Materials Chemistry and Physics 309 (2023) 128324

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Materials Chemistry and Physics

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

Predicting the electrical conductivity of short carbon fiber/graphene

nanoplatelet/polymer composites
Maedeh Saberi a, Reza Ansari a, **, Mohammad Kazem Hassanzadeh-Aghdam b, *
a
Faculty of Mechanical Engineering, University of Guilan, Rasht, Iran
b
Department of Engineering Science, Faculty of Technology and Engineering, East of Guilan, University of Guilan, Rudsar-Vajargah, Iran

H I G H L I G H T S

• Electrical conductivity of SCF/GNP-filled polymer composites is modeled.

• More enhancement in conductance is found by incorporation of GNPs.
• Effect of percentage and size of reinforcements and interphase is examined.

A R T I C L E I N F O A B S T R A C T

Keywords: The current work examines the effect of graphene nanoplatelet (GNP) additives upon the electrical conductivity
Multifunctional composite of short carbon fiber (SCF)-reinforced polymer multifunctional composites. GNPs and SCFs are randomly
Short carbon fiber dispersed into the representative volume element of the composite. A multi-step physics-based approach is
Graphene nanoplatelet
developed to determine the effective electrical conductivity of SCF/GNP/polymer composites. Outcomes of the
Electrical conductivity
Physics-based method
current work are compared with the available experimental data and other numerical results to verify its ac­
curacy. Changes in the volume fraction and geometry of multi-scale reinforcements, interphase characteristics,
barrier height, nanofiller tunneling distance and fiber material property are considered to reflect the influence of
microstructures on the electrical conducing behavior of SCF/GNP/polymer multifunctional composites. It is
found that the electrical conductivity of the multifunctional composite enhances by the increase of volume
fraction and aspect ratio of GNP as well as the reduction of its thickness. Moreover, the multifunctional com­
posite shows a higher electrical conductivity with the increase of fiber aspect ratio. The electrical conductivity of
the SCF/GNP-reinforced composite depends on the interphase such that its value increases by the increase of
interphase thickness. The developed method can be adopted to provide useful guidelines for the design and
optimization of multifunctional composites filled by hybrid reinforcements.

1. Introduction applications and sensors. There is an excessive number of papers that

Nowadays great attention is paid to the study of GNPs application for
improving the mechanical and physical properties of the polymer
composite due to their high stiffness and strength, remarkable thermal
and electrical properties and high aspect ratio [1–6]. Also, graphene has
a wide range of application in industry, such as its use as a material for
manufacturing sensors [7–9]. According to Meng et al. [10], GNPs’
intrinsic conductivity is dependent on their physical characteristics,
particularly their thickness.
Composites with good electrical conductivity are used in aerospace
discuss the utilization of GNPs in polymer matrixes [11]. The compos­
ites’ conductivity varies depending on the type of polymer matrix and
the graphene filler, the manufacturing process, and the post-production
treatments. Most industrial applications use polymer materials as ma­
trixes because of their lightweight and corrosion resistance. However,
their wide usage is limited by their poor electrical conductivity due to
the fact that most polymers act as insulation. Conductive nanoparticles
can be added into the polymer materials to enhance their electrical
conductivity. For example, carbon nanotubes (CNTs)/polymer nano­
composites find extensive use across various industries [12,13].

* Corresponding author.
** Corresponding author.
E-mail addresses: r_ansari@guilan.ac.ir (R. Ansari), mk_hassanzadehaghdam@guilan.ac.ir (M.K. Hassanzadeh-Aghdam).

https://doi.org/10.1016/j.matchemphys.2023.128324
Received 23 May 2023; Received in revised form 14 August 2023; Accepted 17 August 2023
Available online 18 August 2023
0254-0584/© 2023 Elsevier B.V. All rights reserved.
M. Saberi et al.
Although, GNPs are often less expensive than other types of CNTs
[14–16]. Various phenomena, such as easier aggregate formation of
graphene, crimping and wrinkling, may increase the percolation
threshold of graphene-filled nanocomposites [15]. Experimentation is
the most accurate technique to evaluate the electrical conductivity of
composites, but due to issues such as production difficulty and high cost,
it cannot be widely used. To estimate the electrical conductivity of
polymer matrix composites, a variety of techniques, including numerical
simulations and micromechanical approaches, have recently been used.
Several studies on the electrical conductivity of GNP-polymer com­
posites have been appeared in the literature [16]. Experimentally, it was
found that many parameters affect the effective electrical conductivity
of composites, such as nanoparticles’ size, volume fraction and electrical
resistivity or interphase thickness. The system’s interphase section is
produced by the large area of interfacial gap between the nanoparticle
and the matrix in the composites. The percolation threshold, the point at
which the conductive network begins to form, is mostly impacted by the
interphase because the filler network’s size can be increased by the
interphase thickness [17]. The effective electrical conductivity of poly­
mers can be significantly increased by adding a small amount of GNP
[18,19]. When the GNP volume fraction rises above the percolation
threshold, continuous electron paths start to be formed. However, the
extent of improvement also depends on GNP’s dispersion in the polymer
matrix [20]. There is lower possibility to form connective paths when
nanoparticles are perfectly aligned. So, the primary variable that im­
pacts the percolation threshold is the GNP dispersion in the matrix.
Cobos et al. [21] showed that the hydrogen bonds and electrostatic in­
teractions between the nanoparticles and the chitosan help to randomly
distribute graphene oxide within the chitosan matrix. Chitosan’s ther­
mal stability, stiffness, and tensile strength were all enhanced by gra­
phene oxide.
Kim et al. [22] investigated the impact of several processing tech­
niques on the conductivity of polyurethane/graphene nanocomposites.
It was observed that composites made by solution mixing had the
highest conductivity values. It should be noted that post-processing
techniques like hot pressing or injection molding can also influence
the distribution of the nanoparticles and the effective conductivity of the
composite for production methods [23,24].
Hybrid composites contain two or more types of particles in a com­
mon matrix. The electrical conductivity of the hybrid composites can be
greatly enhanced due to the fact that shorter particles provide electron
paths between the longer particles [25]. The investigations on the short
carbon fiber (SCF)-polymer composites showed that the electrical con­
ductivity of the composite improved with increasing the volume fraction
of SCF, although after the percolation threshold it reaches a maximum
limit [26]. But by adding GNPs, which offers a different scale of elec­
trical channels in the composites, this electrical conductivity limit of
SCF-polymer materials can be pushed much further.
Many models have been developed to predict the effective properties
of nanoparticle-filled composites. Several studies used a simple power-
law percolation theory [27]. They only worked with estimates of
exponent and percolation inception in nanocomposite, while compared
to microparticles, nanoscale particles such as GNPs have different im­
pacts on conductivity. Nazarov et al. [28] studied the effective medium
theory for multi-particle composites. They used an iterative model to
compute the effective properties of materials with more than one par­
ticle and suggested that for N-particle composites, the iterative method
is more accurate than the synergic model. Some studies were carried out
to suggest models that consider the interphase effect for predicting both
electrical and thermal conductivity of CNT-filled composites [29,30].
Haghgoo et al. [31] studied a model framework based on the assumption
of randomly oriented, aligned, and agglomerated CNT dispersion that
can predict the effective electrical conductivity of a carbon fiber
(CF)-CNT reinforced polymer hybrid composite. Payandepeyman et al.
[32] suggested a model for predicting the electrical conductivity of
GNP-polymer composites. They studied the impact of GNP aspect ratio
2
Materials Chemistry and Physics 309 (2023) 128324
and thickness. In contrast, the electrical conductivity of GNP-SCF
polymer composites has not been studied comprehensively, according
to the best knowledge of the authors.
The aim of the present work is to develop a physics-based model
capable of predicting the effective electrical conductivity of a
GNP–SCF–polymer multifunctional composite. Since these two sets of
inhomogeneities have widely different spatial scales and electrical
conductivities, the solution is divided into several stages. To provide the
matrix conductivity, the effective GNPs are dispersed randomly in the
non-conductive polymer in the first stage. In the second stage, the SCFs
are distributed in the conductive matrix to create new paths for elec­
trons. The developed analytical models were validated by comparing the
prediction results with experimental data and other numerical results. In
this paper, the effect of GNP and SCF content and geometry, electrical
conductivity of SCFs, barrier height, tunneling distance and interphase
thickness is investigated.
2. Modeling the electrical conductivity of the SCF/GNP-
reinforced composites
2.1. Effective electrical conductivity of GNP/polymer composites
Fig. 1 shows a schematic representation of the modeling procedure of
electrical conductivity for the GNP/SCF/polymer multifunctional com­
posite. Consider a random distribution of GNP surrounded by a thin
layer of interphase in a representative volume element (RVE) of the
polymer composite system, as shown in Fig. 2(a).
There are two coordinate systems: a local coordinate system (x, y, z)
based on GNP in which the z axis is the thickness of nanoparticle and a
global coordinate system (X, Y, Z) based on polymer composite. Fig. 2(b)
represents the schematic of the effective GNP. To take the effect of
interphase into account, the effective electrical conductivity of nano­
particle is calculated in two steps in each direction. According to Fig. 2
(c) and (d), the nanoparticle can be divided into three parts: parts 1 and
3 are interphase cuboids; part 2 is a mixture of interphase and GNP. Due
to the symmetric geometry of the nanoparticle, the electrical conduc­
tivity (σ ) of the effective GNP becomes transversely isotropic, so the
electrical conductivity in the x and y directions (σx = σy ) can be
considered to be equal.
The electrical resistance can be expressed as follows [26,32].
Li
Ri = (1)
σ i Ai
where Ai and Li are the cross-section area and length of corresponding
part, respectively. Hence, the electrical resistance of parts 1 and 3 in x
directions is given by
R3x = R1x =
t
(2)
σ int (L + 2t)(d + 2t)
where σint is the electrical conductivity of the interphase, t is the
thickness of interphase layer, d and L are thickness and height of GNP,
respectively. R3x denotes the electrical resistance of part 3 in x direction.
For part 2, the electrical resistance of interphase and GNP is calculated
by Eqs. (3) and (4), respectively
L
R2x− = (3)
int
σint ((L + 2t)(d + 2t) − dL)
R2x− =
L
(4)
GNP
σ GNP dL
where σGNP is the electrical conductivity of GNP. Considering Fig. 3, the
law of mixture can be used to calculate the electrical resistivity of
nanoparticle along x direction.
The electrical resistance of the intermediate particle (Rmx ) can be
calculated by parallel combination of part 2 resistances as expressed
M. Saberi et al. Materials Chemistry and Physics 309 (2023) 128324

Fig. 1. Schematic representation of analytical modeling of GNP–SCF–polymer composite electrical conductivity: a) GNP + interphase around it; b) effective
nanoparticle; c) random distribution of effective nanoparticles into non-conductive polymer matrix; d) random distribution of SCF into conductive matrix.

Fig. 2. (a) RVE with random distribution of GNPs, (b) view of rectangular cuboid of GNP, (c) side view of effective GNP, (d) front view of effective GNP.

3
M. Saberi et al. Materials Chemistry and Physics 309 (2023) 128324

L2 d
α= (12)
Ar2 (d + 2t)3

where Ar is the aspect ratio of the effective GNP nanoparticle, i.e., Ar =

Fig. 3. Law of mixture for effective particle in the x direction.
(L + 2t) /(d + 2t). To determine the electrical conductivity of GNP/
polymer composites, a RVE with randomly oriented nanoparticles was
chosen. The uniform dispersion of GNPs in the polymer converts it to an
isotropic conductive composite. The GNP/polymer composite is sub­
jected to a uniform electrical field E. Let the electrical field E be defined
by [29]

( ) E = − ∇∅ (13)
1 1 1
= + (5)
Rmx R2x− int R2x− GNP where ∅ is the electrical potential. Correspondingly, the current flux j
that obeys Ohm law can be determined as follows
So, the equivalent resistence in the x direction is
j = σE (14)
Rx = R1x + Rmx + R3x (6)
Using Eqs. (2) and (5) and taking σx = (L + 2t) /(Rx (L + 2t)(d + 2t)), According to the average polarization theory, the effective electrical
the effective electrical conductivity in the x direction is derived as [32] conductivity of GNP/polymer σ GNP
e is defined by

σ int (L + 2t)[σGNP Ld + σ int ((d + 2t)(L + 2t) − Ld)] < j >= σGNP <E> (15)
σx = (7) e
2t(σ GNP Ld + σ int ((d + 2t)(L + 2t) − Ld)) ∫ ∫
where < j >= 1v V jdv and < E >= 1v V Edv denotes the average of the
The effective electrical conductivity of nanoparticle in the z direction
current flux and electrical field, respectively. The average internal
is calculated as
electrical field in GNP and matrix particles is expressed as [30]
[ ]
(d + 2t)σint σGNP L2 + σint (4Lt + 4t2 ) ∑
σz = (8) < Ein,m > = (
1
)/ E < Ein,GNP >
2tσ GNP L2 + 2tσ int (4Lt + 4t2 ) + σ int d(L + 2t)2
+ Bm,k σm,k − σ GNP
k=x,y,z1 e,k σGNP
e,k
From Eqs. (7) and (8), it is clearly indicated that the thickness and ∑ (16)
1
conductivity of the interphase play an important role in the effective = (
GNP
)/ E
k=x,y,z1 + BGNP,k σ GNP,k − σ e,k σGNP
conductivity of nanoparticle. The electrical conductivity of the inter­ e,k

phase surrounding the GNP can be expressed as [33].

where BGNP,k and Bm,k are the demagnetization factor of the effective
σ int =
dc
(9) GNP and matrix particles, respectively, which depend on M factor
Ac Rint (dc ) (M = 1 /Ar) and shapes of effective GNP and matrix particles along the k
axis [37]. The average current flux in the GNP and matrix particles is
where dc and Ac are the tunneling distance and over lapping contact expressed as
area, respectively. For evaluating the interphase resistance, an
assumption for dc was made based on this quantity [33]. The tunneling < jin,m >= σ m < Ein,m > < jin,GNP >= σGNP < Ein,GNP > (17)
distance is determined as
Substituting Eqs. (16) and (17) into Eq. (15), we have
dc = 2t (10) ∑( )
VGNP σGNP
e,k − σ m,k
1− ( )
By using Simmon’s model [34], the tunneling resistance between α σ GNP GNP
k=x,y,z + B m,k σ m,k − σ e,k
two nanoparticles can be expressed as
e,k
(18)
( ) ∑ VGNP σ GNP
e,k − σ GNP,k
+ ( )=0
dc h2 4πdc (2mλ)1/2 α σGNP + BGNP,k σGNP,k − σGNP
Rint (dc ) = exp (11) k=x,y,z e,k e,k
Ac e2 (2mλ)1/2 h
where VGNP is the volume fraction of effective GNP. The matrix particles’
where h is Planck constant (6.626068 × 10− 34 m2 kg/s), e is the electric dimensions are much smaller than the GNP’s. Due to the simplicity, all
charge of an electron (− 1.602176565 × 10− 19 C), m is the mass of an the matrix particles can be considered as balls and GNP’s particles can be
electron (9.10938291 × 10− 31 kg) and λ is the work function or potential regarded as square prism. The value of Bm and BGNP in different di­
barrier height of the polymer matrix. The probability that an electron rections are determined as follows
may pass through and override the potential barrier between two /
nanoparticles has an impact on the conductivity between them [35]. The Bm,x = Bm,y = Bm,z = 1 3 (19)
effect of potential barrier height is discussed below. From Eq. (11), the
overlapping contact area was found to have no effect in electrical 1 − BGNP,z
BGNP,x = BGNP,y = (20)
resistance [36]. As we consider an interphase layer around the GNP, the 2
ratio of the GNPs’ volume to the volume of effective particle is defined The electrical conductivity of a nanoparticle/polymer composite can
by be obtained from the following equation

( ) GNP [ ]
VGNP σ e − σm VGNP σ GNP − σz σGNP − σx
3 1− + e ( )+4 ( e )( ) =0 (21)
α 2σ GNP
e + σm 3α σGNP
e + BGNP,z σ z − σ GNP
e 2σGNP
e + 1 − BGNP,z σ x − σ GNP
e

4
M. Saberi et al. Materials Chemistry and Physics 309 (2023) 128324

2.2. Effective electrical conductivity of SCF/GNP polymer composites
Dispersion of GNPs into the non-conductivity polymer, converts it
into a conductive matrix, which in turn increases the maximum limit of
electrical property for random SCF composite. The electrical conduc­
tivity of the conductive matrix was estimated using Eq. (21). In this
section, an analytical model is presented to predict the electrical con­
ductivity of the GNP–SCF–polymer composite. Consider a random dis­
tribution of SCFs into the conductive matrix. After the SCF volume
fraction exceeds a particular threshold, literature has demonstrated that
SCF composites have a significant increase in the electrical conductivity.
The percolation threshold, Vc , for a two-phase composite with a random
distribution of SCFs, can be calculated by the following equation [38]
9H(1 − H)
Vc (H) =
2 + 15H − 9H 2
here H is obtained as follows
[ ]
1 A ( √̅̅̅̅̅̅̅̅̅̅̅̅̅̅ )
H(A) = 2 √̅̅̅̅̅̅̅̅̅̅̅̅̅̅ ln A + A2 − 1 − 1
A − 1 A2 − 1
where A is the aspect ratio of SCF, i.e., A = l/D. l and D are the length
and diameter of SCF, respectively. The percolation threshold is the
critical SCF volume fraction at which electrical conductivity increases
rapidly.
The electrical conductivity of a microfiber-filled composite can be
determined as [36].
⎡ ⎤
σc VSCF ⎢ σSCF 1 ⎥
=1 + ⎣ξ + (1 − ξ) σm.con ⎦ (24)
σ m.con 3 σ m.con σSCF + H
where σm.con is the conductive matrix electrical conductivity that was
calculated in stage 1. σ SCF and VSCF are the electrical conductivity and
volume fraction of SCF, respectively. ξ is the percentage of percolated
SCFs and can be approximately estimated as [39]
1/3
VSCF − Vc1/3
ξ=
1 − Vc1/3
From Eq. (22), it should be noted that VSCF increases from Vc to 1 and ξ
varies from 0 to 1.
3. Results and discussion
To validate the proposed model developed in the current paper, the
present modeling results are compared with the experimental mea­
surements and other numerical results from the literature [26,40–42].
All parameters used in the analysis, such as filler length, diameter,
interphase thickness and electrical conductivity are listed in Table 1 [26,
40–42]. It should be noted that for the analytical models in stages 1 and
2, GNTs and SCFs were assumed to be uniformly dispersed in a matrix.
As shown in Fig. 4(a), the present analytical results are in good
agreement with the experimental data given by Zhang et al. [40] for a
polyethylene terephthalate (PET)/graphene composite. The second data
set for validation is related to the work of Stankovich et al. [41] for a
polystyrene (PS)/graphene composite. Fig. 4(b) demonstrates that the
calculated curve can reflect the experimental result properly. To further
verify the present model, the electrical conductivity of the polyurethane
(PU)/graphene composite was estimated and compared with experi­
mental data [42]. The model results shown in Fig. 4(c) suitably agree
with the experimental data reported by Yousefi et al. [42]. However,
there are some differences between analytical modeling results and the
experimental data in fact are related to the high sensitivity of electrical
conductivity to the tunneling distance and size of GNP which is a sig­
nificant challenge for accurate measurement using experimental tools.
Fig. 4(d) shows the comparison between the present predictions and the
numerical results of Pal et al. [26] for a SCF/polymer composite. It is
found that a good agreement exists between the two sets of results.
It was considered that the barrier height between two GNPs is λ ≈
0.17 eV [32]. Fig. 5 shows the effect of barrier height on the electrical
conductivity of the GNP/polymer composite. It is simple to discover that
(22)
for the same GNP volume fraction, the overall electrical conductivity
increases with the decrease in barrier height. The parameters were taken
as σ GNP = 105 mS [33], σ m = 10− 16 mS [34], Ar = 330, d = 1 nm, t = 1 nm.
Fig. 5 demonstrates that the percolation threshold has not changed for
(23)
various values of the height barrier.
Fig. 6 presents the effective electrical conductivity of the GNP/SCF/
polymer multifunctional composites before and after the GNP percola­
tion threshold. The SCF parameters in the calculations are chosen as
σ SCF = 66250 ms [36], D = 5μm, A = 100 as default values. It can be
concluded from Fig. 6(a), before the percolation threshold value, the
electrical conductivity of the SCF/GNP composite is nearly equal to the
one of the matrixes, which is not high enough to create a conductive
network. It can be seen that the SCF volume fraction approaches the
percolation threshold, the conductivity of the composite increases
rapidly. The tunneling effect theory can also be used to explain this
rapidly changing of the electrical conductivity. Once the SCF volume
fraction exceeds the percolation threshold, the GNP’s volume fraction
has approximately no effect on the electrical conductivity. It is easy to
distinguish from Fig. 6(b) that increasing the GNP volume fraction
causes an increase in the electrical conductivity. This is due to the fact
that the increase in the GNP volume fraction makes it easier to form a
conductive network. Also, the distance between two SCFs is too large,
(25) when the SCF volume fraction is low, therefore, the possibility of con­
necting to each other is low and the conductive network paths are un­
able to be constructed. As the SCF volume fraction increases, the
electrical conductivity increases because of the variety of different
conductive paths that can be built. It was discovered that when the GNP
volume fraction is less than the percolation threshold, the intensity in­
crease of effective electrical conductivity is greater.
Fig. 7 shows the variation of electrical conductivity for the GNP/
SCF/polymer multifunctional composite for different values of GNP
sizes. The effect of aspect ratio Ar and thickness d on the effective
electrical conductivity is shown in Fig. 7 (a) and (b), respectively. From
Fig. 7(a) it can be concluded that as the aspect ratio increases, the
electrical conductivity increases. There is a strong connection between
the GNP aspect ratio and the electrical conductivity of hybrid compos­
ites. The smaller proportion of length to thickness makes it harder for
GNPs to connect to each other. Also, the presence of more GNP
conductive paths with larger aspect ratio in the same volume fraction

Table 1
Parameters used in the simulation of electrical conductivity of GNP/polymer and SCF/polymer composites [26,40–42].
(s) (s)
Composition d-l (nm) t (nm) dc (nm) σm σf Aspect ratio Ref.
m m

Graphene/PET 1.57 1.3 2.6 10− 14

105 344 [40]
Graphene/PS 1 1.5 3 10− 16
105 1428 [41]
Graphene/PU 1 1.75 3.5 10− 9 105 1538 [42]
SCF/Polymer 50,000 – – 1 66,250 100 [26]

5
M. Saberi et al.
Fig. 4. Comparison between the present predictions and (a) experimental data
of PET/graphene composite [40], (b) experimental data of PS/graphene com­
posite [41], (c) experimental data of PU/graphene composite [42]and (d)
simulation results of Ref. [26].
6
Materials Chemistry and Physics 309 (2023) 128324
Fig. 5. Electrical conductivity of GNP-filled polymer composite for different
values of barrier height.
Fig. 6. Electrical conductivity of GNP/SCF/polymer composite (a) before GNP
percolation threshold and (b) after GNP percolation threshold.
can explain this occurrence of improved conductivity. Furthermore,
GNP with a high aspect ratio also has longer continuous electron path­
ways. It is clear from Fig. 7(b) that the electrical conductivity of the
GNP/SCF/polymer multifunctional composite can be improved by
decreasing the GNPs’ thickness.
M. Saberi et al. Materials Chemistry and Physics 309 (2023) 128324

Fig. 7. Electrical conductivity of GNP/SCF/polymer composite for different

values of (a) GNP aspect ratio and (b) GNP thickness.

The influence of interphase parameters on the electrical conductivity

was also investigated in Fig. 8. From Fig. 8(a), it can be seen that as the
interphase thickness (t) is increased, the electrical conductivity attains a
higher value. The interphase thickness effects can be explained based on
the fact that the effective volume of nanofiller increased with the in­
crease in interphase thickness. Consequently, there is a greater possi­
bility that GNPs will overlap each other to create a conductive network.
The magnitude of electrical conductivity is greatly affected by the bar­
rier height between two GNPs. It is observed from Fig. 8(b) that as the
barrier height increases, the electrical conductivity decreases. Barrier
height can be explained as the difference in work functions between the
nanoparticle and polymer [43]. Over the percolation threshold value,
the conductivity of composites generally rises as the SCF volume fraction
increases. But it can be seen that, the greater barrier height followed by
much more rapid increase in electrical conductivity. The electrical
conductivity of GNP/SCF/polymer multifunctional composite is greatly Fig. 8. Electrical conductivity of GNP/SCF/polymer composite for different
affected by the tunneling distance between GNPs. Fig. 8(c) shows the values of (a) interphase thickness, (b) barrier height and (c) GNP
variation of GNP/SCF composite electrical conductivity with SCF vol­ tunneling distance.
ume fraction at different tunneling distances. It can be concluded that
the electrical conductivity of composites decreases with an increase in role in electrical conductivity and percolation threshold values.
the tunneling distance. Generally, composites reinforced with a very low Increasing the SCF aspect ratio causes an increase in the probability of
SCF volume fraction are poor conductors and the percolation threshold forming long, continuous electron pathways and it could decrease the
is unaffected by GNP nanofiller. volume fraction of SCF needed to form a conductive network. So, the
To present the influence of SCF parameters, a series of evaluations percolation threshold value of the hybrid composite with a high SCF
using the physics-based model are carried out, as depicted in Fig. 9. As aspect ratio is lower than that of a lower SCF aspect ratio.
can be seen from Fig. 9(a), the SCF aspect ratio (A) plays an important Because of the existence of GNP, electrical conductivity paths can be

7
M. Saberi et al.
Fig. 9. Electrical conductivity of GNP/SCF/polymer composite for different
values of (a) SCF aspect ratio and (b) SCF electrical conductivity.
formed in the case of a low SCF volume fraction. After the percolation
threshold, as the aspect ratio increases more and more, percolation paths
are formed and the increase in electrical conductivity tends to be more
stable. Fig. 9(b) shows the variation of electrical conductivity with the
SCF volume fraction in a GNP/SCF/polymer composite for different
values of SCF electrical conductivity. It is demonstrated that the SCF
electrical conductivity done not affect the GNP/SCF/polymer composite
electrical conductivity before the percolation threshold. After the
percolation threshold, the increase in SCF conductivity increases the
hybrid composite electrical conductivity. This is due to the fact that
stronger conductive paths are formed by the higher electrical
conductivity.
4. Conclusion
In this work, the electrical conductivity of the SCF-reinforced poly­
mer composites containing graphene nanofillers was predicted using a
multi-step physics-based method. Comparison between the model pre­
dictions with available experimental data and other numerical results
revealed a good agreement. The main findings of this paper are sum­
marized below.
• After the percolation threshold, the increase of graphene percentage
causes an enhancement in the composite electrical conductivity.
8
Materials Chemistry and Physics 309 (2023) 128324
• The electrical conductivity of the SCF/polymer multifunctional
composite increases by the increase of GNP aspect ratio and by the
decrease of GNP thickness.
• Increasing the interphase thickness, decreasing both the barrier
height and tunneling distance lead to the improvement in the elec­
trical conductivity of the SCF/GNP/polymer composites.
• The change of SCF aspect ratio significantly affects the percolation
threshold value and electrical conductivity of the graphene-filled
multifunctional composites.
CRediT authorship contribution statement
Maedeh Saberi: Methodology, Software, Formal analysis, Writing –
original draft. Reza Ansari: Validation, Resources, Writing – review &
editing, Supervision, Investigation. Mohammad Kazem Hassanzadeh-
Aghdam: Conceptualization, Data curation, Visualization, Resources.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
Data will be made available on request.
References
[1] C. Lee, X. Wei, J.W. Kysar, J. Hone, Measurement of the elastic properties and
intrinsic strength of monolayer graphene, Science 321 (5887) (2008) 385–388,
https://doi.org/10.1126/science.1157996.
[2] K. Chu, C.C. Jia, W.S. Li, Effective thermal conductivity of graphene-based
composites, Appl. Phys. Lett. 101 (12) (2012) 2012–2015, https://doi.org/
10.1063/1.4754120.
[3] A.A. Basheer, Graphene materials for fabrication of robots, Mater. Chem. Phys. 302
(2023).
[4] H. Wang, M. Narasaki, Z. Zhang, K. Takahashi, J. Chen, Ultra - strong stability of
double - sided fluorinated monolayer graphene and its electrical property
characterization, Sci. Rep. (2020) 1–10, https://doi.org/10.1038/s41598-020-
74618-4.
[5] J. Naseri, K. Ranjbar, M. Reihanian, Optimizing the strength and electrical
conductivity of graphene reinforced Cu–Cr–Zr alloy fabricated by powder
metallurgy and spark plasma sintering, Mater. Chem. Phys. 300 (2023), 127524.
[6] D. Xiang, L. Wang, Y. Tang, C. Zhao, E. Harkin-Jones, Y. Li, Effect of phase
transitions on the electrical properties of polymer/carbon nanotube and polymer/
graphene nanoplatelet composites with different conductive network structures,
Polym. Int. 67 (2) (2018) 227–235.
[7] D. Xiang, et al., Damage self-sensing behavior of carbon nano fi ller reinforced
polymer composites with di ff erent conductive network structures, Polymer 158
(August) (2018) 308–319, https://doi.org/10.1016/j.polymer.2018.11.007.
[8] X. Zhang, et al., High-performance flexible strain sensors based on biaxially
stretched conductive polymer composites with carbon nanotubes immobilized on
reduced graphene oxide, Composer Part A 151 (October) (2021), 106665, https://
doi.org/10.1016/j.compositesa.2021.106665.
[9] X. Zhang, et al., Flexible and high-performance piezoresistive strain sensors based
on carbon nanoparticles@polyurethane sponges, Compos. Sci. Technol. 200
(2020), 108437, https://doi.org/10.1016/j.compscitech.2020.108437.
[10] Q. Meng, et al., Processable 3-nm thick graphene platelets of high electrical
conductivity and their epoxy composites, Nanotechnology 25 (12) (2014), https://
doi.org/10.1088/0957-4484/25/12/125707.
[11] D. Xiang, Z. Zhang, Y. Wu, J. Shen, E. Harkin-jones, Z. Li, 3D-Printed Flexible
Piezoresistive Sensors for Stretching and Out-Of-Plane Forces, vol. 2100437, 2021,
pp. 1–10, https://doi.org/10.1002/mame.202100437.
[12] D. Xiang, et al., Enhanced performance of 3D printed highly elastic strain sensors of
carbon nanotube/thermoplastic polyurethane nanocomposites via non-covalent
interactions, Composer Part B 176 (July) (2019), 107250, https://doi.org/
10.1016/j.compositesb.2019.107250.
[13] D. Xiang, et al., Synergistic effects of hybrid conductive nanofillers on the
performance of 3D printed highly elastic strain sensors, Composer Part A (2019),
105730, https://doi.org/10.1016/j.compositesa.2019.105730.
[14] N.A. Kotov, Carbon sheet solutions, Nature 442 (7100) (2006) 254–255.
[15] J. Du, L. Zhao, Comparison of electrical properties between multi-walled carbon
nanotube and graphene nanosheet/high density polyethylene composites with a
segregated network structure, Carbon N. Y. 49 (4) (2010) 1094–1100, https://doi.
org/10.1016/j.carbon.2010.11.013.
M. Saberi et al.
[16] J. Liang, et al., Electromagnetic interference shielding of graphene/epoxy
composites, Carbon N. Y. 47 (3) (2009) 922–925, https://doi.org/10.1016/j.
carbon.2008.12.038.
[17] Y. Zare, K.Y. Rhee, An innovative model for conductivity of graphene - based
system by networked nano - sheets , interphase and tunneling zone, Sci. Rep. (–9)
(2022) 1, https://doi.org/10.1038/s41598-022-19479-9.
[18] A. Marsden, et al., Electrical percolation in graphene-polymer composites, 2D
Mater. 5 (2018), https://doi.org/10.1088/2053-1583/aac055.
[19] X.-Y. Qi, et al., Enhanced electrical conductivity in polystyrene nanocomposites at,
ACS Appl. Mater. Interfaces 3 (8) (2011) 3130–3133.
[20] M. Haghgoo, R. Ansari, M.K. Hassanzadeh-Aghdam, Synergic effect of graphene
nanoplatelets and carbon nanotubes on the electrical resistivity and percolation
threshold of polymer hybrid nanocomposites, Eur. Phys. J. A 136 (7) (2021),
https://doi.org/10.1140/epjp/s13360-021-01774-5.
[21] M. Cobos, B. González, M.J. Fernández, M.D. Fernández, Chitosan–graphene oxide
nanocomposites: effect of graphene oxide nanosheets and glycerol plasticizer on
thermal and mechanical properties, J. Appl. Polym. Sci. 134 (30) (2017) 1–14,
https://doi.org/10.1002/app.45092.
[22] H. Kim, Y. Miura, C.W. MacOsko, Graphene/polyurethane nanocomposites for
improved gas barrier and electrical conductivity, Chem. Mater. 22 (11) (2010)
3441–3450, https://doi.org/10.1021/cm100477v.
[23] H. Kim, et al., Graphene/polyethylene nanocomposites: effect of polyethylene
functionalization and blending methods, Polymer 52 (8) (2011) 1837–1846,
https://doi.org/10.1016/j.polymer.2011.02.017.
[24] H. Xu, et al., Influence of processing conditions on dispersion, electrical and
mechanical properties of graphene-filled-silicone rubber composites, Composer
Part A Appl. Sci. Manuf. 91 (2016) 53–64, https://doi.org/10.1016/j.
compositesa.2016.09.011.
[25] R. Socher, B. Krause, S. Hermasch, R. Wursche, P. Pötschke, Electrical and thermal
properties of polyamide 12 composites with hybrid fillers systems of multiwalled
carbon nanotubes and carbon black, Compos. Sci. Technol. 71 (8) (2011)
1053–1059, https://doi.org/10.1016/j.compscitech.2011.03.004.
[26] G. Pal, S. Kumar, Multiscale modeling of effective electrical conductivity of short
carbon fiber-carbon nanotube-polymer matrix hybrid composites, Mater. Des. 89
(2016) 129–136, https://doi.org/10.1016/j.matdes.2015.09.105.
[27] A. Motaghi, A. Hrymak, G.H. Motlagh, Electrical conductivity and percolation
threshold of hybrid carbon/polymer composites, J. Appl. Polym. Sci. 132 (13)
(2015) 1–9, https://doi.org/10.1002/app.41744.
[28] R. Nazarov, T. Zhang, M. Khodzitsky, Effective medium theory for multi-
component materials based on iterative method, Photonics 7 (4) (2020) 1–8,
https://doi.org/10.3390/photonics7040113.
[29] K.Y. Yan, Q.Z. Xue, Q.B. Zheng, L.Z. Hao, The interface effect of the effective
electrical conductivity of carbon nanotube composites, Nanotechnology 18 (25)
(2007), https://doi.org/10.1088/0957-4484/18/25/255705.
Materials Chemistry and Physics 309 (2023) 128324
[30] Q.Z. Xue, Model for the effective thermal conductivity of carbon nanotube
composites, Nanotechnology 17 (6) (2006) 1655–1660, https://doi.org/10.1088/
0957-4484/17/6/020.
[31] M. Haghgoo, R. Ansari, M.K. Hassanzadeh-Aghdam, Prediction of electrical
conductivity of carbon fiber-carbon nanotube-reinforced polymer hybrid
composites, Composites, Part B 167 (February) (2019) 728–735, https://doi.org/
10.1016/j.compositesb.2019.03.046.
[32] J. Payandehpeyman, M. Mazaheri, M. Khamehchi, Prediction of electrical
conductivity of polymer-graphene nanocomposites by developing an analytical
model considering interphase, tunneling and geometry effects, Compos. Commun.
21 (2020), 100364, https://doi.org/10.1016/j.coco.2020.100364.
[33] C. Feng, L. Jiang, Micromechanics modeling of the electrical conductivity of carbon
nanotube (CNT)-polymer nanocomposites, Composer Part A Appl. Sci. Manuf. 47
(1) (2013) 143–149, https://doi.org/10.1016/j.compositesa.2012.12.008.
[34] J.G. Simmons, Generalized formula for the electric tunnel effect between similar
electrodes separated by a thin insulating film, J. Appl. Phys. 34 (6) (1963)
1793–1803, https://doi.org/10.1063/1.1702682.
[35] M.A.S. Matos, V.L. Tagarielli, P.M. Baiz-Villafranca, S.T. Pinho, Predictions of the
electro-mechanical response of conductive CNT-polymer composites, J. Mech.
Phys. Solid. 114 (2018) 84–96, https://doi.org/10.1016/j.jmps.2018.02.014.
[36] A. Chanda, S.K. Sinha, N.V. Datla, Electrical conductivity of random and aligned
nanocomposites: theoretical models and experimental validation, Composer Part A
Appl. Sci. Manuf. 149 (July) (2021), 106543, https://doi.org/10.1016/j.
compositesa.2021.106543.
[37] A. Aharoni, Demagnetizing factors for rectangular ferromagnetic prisms, J. Appl.
Phys. 83 (6) (1998) 3432–3434, https://doi.org/10.1063/1.367113.
[38] L. Gao, Z. Li, Effective medium approximation for two-component nonlinear
composites with shape distribution, J. Phys. Condens. Matter 15 (25) (2003) 4397.
[39] F. Deng, Q.S. Zheng, An analytical model of effective electrical conductivity of
carbon nanotube composites, Appl. Phys. Lett. 92 (7) (2008), https://doi.org/
10.1063/1.2857468.
[40] H. Bin Zhang, et al., Electrically conductive polyethylene terephthalate/graphene
nanocomposites prepared by melt compounding, Polymer 51 (5) (2010)
1191–1196, https://doi.org/10.1016/j.polymer.2010.01.027.
[41] S. Stankovich, et al., Graphene-based composite materials, Nature 442 (7100)
(2006) 282–286, https://doi.org/10.1038/nature04969.
[42] N. Yousefi, M.M. Gudarzi, Q. Zheng, S.H. Aboutalebi, F. Sharif, J.K. Kim, Self-
alignment and high electrical conductivity of ultralarge graphene oxide-
polyurethane nanocomposites, J. Mater. Chem. 22 (25) (2012) 12709–12717,
https://doi.org/10.1039/c2jm30590a.
[43] M.V. Zdorovets, I.E. Kenzhina, V. Kudryashov, A.L. Kozlovskiy, Helium swelling in
WO3 microcomposites, Ceram. Int. 46 (8) (2020) 10521–10529, https://doi.org/
10.1016/j.ceramint.2020.01.053.