers aggregation. Thus best results in terms of
mechanical properties are investigated for hybrid composite with
0.5 wt% filler content due to homogeneous mixture of composite
as confirmed by SEM micrographs.. An increased performance in
the form of tensile properties is obtained [28].
4.2.2. Morphology analysis
The fractured surfaces of hybrid composite samples are ana-
lyzed using SEM micrographs as shown in Fig. 12 (a)-(e). Optimum
dispersion of fillers in epoxy resin is exhibited by sample B and C.
Moreover agglomeration of fillers in 1 wt% is observed. Microstruc-
ture further degrades for quantity to 2 wt% indicating presence of
crack initiation and propagation.
5. Conclusions
Continuum based Halpin-Tsai and Mori-Tanaka micromechan-
ical models were deployed to predict the mechanical properties
of Gr/Ep-C nano composites as well as on graphene/CNT epoxy
nano composite. These models have been tested for higher
aspect ratio’s and predefined weight fraction of graphene epoxy
nano composite and graphene/CNT epoxy nano composite. A sig-
nificant improvement in strengthening efficiency of Gr/Ep-C
nano composite and synergistically combined graphene/CNT
nano composite with different weight fractions in ratio 1:1
was observed with an increase of aspect ratio’s and weight frac-
tions of nano filler. These enhancement in the properties may be
due to the reason that as aspect ratio increases, the tendency of
filler getting embedded in the matrix simultaneously increases,
result of which an overall improvement in strengthening effi-
ciency. Synergistically combined graphene/CNT composite gives
better results in H-T and M-T models then the graphene epoxy
composite for H-T and M-T models.
Please cite this article as: S. Nagar, K. Sharma, N. Kukreja et al., Micromechanical and experimental analysis of mechanical properties of graphene/CNT
epoxy composites, Materials Today: Proceedings, https://doi.org/10.1016/j.matpr.2020.02.407
An improvement of about 2–11% was noticed in longitudinal
modulus of nano composite (graphene epoxy composites) for
same aspect ratio’s, when compared with other research work.
Finally these micromechanical models can be used to predict
the strengthening properties for a variety of nano filler/polymer
composites. The novelty and purpose of this research is to have
materials with high strengthening efficiency which may play a
major roles in structural applications. The materials are both
Graphene/CNT epoxy composites and graphene based epoxy
composite of which graphene/CNT epoxy composite shows better
results.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
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epoxy composites, Materials Today: Proceedings, https://doi.org/10.1016/j.matpr.2020.02.407
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