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Micromechanical analysis of effective mechanical properties of graphene/ZrO 2

-hybrid poly (methyl methacrylate) nanocomposites

Article  in  Journal of Micromanufacturing · August 2021

DOI: 10.1177/25165984211038861

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 Original Research Paper
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ZrO2-hybrid poly (methyl methacrylate) https://doi.org/10.1177/25165984211038861
DOI: 10.1177/25165984211038861
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nanocomposites

Ankit Rathi1 and S. I. Kundalwal1

Abstract
In this study, the tensile properties of two-phase and three-phase graphene/ZrO2-hybrid poly (methyl methacrylate) (PMMA)
AQ: 1 nanocomposites are investigated by developing finite element model using ANSYS. Primarily, the effective elastic properties
of two- and three-phase graphene/ZrO2-hybrid PMMA nanocomposites (GRPCs) are estimated by developing mechanics
of material (MOM) model. Results indicated that the effective elastic properties of GRPCs increase with an increase in the
volume fraction of graphene. Also, the stiffness of GRPCs is increased by 78.12% with increasing in the volume fraction
of graphene from 0.1 to 0.5 Vf. The incorporation of an additional ZrO2 interphase significantly improved the mechanical
performance of resulting GRPCs.

Keywords
Effective elastic properties, GRPC, PMMA, graphene, micromechanics model

1. Introduction dispersed exfoliated graphite nano-platelets in polypropylene

Polymer nanocomposites act as an outstanding structural
material, having lightweight and exceptional mechanical,
thermal and optical properties. Therefore, these
nanocomposites are widely used in various applications such
as automobile, coating and paint industries, medical
equipment, aircraft and aerospace industry.1–5 The exceptional
properties of polymer nanocomposites primarily depend on
the type of nanofiller used and their dispersion with the
polymer matrix. Several nanofillers are available such as
nano-fibre, nano-clay and nanoparticles that can be easily
mixed with the polymer matrix in achieving desired properties.
Graphene is one of the most promising two-dimensional
nanofiller since its discovery by Geim and Novoselov in
2004.6,7 The high mechanical strength and high specific
surface area (SSA) of graphene make it an appealing option
for developing high-performance polymer nanocomposites.
In fact, single layer of graphene with tensile strength of
130 GPa and Young’s modulus of 1000 GPa, is the strongest
material discovered till date.8 However, the homogeneous
dispersion and strong interfacial bonding of graphene with
the polymer matrix are the key challenges in fabricating
desired nanocomposites.9 Several research studies have been
previously carried out based on the extraordinary thermo-
mechanical and electrical properties of graphene-reinforced
polymer nanocomposite. For example, Kalaitzidou et al.10
matrix by using melt-mixing and injection moulding process
and found that a low-volume fraction of graphene enhanced
the elastic modulus, flexural and impact strength of
nanocomposites. Stankovich et al.11 have reported graphene-
based polystyrene composites, which exhibited a percolation
threshold of ∼0.1  volume percent for room-temperature
electrical conductivity. Tripathi et al.12 used different
technique for preparation of reduced graphene oxide–poly
(methyl methacrylate) (PMMA) nanocomposites. Results
show that the conductivity depends on the amount of graphene
oxide and method of preparation of polymer nanocomposite.
Bacali et al.13 studied the morphological and mechanical
performance of graphene-reinforced PMMA composites for
clinical applications. Lin et al.14 used dissipative particle
dynamics (DPD) method and continuum mechanics–based
finite element (FE) method to study the mechanical properties
of graphene-reinforced PMMA nanocomposites.
1 Applied and Theoretical Mechanics (ATOM) Laboratory, Department
of Mechanical Engineering, Indian Institute of Technology Indore, Simrol,
Indore, Madhya Pradesh, India
Corresponding author:
Department of Mechanical Engineering, Indian Institute of Technology
Indore, Simrol, Indore, Madhya Pradesh 453552, India.
Email: kundalwal@iiti.ac.in
2 Journal of Micromanufacturing

In the past decades, various micromechanical models have system (1–2–3), the graphene is dispersed in PMMA matrix
been developed to study the effective mechanical properties along the third direction. The RVE of GRPC is presented in
of composite materials. For example, Thostenson et al.15 Figure 1, where graphene acts as a solid fibre, and PMMA
studied the elastic properties, microstructural and geometric acts as a matrix.
parameters by using Halpin–Tsai theory. Song and Youn16
predict the effective elastic properties of the composite by
using asymptotic expansion homogenization method. Ying ji 2.2 Two-phase mechanics of material approach
et al.17 studied the micromechanical analysis of graphene- The stress and strain relationship of individual phases of
reinforced polymer nanocomposites by using micromechanical proposed GRPC can be written as follows:
MT method. Giannopoulos and Kallivokas18 predict the
effective elastic properties of graphene-based composite by   r
61
 C r 
6 6
 
r
61
(1)
using multi-scale FE approach. Selmi et al.19 studied several
micromechanical models for the estimation of effective where, r = g, p and nc
elastic properties of single-walled carbon nanotube– where σr denotes the stresses, ∈r denotes the strains and Cr
reinforced composites. Kundalwal and Ray20 developed the denotes elastic constant of a matrix. The superscript r used for
mechanics of materials (MOM) approach to estimate the g, p and nc represents graphene, PMMA matrix and GRPC
effective elastic properties of fuzzy fibre reinforced nanocomposite, respectively.
composite. By using iso-field condition and ROM, the equation can
Among all the models developed, the MOM approach is be written as:
found to be the most accurate, efficient, reliable and time-
saving technique in determining the overall mechanical        
g
3
p
3
nc
3
(2)
performance of complex and heterogeneous composite by
v    v     
g p nc
(3)
considering small representative volume element (RVE) of g 3 p 3 3

the bulk composite material.21 It is a well-known fact that the In Equation (3), vg and vp represent the volume fraction of
fibre properties play a dominant role in estimating the axial graphene and PMMA matrix, respectively. By correlating
properties of composites. Therefore, the objective of this Equations (1)–(3), the stress and strain can be written as
study is to estimate the effective elastic and mechanical follows:
properties of graphene/ZrO2-hybrid PMMA nanocomposites
(GRPC), using MOM and FE modelling (FEM) approach,   nc
61
 V1 66  g 
61
 V2 66  p 
61
(4)
respectively. The insignificant role of ZrO2 nanoparticles on
effective mechanical properties is briefly described. The    C     C   
nc
1
g
2
p
(5)
FEM-based numerical analysis is conceded, using commercial
From Equation (2), we can write as
software ANSYS-15.0, to estimate tensile properties of
resulting nanocomposites, while the analytical calculation is C3   g   C4   p   0 (6)
carried out using the MOM model to predict effective elastic
V3   V1   V2 C4  C3 
1
properties. (7)

V4   V2   V1 C3  C4 

1
(8)
2. Modelling
C nc   C1 V3   C2 V4 
1 1
(9)
2.1 Effective elastic properties of graphene/ZrO2-
hybrid poly (methyl methacrylate) nanocomposites Here, matrix from [C1] – [C4] and [V1]– [V4] are obtained by
using some assumptions and curtailments.21 The matrix [Cnc]
The MOM approach was primarily developed by Kundalwal
and Ray20 in 2011 and was, modified to estimate the effective
elastic properties of transversely isotropic composite material.
Certain assumptions have been made while developing two-
phase MOM model of GRPC, such as (a) the resultant
composite should be transversally isotropic; (b) graphene is
uniformly dispersed in PMMA matrix; (c) there is a perfect
bonding between graphene fibre and PMMA matrix, which
means the resulting composite is free of voids and has a
strong interfacial bonding interaction between the filler and Figure 1. Representation of cross-section of RVE of two-phase AQ: 2
GRPC.
the matrix and (d) The iso-field condition and rules of mixture
(ROM) should be followed. In the principal coordinate Source: AQ: 3
Rathi and Kundalwal 3

in Equation (9) gives the effective elastic properties of the

resulting GRPC.
C5   i   C6   p   0 (16)
Finally, the effective elastic coefficient of GRPC can be
obtained as follows:
2.3 Three-phase mechanics of material approach
[C ]  C1 V5   C7 V6 
1 1
(17)
Three-phase MOM model was developed to recognize the
significance of an additional interphase on effective elastic where
properties of GRPC. Each constituent must be fully utilized
C7   C3   C2 C5  C6  ,
1
to obtain optimum mechanical performance of GRPC. It is
possible only when there is a certain interaction between
V4   V3   V2 C5  C6  ,
1
graphene fibre and PMMA matrix.
V5   V1   V4 C6  C4  ,
1
In this work, ZrO2 nanoparticles are introduced as an
interphase between the graphene fibre and PMMA matrix to
V6   V4   V1 C4  C6 
1
study the effect of interphase on effective elastic properties.
From Figure 2, based on the principal coordinate axis (1–2–
Here, matrix from [C1] – [C4] and [V1]– [V4] are obtained by
3), the constitutive relations for the constituent phases of
using some assumptions and curtailments.
three-phase GRPC are written as follows:
 r
61
 C r 
6 6
 
r
61
(10)
2.4 Tensile test
where, r = g, p, i and nc
The obtained effective elastic properties of two- and three-
In Equation (10), g, p, i and nc denote graphene fibre,
phase GRPCs, using MOM modelling approach, are used to
PMMA matrix, ZrO2 interphase and GRPC nanocomposite,
drive the tensile test simulation by using ANSYS 15.0. The
respectively. To satisfy the perfect bonding condition between
dimensions of the tensile test specimen are presented in
graphene and the neighbouring phases, iso-stress and iso-
Figure 3, which follow ASTM D 638-14 standard.22
strain conditions, and rule of mixture can be expressed as
The tensile test specimen with required dimension is
follows:
created by using a three-dimensional (3-D) computer-aided
          
g
3
p
3
i
3
nc
3 (11) design (CAD) modelling software. The effective elastic
properties of GRPC with varying fibre volume fraction are
 33   vg  33g   vi  33i   vp  33p  (12) introduced in ANSYS 15.0 software. The previously created
tensile test specimen by CAD software is then imported into
In Equation (12), vp, vg and vi represent the volume fraction of ANSYS workbench by using an ‘import geometry option’.
PMMA matrix, graphene fibre and ZrO2 interphase,
respectively, present in the RVE. Substituting Equation (10)
into Equations (11) and (12), the corresponding stress and
strain vectors of GRPC can be written as follows:

{ }  C1   g   C2   i   C3   p  (13)

{ }   V1   g    V2   i    V3   p  (14)
Figure 3. Dimension of tensile test specimen.
C4   g   C5   i   0 (15)
Source:

Figure 2. Representation of cross-section of RVE of three-phase

GRPC. Figure 4. Loading conditions in tensile test specimen.
Source: Source:
4 Journal of Micromanufacturing

The specimen is meshed to a fine shell, and appropriate

boundary conditions are applied as shown in Figure 4. The
one end of the specimen is fixed, and load is applied to the
moving end in positive x-direction. The obtained deformation
curve varies with change in applied load. A similar process is
followed with varying volume fraction ranges from 0.1 to 0.5.
Finally, the load versus extension curves are plotted for
different volume fractions of GRPC.

3. Results and discussion

In this section, the predicted value of effective elastic
properties of two- and three-phase GRPCs are evaluated by
using the MOM approach. The effect of ZrO2 interphase on
effective elastic properties is demonstrated. Further, these Figure 5. Variation of C11 of the GRPC with varying fibre volume
effective elastic properties are used for numerical simulation, fraction (Vg).
to carry out the tensile test, using ANSYS software. Source:

3.1 Effective elastic properties of graphene/ZrO2-

hybrid poly (methyl methacrylate) nanocomposites
The mechanical properties such as elastic modulus ‘E’ and
Poisson’s ratio ‘ν’ of graphene fibre, ZrO2 nanoparticles and
PMMA matrix were taken from literature, as summarized in
Table 1. These mechanical properties are used to obtain the
effective elastic properties of GRPCs.
The variation of effective elastic coefficient C11 of GRPC
with respect to the graphene volume fraction (Vg) is presented
in Figure 5. It is observed that the effect of ZrO2 interphase on
the effective elastic properties is increased with an increase in
the value of Vf over the entire range. The presence of ZrO2
interphase not only improved the interfacial bonding between
the graphene fibre and the PMMA matrix but also showed Figure 6. Variation of C12 of the GRPC with Varying Fibre
individual effect in improving the value of effective elastic Volume Fraction (Vg).
coefficient C11 of three-phase GRPC.26–28
Source:
Similar results have been obtained for the effective elastic
coefficient C12 of GRPC with respect to the graphene volume
fraction (Vg), presented in Figure 6. The variation of effective of two- and three-phase GRPCs with respect to graphene
elastic coefficients C23 of transversely isotropic two- and volume fraction (Vg) are mainly due to the iso-stress condition.
three-phase GRPC with respect to the graphene volume In Figure 8, the effective elastic coefficients C33 gives the
fraction (Vg) are presented in Figure 7. Results indicate that straight-line linear curves for two- and three-phase GRPC
the value of C23 for two- and three-phase GRPCs is increased with respect to graphene volume fraction (Vg). This is mainly
with varying graphene volume fraction (Vg) by presenting the due to the iso-strain condition, which means the direction of
interfacial effect of ZrO2 nanoparticles. The non-linear curves graphene fibre is the same as that of PMMA matrix as well as
GRPC. When the load is applied, the graphene, which is
Table 1. Elastic properties of the constituent phases of GRPC. being aligned along the third direction, enhances the axial
Elastic modu- Poisson’s stiffness of the GRPC in the same direction. Hence, we
lus (GPa) ratio References obtained the linear straight-line curve along the third direction.
It is worth to note that the slope is also increased with the
Graphene 985 0.26 Kundalwal et al.23
addition of ZrO2 nanoparticles. This indicates that the addition
ZrO2 interphase 200 0.28 Cousland et al.24
of ZrO2 interphase also improves the stiffness of a material.
PMMA matrix 2.963 0.38 Ayatollahi and Figure 9 presents the effective elastic coefficient C44 of
Torabi25 GRPC with respect to graphene volume fraction (Vg). Results
Source: reveal that the incorporation of an additional ZrO2 interphase
Rathi and Kundalwal 5
Figure 7. Variation of C23 of the GRPC with varying fibre volume
fraction (Vg).
Source:
Figure 8. Variation of C33 of the GRPC with varying fibre volume
fraction (Vg).
Source:
enhances the effective elastic properties of GRPC. In the
author’s previous study, the author used a similar modelling
approach by considering 1-D MWCNT as a fibre, ZrO2
nanoparticles as an interphase and epoxy as a matrix and
found a similar trend in the result of effective elastic properties
of resulting nanocomposites.26 It is noteworthy that the two-
and three-phase MOM models evaluate the effective elastic
properties by assuming a perfect bonding condition and ROM
between PMMA matrix and graphene fibre, with and without
considering the effect of ZrO2 interphase.
3.2 Tensile test
In this section, the specimen’s geometry along the loading
and boundary condition was chosen by following ASTM D
638-14 standard. The effective elastic constants obtained by
developing the two- and three-phase MOM models of GRPC
Figure 9. Variation of C44 of the GRPC with varying fibre volume
fraction (Vg).
Source:
Figure 10. Load versus extension curve of the GRPC with
varying graphene volume fraction (Vg).
Source:
were used to perform tensile test FE simulations. The
estimated tensile test results for two-phase GRPC are
presented in Figure 10.
The load versus extension curves of two-phase GRPC
indicates the deflection with respect to the graphene volume
fraction (Vf) of a tensile test specimen. When we applied
the load of 2000 N to the specimens, the deflection curve
decreased from 1.71 mm to 0.96 mm and the slope increased
with an increase in the graphene volume fraction (Vf) from
0.1 to 0.5, respectively. Also, the stiffness of GRPCs is
increased by 78.125%, with an increase in the volume
fraction of graphene from 0.1 to 0.5 Vf. The primary reason
behind this is that at higher volume fraction of graphene,
the polymer chain cross-linked density increases, which
increases the stiffness of a composite material and decreases
the extension curves. Therefore, the strength and stiffness
of GRPC increases with an increase in graphene fibre
volume fraction.
6 Journal of Micromanufacturing
Figure 11. Load versus extension for a two- and three-phase
GRPCs of volume fraction (Vf = 0.1).
Source:
Similarly, to examine the interfacial effect of ZrO2
nanoparticles on tensile properties, we further performed the
tensile test on three-phase GRPC specimens. The load versus
extension curve for two- and three-phase GRPC at 0.1 Vf of
graphene is presented in Figure 11. When the same loading
condition is applied to three-phase GRPC, the deflection
curve decreases from 1.71 to 1.61 and the stiffness increases
by 6.21%, respectively as compared to two-phase GRPC.
This shows that the addition of ZrO2 interphase enhances the
interfacial bonding between the fibre and the PMMA matrix.
However, it is important to note that the presence of ZrO2
interphase not only improves the interfacial bonding between
the graphene fibre and the PMMA matrix but also shows
individual effect in improving the tensile properties of the
resulting GRPC.26,27 Therefore, the incorporation of additional
interphase also gives the positive effect on the tensile
properties of polymer nanocomposites.
4. Conclusion
In this study, the MOM approach was used to estimate the
effective elastic properties of two- and three-phase GRPCs.
The estimated effective elastic properties of GRPC increased
with an increase in the volume fraction of graphene. Also, the
addition of ZrO2 interphase between the graphene fibre and
PMMA matrix significantly enhanced the effective elastic
properties of three-phase GRPCs. Further, these effective
elastic properties were used to perform the tensile test. Results
revealed that the stiffness of the two-phase GRPCs was
increased by 78.125% with an increase in the volume fraction
of graphene from 0.1 to 0.5 Vf. Also, the introduction of ZrO2
interphase in the three-phase GRPC improved the stiffness by
6.21%, respectively, as compared to the two-phase GRPC at
0.1 Vf. The fibre properties played a dominant role in the case
of the prediction of the axial properties of composites.
Therefore, the effect of ZrO2 interphase in GRPC was found
to be insignificant.
Declaration of conflicting interests
The authors declared no potential conflicts of interest with respect to
the research, authorship and/or publication of this article.
Funding
The authors received no financial support for the research, authorship
and/or publication of this article.
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