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Contents lists available at ScienceDirect Mechanics of Materials journal homepage: www.elsevier.com/locate/mechmat Research paper Static and dynamic response of graphene nanocomposite plates with flexoelectric effect K.B. Shingare, S.I. Kundalwal Applied and Theoretical Mechanics (ATOM) Laboratory, Discipline of Mechanical Engineering, Indian Institute of Technology Indore, Simrol, Indore 453 552, India ARTICLE INFO Keywords: Graphene Flexoelectricity Piezoelectricity Nanocomposite Micromechanics Mechanics of materials Finite element Elastic properties ABSTRACT In this work, the electromechanical behaviors of graphene reinforced nanocomposite (GRNC) plates with flexoelectric effect were studied by using Kirchhoff's plate theory, Navier's solution and extended linear piezo- electricity theory in conjunction with the mechanics of materials (MOM) and finite element models. The static and dynamic responses of simply supported flexoelectric GRNC nanoplates under different loadings such as uniformly distributed, varying distributed, inline and point loads were investigated. The developed MOM and FE models envisage that the effective piezoelectric constants of a GRNC account for the actuating capability in its transverse direction due to the applied electric field in the plane. The elastic properties of pristine and defective graphene sheets were also estimated via molecular dynamics (MD) simulations and the obtained results are found in good agreement with the existing experimental and numerical results. Our results reveal that the flexoelectric effect on the static and dynamic responses of GRNC nanoplate is substantial and cannot be ne- glected. The electromechanical response of GRNC plates can be engineered to attain the desired deflection characteristics and resonant frequencies for a range of nanoelectromechanical systems using different boundary conditions as well as geometrical parameters such as aspect ratio/thickness of nanoplate and volume fraction of graphene. 1. Introduction Graphene, one-atom-thick planer layer of carbon atoms discovered and characterized by Novoselov et al. (2004), fascinated rigorous re- search interests and applications in nanoelectromechanical systems (NEMS) owing to its remarkable electro-thermo-mechanical properties such as high Young's modulus ( ∼ 1.1 TPa) and high flexibility, elec- trical conductivity ( ∼ 6000 S/cm), thermal conductivity ( ∼ 5000 W/ m/K) and scale-dependent electronic properties (Zhang et al., 2005; Balandin et al., 2008; Lee et al., 2008; Gupta and Batra 2010; Verma et al., 2014; Cui et al., 2016; Alian et al., 2017; Kundalwal et al., 2017). In the twenty-first century, graphene is considered as one of the most striking 2D material to form next generation NEMS due to its unique multifunctional properties with size-dependent physical structure. Most recently, the piezoelectric effect in non-piezoelectric graphene sheets is found by Kundalwal et al. (2017) using the flexoelectric concept via quantum mechanics calculations. This study revealed that the presence of strain gradient in non-piezoelectric graphene sheet does not only affects the ionic positions, but also the asymmetric redistribution of the electron density, which induces strong polarization in the graphene sheet. This recent finding on the strain gradient polarization in non- piezoelectric graphene added a new functionality in it and this could lead to develop graphene-based energy harvesters. Extensive research has been dedicated to the introduction of gra- phene as the modifiers to the conventional bulk composites in order to improve their multifunctional properties. On the other hand, the use of small quantity of graphene in the conventional matrices is found to alter and improve the thermo-electro-mechanical properties of resulting nanocomposite significantly. For instance, Ji et al. (2016) summarized and reviewed the numerous methods of synthesis of graphene-based nanocomposites and showed the significant enhancement of mechan- ical properties of nanocomposite with mere 0.3 wt.% of graphene over that of the pure aluminum matrix (Ji et al., 2016). Kandpal et al. (2017) experimentally investigated the enhancement of piezo-potential re- sponse such as output voltage of nanogenerator with the accumulation of graphene nanoplates (GNPs) into the polymer nanocomposite, which can be used as an energy harvester. García-Macías et al. (2018) showed that the GNP-based composite is superior than carbon nanotube (CNT)- based composite in terms of the load carrying capacity and stiffening effect. Graphene as well as its derivatives such as graphite oxide and graphene oxide (GO) also highlight promising way towards the bulk use of graphene for commercial applications and NEMS (Cui et al., 2016). https://doi.org/10.1016/j.mechmat.2019.04.006 Received 15 January 2019; Received in revised form 6 April 2019 Corresponding author. E-mail address: [email protected] (S.I. Kundalwal). Mechanics of Materials 134 (2019) 69–84 Available online 13 April 2019 0167-6636/ © 2019 Elsevier Ltd. All rights reserved. T
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Page 1: Mechanics of Materials · electricity theory in conjunction with the mechanics of materials (MOM) and finite element models. The static and dynamic responses of simply supported flexoelectric

Contents lists available at ScienceDirect

Mechanics of Materials

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

Research paper

Static and dynamic response of graphene nanocomposite plates withflexoelectric effectK.B. Shingare, S.I. Kundalwal⁎

Applied and Theoretical Mechanics (ATOM) Laboratory, Discipline of Mechanical Engineering, Indian Institute of Technology Indore, Simrol, Indore 453 552, India

A R T I C L E I N F O

Keywords:GrapheneFlexoelectricityPiezoelectricityNanocompositeMicromechanicsMechanics of materialsFinite elementElastic properties

A B S T R A C T

In this work, the electromechanical behaviors of graphene reinforced nanocomposite (GRNC) plates withflexoelectric effect were studied by using Kirchhoff's plate theory, Navier's solution and extended linear piezo-electricity theory in conjunction with the mechanics of materials (MOM) and finite element models. The staticand dynamic responses of simply supported flexoelectric GRNC nanoplates under different loadings such asuniformly distributed, varying distributed, inline and point loads were investigated. The developed MOM and FEmodels envisage that the effective piezoelectric constants of a GRNC account for the actuating capability in itstransverse direction due to the applied electric field in the plane. The elastic properties of pristine and defectivegraphene sheets were also estimated via molecular dynamics (MD) simulations and the obtained results arefound in good agreement with the existing experimental and numerical results. Our results reveal that theflexoelectric effect on the static and dynamic responses of GRNC nanoplate is substantial and cannot be ne-glected. The electromechanical response of GRNC plates can be engineered to attain the desired deflectioncharacteristics and resonant frequencies for a range of nanoelectromechanical systems using different boundaryconditions as well as geometrical parameters such as aspect ratio/thickness of nanoplate and volume fraction ofgraphene.

1. Introduction

Graphene, one-atom-thick planer layer of carbon atoms discoveredand characterized by Novoselov et al. (2004), fascinated rigorous re-search interests and applications in nanoelectromechanical systems(NEMS) owing to its remarkable electro-thermo-mechanical propertiessuch as high Young's modulus ( ∼ 1.1 TPa) and high flexibility, elec-trical conductivity ( ∼ 6000 S/cm), thermal conductivity ( ∼ 5000 W/m/K) and scale-dependent electronic properties (Zhang et al., 2005;Balandin et al., 2008; Lee et al., 2008; Gupta and Batra 2010; Vermaet al., 2014; Cui et al., 2016; Alian et al., 2017; Kundalwal et al., 2017).In the twenty-first century, graphene is considered as one of the moststriking 2D material to form next generation NEMS due to its uniquemultifunctional properties with size-dependent physical structure. Mostrecently, the piezoelectric effect in non-piezoelectric graphene sheets isfound by Kundalwal et al. (2017) using the flexoelectric concept viaquantum mechanics calculations. This study revealed that the presenceof strain gradient in non-piezoelectric graphene sheet does not onlyaffects the ionic positions, but also the asymmetric redistribution of theelectron density, which induces strong polarization in the graphenesheet. This recent finding on the strain gradient polarization in non-

piezoelectric graphene added a new functionality in it and this couldlead to develop graphene-based energy harvesters.

Extensive research has been dedicated to the introduction of gra-phene as the modifiers to the conventional bulk composites in order toimprove their multifunctional properties. On the other hand, the use ofsmall quantity of graphene in the conventional matrices is found toalter and improve the thermo-electro-mechanical properties of resultingnanocomposite significantly. For instance, Ji et al. (2016) summarizedand reviewed the numerous methods of synthesis of graphene-basednanocomposites and showed the significant enhancement of mechan-ical properties of nanocomposite with mere 0.3 wt.% of graphene overthat of the pure aluminum matrix (Ji et al., 2016). Kandpal et al. (2017)experimentally investigated the enhancement of piezo-potential re-sponse such as output voltage of nanogenerator with the accumulationof graphene nanoplates (GNPs) into the polymer nanocomposite, whichcan be used as an energy harvester. García-Macías et al. (2018) showedthat the GNP-based composite is superior than carbon nanotube (CNT)-based composite in terms of the load carrying capacity and stiffeningeffect. Graphene as well as its derivatives such as graphite oxide andgraphene oxide (GO) also highlight promising way towards the bulk useof graphene for commercial applications and NEMS (Cui et al., 2016).

https://doi.org/10.1016/j.mechmat.2019.04.006Received 15 January 2019; Received in revised form 6 April 2019

⁎ Corresponding author.E-mail address: [email protected] (S.I. Kundalwal).

Mechanics of Materials 134 (2019) 69–84

Available online 13 April 20190167-6636/ © 2019 Elsevier Ltd. All rights reserved.

T

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For instance, Bhavanasi et al. (2016) reported the energy harvestingperformance with the proficient transfer of electromechanical energyfor the film made of bilayer GO and PVDF-TrFE. They observed that GOfilm improved the voltage output and power density of about 2 and 2.5times, respectively, when compared to the PVDF-TrFE film without GO.Few studies elucidated the methods of production, applications, in-ventions and limitations of composites made of graphene and its deri-vatives (Mohan et al., 2018; Sreenivasulu et al., 2018). They focused onseveral components of fortifying, scattering strategies and blendedcomposites utilizing graphene.

Thin composite plates are important types of structural elementsthat have potential applications in NEMS due to their linear behaviorand high sensitivity. For instance, Gao and Shen (2003) demonstratedthat the piezoelectric actuators can significantly reduce the vibrationsof composite plates using the FE analysis. A nonlinear bending analysisfor simply supported antisymmetric cross-ply laminated compositeplates incorporated with the piezoelectric actuators under the com-bined mechanical, electrical and thermal loadings presented byShen (2004). Ray and Pradhan (2006) reported the 1–3 piezoelectricvertically reinforced laminated composite to improve the performanceof hybrid damping using the procedure of active constrained layerdamping (ACLD). Experimental study by Parashar and Mertiny (2012)reported that the buckling capacity of the plate increases when thegraphene reinforced composite is enriched with only low percentage ofgraphene. They reported 26% enhancement in the buckling capacity ofgraphene-based composite plate under the unidirectional compressionwith only 6% volume fraction of graphene. Using the FE method,Chandra et al. (2012) highlighted the enhancement of the natural fre-quencies and mode shapes of graphene/epoxy composite plates. Theyfound that as the plate aspect ratio increases, the natural frequency ofthe graphene/epoxy composite plates decreases. Li and Narita (2014)proposed an active control method to reduce the wind-induced vibra-tion of the laminated composite plates using a velocity feedback controlstrategy. Zhang and Jiang (2014) studied the effect of static bulk flex-oelectricity on the piezoelectric nanoplate to predict its static and dy-namic behavior. Kundalwal and Ray (2016) investigated the influenceof CNT waviness on the smart damping of fuzzy fiber reinforced com-posite plates incorporated with the ACLD patches using 3D FE analysis.Sadeghzadeh (2016) studied the multilayer graphene reinforced plateusing multiscale approach and reported that the spaced multilayergraphene sheets are more efficient than the stacked multilayer gra-phene sheets having interlayer distance 0.34 nm, that is, no metallicnanoparticles or fullerenes exist between two adjacent graphene layers.Song et al. (2006) studied the free and forced vibrations of multilayerGNP-reinforced composite plates subjected to the axial compressionand transverse loadings. They revealed that the small amount of GNPssignificantly increases the critical buckling load of composite plate andreduces its vibration. Feng et al. (2017) examined the nonlinearbending behavior of polymer nanocomposite beams reinforced withmulti-layered GNPs that are non-uniformly dispersed in the thicknessdirection of beam. They found that the bending performance of polymermatrix nanocomposite significantly improved by adding small amountof GNPs. The micromechanical model and multiscale approach weredeveloped by Shen et al. (2017) for analyzing the post-buckling beha-vior of functionally graded (FG) graphene-based laminated compositeplates under the uniaxial compression in thermal environments. Theinfluence of surface effects on the nanoscale plate was investigated byLiu and Rajapakse (2013) and Sapsathiarn and Rajapakse (2017) tostudy its static and dynamic behavior. They also derived a solution forthe nanoscale rectangular plates using the FE approach.Karimi et al. (2017) investigated the effect of different parameters suchas nonlocal and surface layers on the in-phase and out-of-phase naturalfrequencies of double-layer piezoelectric nanoplate subjected to thethermo-electro-mechanical loadings. Zhao et al. (2017) investigated thebending and vibration behavior of FG GNP-reinforced trapezoidalplates using the FE method. They also predicted the effective material

properties such as Young's modulus, mass density and Poisson's ratio ofthe GNP-nanocomposite using modified Halpin–Tsai model and therules of mixture. Most recently, Rouzegar and Abbasi (2018) developedFE model to study the bending analysis of laminated plates integratedwith the piezoelectric fiber-reinforced composite actuators.

The review of literature presented on graphene-based compositeplates clearly indicates that graphene is the most attracting 2D material,vastly studied in the last decade. Nevertheless, to date, to the best of thecurrent authors’ knowledge, there is no single study for investigatingthe static and dynamic response of a flexible piezoelectric graphenereinforced nanocomposite (GRNC) nanoplate considering the flexo-electric effect, which can offer many opportunities for developing nextgeneration NEMS. This provided the motivation for the present re-search. The aim of our research is to further broaden the knowledgebase of existence of strain and electric field gradients in thin nanoplates.Before proceeding further, we discuss the concept of flexoelectricity.

1.1. Flexoelectricity

Over the last two decades, the flexoelectricity phenomenon hasreceived much attention from both fundamental and application pointof view with aim of developing NEMS. Recently, the piezoelectric na-noplate based NEMS have attracted the enormous interest in the re-search community due to their potential use as a numerous nano-technology-based devices such as sensors, actuators, transistors, energyharvesters, nano-generators, electric switches and distributors (Denget al. 2014; Zhang and Jiang, 2014; Sapsathiarn and Rajapakse, 2017).The interfaces in nonpolar materials and symmetry breaking at thesurfaces permit novel forms of electromechanical coupling such asflexoelectricity and surface piezoelectricity, which can be induced onlyin the nanoscale materials. For a better understanding of flexoelec-tricity, first the concept of piezoelectricity and its mathematical relationis described; as follows:

P di ijk jk (1)

In the above relation, Pi denotes the polarization vector, ɛjk is thestrain tensor, and dijk is the piezoelectric tensor. This phenomenonexists in the material where the inversion symmetry plays a significantrole. As it was mentioned earlier, by breaking the inversion symmetryeven in the centrosymmetric crystals one can introduce the polarizationdue to the nonuniform strain gradient, and this phenomenon is wellknown as the flexoelectric effect. In 1964, Kogan Kogan, 1964) reporteda theoretical understanding of electron-phonon coupling which is re-sponsible for the flexoelectricity in centrosymmetric crystals. He hasprovided the estimation for the lower bounds of felxoelectric coeffi-cients with the help of relation between the electronic charge (e) inelectron volt and lattice parameter (a). Hence, the approximated valueof the flexoelectric coefficient (e/a) is interpreted 10 C/m9

(Nguyen et al., 2013). This phenomenon presents in all dielectric andinsulating materials (Tagantsev, 1986; Ma and Cross, 2006; Marangantiet al., 2006). The constitutive relation ((1) for the polarization vectoraccounting the flexoelectric effect may be re-written as

+P d fddxi ijk jk ijkl

jk

l (2)

where fijkl is the flexoelectric tensor and ddx

jk

lis strain gradient.

The organization of the article is as follows: Section 2 presents thedevelopment of modified mechanics of materials (MOM) model to de-termine the effective properties of GRNC. In this section, FE modelswere also developed, and they provided interesting numerical valuesfor validating the predictions of MOM model. In Section 3, we pre-sented an analytical model based on Kirchhoff's plate theory and Na-vier's solution for the simply supported GRNC nanoplates with flexo-electric effect. We derived closed form solutions for nanoplates withdifferent boundary and loading conditions which were not considered

K.B. Shingare and S.I. Kundalwal Mechanics of Materials 134 (2019) 69–84

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in the literature. In Section 4, the elastic properties of pristine anddefective graphene layers were evaluated using the molecular dynamics(MD) simulations. Section 5 presents the validations of our findings aswell as results for analyzing the static and dynamic behavior of GRNCnanoplates with flexoelectric effect considering different boundaryconditions and geometrical parameters. In Section 6, main inferencesare drawn from the current study.

2. Effective properties of GRNC

In this section, assuming a graphene sheet as a piezoelectric con-tinuum, the piezoelectric and elastic (piezoelastic) as well as dielectricproperties of GRNC were estimated. To simplify computational efforts,bulk properties of 2D graphene layer were obtained by considering it asa continuum plate (Roberts et al., 2010; Politano and Chiarello, 2013,and references therein; Hosseini-Hashemia et al., 2018). Using theconcept of continuum elasticity, analytical and numerical solutionswere obtained for graphene layers under strains (Gupta and Batra,2010; Gradinar et al., 2013; Verma et al., 2014; Bahamon et al., 2015).This suggests that the displacement of each carbon atom in homo-geneously deformed graphene layer is given by the deformation of thecontinuum medium, on which the atom is embedded.

A novel GRNC is reinforced with the multilayers of piezoelectricgraphene sheets and polyimide matrix. Such GRNC can be considered ascomposed of rectangular representative volume elements (RVEs) com-prising both graphene and polyimide matrix, as shown in Fig. 1, and welimited the development of our micromechanical model to a single RVE.We assumed that no slippage occurs between a graphene sheet and thesurrounding matrix, and the resulting nanocomposite is linearly elasticand homogeneous (Gao and Li, 2005; Song and Youn, 2006; Jiang et al.,2009; Kundalwal and Ray, 2011, 2013). The top and bottom surfaces of

the GRNC lamina are electroded and the electric field is applied alongits thickness. The conducting electrodes maintain constant electrostaticpotentials on both the upper and lower surfaces of GRNC lamina. SuchGRNC lamina demonstrates the inverse piezoelectric effect and may beconsidered as a capacitor having two parallel plates in which the gra-phene layers and polyimide matrix act as the dielectric mediums. Theeffective piezoelastic and dielectric properties of GRNC can be de-termined by using the analytical and numerical micromechanicalmodels.

Fig. 1. (a) Schematic representation of GRNC lamina and (b) cross-sections of an RVE of GRNC.

Fig. 2. Finite element meshing of RVE of GRNC.

K.B. Shingare and S.I. Kundalwal Mechanics of Materials 134 (2019) 69–84

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2.1. Mechanic of materials (MOM) model for GRNC

The effective piezoelastic and dielectric properties of GRNC can beobtained by modifying the existing mechanics of materials (MOM)model (Kundalwal and Ray, 2011). Fig. 1(b) demonstrates an RVE ofthe GRNC lamina in which the graphene layers are incorporated alongits thickness direction. Smith and Auld (1991) used the strength ofmaterials approach to predict the effective piezoelastic properties of the1–3 piezoelectric composite in which PZT fibers of square cross-sectionwere surrounded by the epoxy matrix. Note that the effective piezo-elastic properties predicted by Smith and Auld (1991) are most feasiblefor controlling the thickness mode oscillations of thin composite plates.Our micromechanical analysis was confined to the RVE of GRNC (seeFig. 1(b)) for determining the effective properties of bulk GRNC.

We assumed plane strain deformations in the GRNC lamina andnormal stresses can be induced in it due to the applied electric field (E3)along the 3-axis of the GRNC. The constitutive equations for the con-stituents of GRNC can be written as follows:

= ={ } [C ]{ } {e }E and { } [C ]{ }g g g g3

m m m (3)

= ={ } , { }r

1r

2r

3r

23r

13r

12r

r

1r

2r

3r

23r

13r

12r (4)

= = =[C ]

C C C 0 0 0C C C 0 0 0C C C 0 0 00 0 0 C 0 00 0 0 0 C 00 0 0 0 0 C

, {e }

eee000

, r g and mr

11r

12r

13r

12r

22r

23r

13r

23r

33r

44r

55r

66r

g

31g

32g

33g

In Eqs. (3) and (4), the respective g and m superscripts represent thegraphene and polyimide matrix. The superscript r is used to indicate thecorresponding constituent phase; 1

r, 2r, and 3

r are the normal stressesin the directions 1, 2, and 3, respectively; 1

r, 2r, and 3

r are the re-spective normal strains; 12

r , 13r , and 23

r are the shear stresses; 12r , 13

r ,and 23

r are the shear strains; Cijr (i,j= 1,2 and 6) are the elastic coeffi-

cients of rth phase; and e31g , e32

g , and e33g are the piezoelectric coefficients

of a graphene.Using isostrain and isostress conditions (Smith and Auld, 1991;

Benveniste and Dvorak, 1992; Ray, 2006), the perfect bonding amongsta graphene layer and the matrix can be modelled by satisfying thefollowing:

= = and

1g

2g

3g

23g

13g

12g

1m

2m

3m

23m

13m

12m

1NC

2NC

3NC

23NC

13NC

12NC

(5)

Using the rules of mixture, we can write:

+ =v vg

1g

2g

3g

23g

13g

12g

m

1m

2m

3m

23m

13m

12m

1NC

2NC

3NC

23NC

13NC

12NC

(6)

in which the superscript NC denotes the quantities of RVE of GRNC, andvg and vm are the volume fractions of a graphene layer and the poly-imide matrix, respectively. Using Eqs. (3–6), the stress and strain vec-tors of homogenized GRNC can be written in terms of the respectivestress and strain vectors of constituent phases as follows:

= +=

= +C

{ } [C ]{ } [C ]{ } {e }E ,[ ]{ } [C ]{ } {e }E and{ } [V ]{ } [V ]{ }

NC1

g2

m1 3

3m

4m 2

3NC

1g

2m (7)

The matrices appeared in Eq. (7) are given as follows:

=[C ]

C C C 0 0 0C C C 0 0 0

v C v C v C 0 0 00 0 0 C 0 00 0 0 0 C 00 0 0 0 0 C

1

11g

12g

13g

12g

22g

23g

g 13g

g 23g

g 33g

44p

55p

66p

= = =[C ]

0 0 0 0 0 00 0 0 0 0 0

v C v C v C 0 0 00 0 0 0 0 00 0 0 0 0 00 0 0 0 0 0

, {e }

ee

v e000

, {e }

ee0000

2m 13

mm 23

mm 33

m1

31g

32g

g 33g

2

31g

32g

=

=

[C ]

C C C 0 0 0C C C 0 0 00 0 1 0 0 00 0 0 C 0 00 0 0 0 C 00 0 0 0 0 C

,

[C ]

C C C 0 0 0C C C 0 0 00 0 1 0 0 00 0 0 C 0 00 0 0 0 C 00 0 0 0 0 C

3

11g

12g

13g

12g

22g

23g

44g

55g

66g

4

11m

12m

13m

12m

22m

23m

44m

55m

66m

= =[V ]

v 0 0 0 0 00 v 0 0 0 00 0 1 0 0 00 0 0 v 0 00 0 0 0 v 00 0 0 0 0 v

, and [V ]

v 0 0 0 0 00 v 0 0 0 00 0 0 0 0 00 0 0 v 0 00 0 0 0 v 00 0 0 0 0 v

1

g

g

g

g

g

2

m

m

m

m

m

Making the use of Eq. (5) into Eq. (7), a constitutive relation for theGRNC can be written as:

={ } [C ]{ } {e }ENC NC NC NC3 (8)

in which CNC and {eNC} are the matrices for the effective elastic andpiezoelectric properties of GRNC, respectively, and can be obtained asfollows:

= += += +

= +

[C ] [C ][V ] [C ][V ] ,[V ] [V ] [V ][C ] [C ],[V ] [V ] [V ][C ] [C ] and{e } {e } [C ][V ] [V ][C ] {e } [C ][V ] [V ][C ] {e }

NC1 3

12 4

1

3 1 2 41

3

4 2 1 31

4NC

1 1 31

2 41

2 2 41

1 31

2 (9)

From Eq. (9), the effective piezoelectric coefficients of the GRNCcan be identified as =e e (1)31

NC , =e e (2)32NC , and =e e (3)33

NC .Consequently, the effective dielectric constant ( 33

NC) of GRNC is derivedby using the following relation (Ray and Pradhan 2006):

= + + +v v e v v /(v C v C )33NC

g 33g

m 33m

31g

g m m 11g

g 11m (10)

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2.2. Finite element (FE) modeling of GRNC

The MOM model developed in the preceding section is based on theisofield conditions in which the RVE of GRNC was imposed to theuniform stresses and strains. To validate such assumptions, the FEmodels can be developed which do not require any such assumption. Inthis section, FE models were developed using the commercial softwareANSYS 15.0. The FE approach allows the fully coupled electro-mechanical analysis and we obtained the homogenized effective ma-terial properties by modeling 3-D RVE of GRNC with 20 noded brickelements “solid 226″ having both displacement and electric potential(voltage) degrees of freedom (DOF). Using the material properties of agraphene layer and the polyimide matrix, a two-phase FE model of theRVE with its axis of transverse isotropy being the 3-axis is to be de-veloped for estimating the independent piezoelastic and dielectricconstants: C11

NC, C12NC, C23

NC, C33NC, e31

NC, e33NC, and 33

NC. These effective con-stants of the GRNC can be evaluated by applying the appropriateboundary constraints to its RVE.

The constitutive relations for the effective elastic constants (CijNC),

piezoelectric constants (eijNC), and dielectric constants ( ij

NC) of GRNCcan be written as:

=

¯¯¯¯¯¯DDD

C C C 0 0 0 0 0 eC C C 0 0 0 0 0 eC C C 0 0 0 0 0 e

0 0 0 C 0 0 0 e 00 0 0 0 C 0 e 0 00 0 0 0 0 C 0 0 00 0 0 0 e 0 0 00 0 0 e 0 0 0 0

e e e 0 0 0 0 0

¯¯¯¯¯¯EEE

11

22

33

23

13

12

1

2

3

11NC

12NC

13NC

31NC

12NC

22NC

13NC

31NC

13NC

13NC

33NC

33NC

44NC

15NC

55NC

15NC

66NC

15NC

11NC

15NC

22NC

31NC

31NC

33NC

33NC

11

22

33

23

13

12

1

2

3

(11)

The averaged stresses {¯ij}, strains { ij}, electrical displacements{Di}, and electric field {Ei} can be evaluated using the following rela-tions when the RVE is subjected to the electromechanical loads:

= =

= =

{ ¯ } { }V , {¯ } { }V

{D } {D }V , {E } {E }Vij

1V 1

nij e ij

1V 1

nij e

i1V 1

ni e i

1V 1

ni e (12)

where V denotes the volume of the RVE, Ve is the volume of finiteelement, and n is the total number of finite elements. The quantityhaving overbar symbolizes the volume averaged quantity. It is ob-served from Eq. (11) that if at any point in the GRNC only one normalstrain exists while the other strain components are zero, then threenormal stresses are nonzero. The ratio of one of these three normalstresses and the strain yields respective effective elastic constant.Hence, with one FE numerical simulation, we can obtain three effec-tive elastic constants at a point in the RVE. Detailed procedure ofdevelopment FE models under appropriate boundary conditions isdescribed elsewhere Kundalwal and Ray, 2012; Kundalwal et al.,2018.

3. Electromechanical response of GRNC nanoplates

3.1. Governing equations for GRNC nanoplates

In this section, the governing equations for simply supported (SS)piezoelectric GRNC nanoplate subjected to the uniformly distributedmechanical load (q0) are derived to investigate its static bending anddynamic behavior. Fig. 3 shows the schematic of SS GRNC nanoplatehaving thickness h, length a, and width b. A Cartesian coordinatesystem was used to describe the nanoplate with thickness along the z-axis and the mid plane of the undeformed nanoplate coincides with thex–y plane.

As per Kirchhoff's plate theory, the plate displacement in terms oftransverse displacement w(x, y, t) can be expressed as (Zhao et al.,2012):

=u(x, y, z, t) z w(x, y, t)x (13)

=v(x, y, z, t) z w(x, y, t)y (14)

=w(x, y, z, t) w(x, y, t) (15)

in which u and v are the displacement components along the x and ydirections, respectively; t is the time; and w is the transverse dis-placement. Consequently, the nonzero strains can be written as follows:

= = =z wx

, z wy

, z wx yxx

2

2 yy2

2 xy2

(15a)

Assuming the electric field Ez exists only in the z-direction of thenanoplate, the in-plane dimensions and electric field components in thex y plane can be eliminated when they are compared with that in thethickness direction (Ying and Zhifei, 2005; Ray and Pradhan, 2006).Assuming infinitesimal deformation, considering the electric field,strain gradient coupling and purely nonlocal elastic effects the gen-eralized equation for the electric Gibbs free energy density function Ucan be written as follows (Hu and Shen, 2009):

= +

+ +

U 12

E E 12

C e E f E

r 12

g

kl k l ijkl ij kl ijk ij k ijkl i jkl

ijklm ij klm ijklmn ijk lmn (16)

rijklm represents the coupling between the strain and strain gradientwhile gijklmn represent the elements for purely nonlocal elastic effects,related to the strain gradient elastic theories. For the sake of simplicity,in centrosymmetric materials, the terms gijklmn and rijklm are assumed tobe zero. Under infinitesimal deformation, the constitutive equations forthe dielectric material considering the flexoelectric effect at nanoscalelevel can be written as (Hu and Shen, 2009):

= =U C e Eijij

ijkl kl ijk k(17)

= =U f Eijmijm

kijm k(18)

= = + +D UE

e E fii

jki jk ij j ijkl jkl (19)

where, ∈ ij, Cijkl and eijk are the dielectric, elastic and piezoelectrictensors, respectively; fijkl is the fourth order tensor representing thehigher order electric field-strain gradient coupling; σij is the traditionalstress tensor which is analogous to that in the classical theory of elas-ticity; Di and τijm are the electric displacement vector and higher-order

Fig. 3. Schematic of GRNC nanoplate subjected to the uniformly distributedload.

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stress tensor, respectively; Ei and ηjkl are the electric field vector andstrain gradient tensor, respectively, which can be obtained as follows:

=jkl jk,l (20)

Using the Eqs. (17)–(19), the constitutive relations can be re-formulated as:

= +C C e Exx 11 xx 12 yy 31 z (21)

= +C C e Eyy 12 xx 11 yy 31 z (22)

= 2Cxy 66 xy (23)

= f Exxz 14 z (24)

= f Eyyz 14 z (25)

= + + + +D e ( ) E f ( )z 31 xx yy 33 z 14 xxz yyz (26)

where f14 = f3113 = f3223 (Shu et al., 2011). For the sake of simplicity,the strain gradients other than =xxz

wx

22 and =yyz

wy

22 are as-

sumed to be zero, since the associated flexoelectric coefficients or straingradients are much smaller as compared to those along the thicknessdirection of GRNC nanoplate. Due to the absence of external electricfield, it can be clearly seen that the 3rd term in Eq. (26) indicates thepolarization induced in the nanoplate due to the strain gradients.

Using the equations of Gauss' Law of Electrostatics, in the absence offree electric charge, the electric displacement for the thin nanoplate canbe written as

=Dz

0z(27)

In case of open-circuit condition, on the surface of nanoplate theelectric displacement is zero. Therefore, from Eq. (27), the internalelectric field can be derived as follows:

= + + +E e wx

wy

z f wx

wyz

31

33

2

2

2

214

33

2

2

2

2 (28)

From Eq. (28) it can be observed that the first term e3133

related tothe piezoelectricity signifies the electric field induced due to the ap-plication of elastic strains, and the second term f14

33related to the

flexoelectricity signifies the electric field induced due to the applica-tion of elastic strain gradients. Considering the flexoelectricity, thepiezoelectricity associated internal electric field no longer remainsanti-symmetric respective to the midplane of the nanoplate in thedirection of its thickness. Then, taking the summation of the curva-tures at an arbitrary point in the nanoplate as a whole, Eq. (28) can berewritten as = +Ez

e z f31 1433

G with G= +wx

wy

22

22 . Note that the response

of the electric field Ez to G is intensely dependent on the z-coordinate.In addition, term +ze f31 14 is dependent on the thickness of nanoplateand its flexoelectric coefficient. If the piezoelectric effect is not takeninto account then the solution is attributed to the flis dependen effect(i.e., f14).

The governing equations for the SS nanoplate problems can be de-rived using Hamilton's variational principle; such as (Mindlin, 1968):

+ + =UdV K W dt 0t1

t2

V (29)

where V is the entire volume occupied by the GRNC nanoplate and U isthe electric Gibbs free energy density. In case of open-circuit condition,the relation of U can be written as

= +U 12

12ij ij ijk ijk (30)

If the vibration along the x y plane is ignored then the kineticenergy (K) is given by

=K 12

wt

dVV

2

(31)

where ρ is the mass density.The work done (W) due to the application of external load can be

determined as follows:

=W q wdydx0

a

0

b0 (32)

An energy formulation for continuum electro-elasticity is based onthe principle of minimum free energy, which is mainly suitable forcomplex materials with significant gradient effects and analysis ofstability (Liu et al., 2013). Therefore, the governing equation can bewritten as

+ + + + + + =qMx

Mx y

Mx y

My

Nx

Ny

h wt

02

xx2

2xy

2yx

2yy

2

2xxz2

2yyz2

2

2 0

(33)

Boundary conditions for SS rectangular GRNC nanoplates on all fouredges are prescribed and can be deduced as at =x 0 and =x a:

+

+ +

M N or

M or

or w

xx xxzwx

xywy

Mx

My

Nx

xx yx xxz(34)

at =y 0 and =y b:

+

+ +

M or

M N or

or w

yxwx

yy yyzwy

Mx

My

Ny

xy yy yyz

(35)

where Mxx, Mxy, Myx and Myy are the bending moments, andNxxz and Nyyz are the axial forces along the thickness; these can be ob-tained as follows:

= = = =M zdz, M zdz, M M zdzxx h/2

h/2xx yy h/2

h/2yy xy yx h/2

h/2xy

(36)

= =N dz, N dzxxz h/2

h/2xxz yyz h/2

h/2yyz (37)

Substituting Eqs. (15a) and (28) into the constitutive relations(21)–(25), the explicit expressions for the stresses and higher-orderstresses related to the transverse deflection (w) can be written as,

= + +

+

C e wx

z C e wy

z

e f wx

wy

xx 11312

33

2

2 12312

33

2

2

31 14

33

2

2

2

2 (38)

= + +

+

C e wx

z C e wy

z

e f wx

wy

yy 12312

33

2

2 11312

33

2

2

31 14

33

2

2

2

2 (39)

= 2C wx y

zxy 662

(40)

= = + +e f wx

wy

z f wx

wyxxz yyz

31 14

33

2

2

2

2142

33

2

2

2

2 (41)

Making the use of Eqs. (38)–(41) into Eqs. (36)–(37), the bendingmoments can be obtained in terms of w as follows:

= + +M C e h12

wx

C e h12

wyxx 11

312

33

3 2

2 12312

33

3 2

2 (42)

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= + +M C e h12

wx

C e h12

wyyy 12

312

33

3 2

2 11312

33

3 2

2 (43)

= =M M 2C h12

wx yxy yx 66

3 2

(44)

= = +N N f wx

wy

hxxz yyz142

33

2

2

2

2 (45)

After careful observations of Eqs. (38)–(45), it can be observed thatthe fl, it can be ob significantly influences the distribution of stress andhigher-order stresses. Accordingly, the higher-order stress vanisheswhen the flexoelectric effect is not considered and the conventionalbending moments are not influenced by the strain gradient polarization.Moreover, the introduction of flexoelectric effect is n effect yields thesummations of higher-order stresses.

Using Eqs. (42)–(45) into Eq. (33), the governing equation can bewritten in terms of w as follows:

+ + + + = qD wx

wy

2(D 2D ) wx y

h wt11

4

4

4

4 12 664

2 2

2

2 0 (46)

with

= + +

= + +

=

h

h

D C

D C

D C

11 11e h

12f

12 12e h

12f

66 66h12

312

33

3 142

33

312

33

3 142

33

3

(47)

3.2. Exact solution for static bending response of GRNC nanoplates

For static bending response of the piezoelectric GRNC nanoplates,the governing Eq. (46) can be re-written as follows Reddy (2003):

+ + + = qD wx

wy

2(D 2D ) wx y11

4

4

4

4 12 664

2 2 0 (48)

It may be noted that in the absence of flexoelectricity, the governingEq. (48) follows the conventional classical Kirchhoff plate theory con-sidering linear piezoelectricity. According to the conventional platetheory, for solving the governing Eq. (48) of the SS GRNC nanoplate,the following Fourier series can be used to determine w (x, y)

== =

x yw(x, y) A sin sinm 1 n 1

mn(49)

where = =,ma

nb and Amn are the coefficients to be calculated for

each m and n half wave numbers that should be satisfied everywhere inthe domain of a nanoplate. It has previously corroborated that Eq. (49)satisfies the boundary conditions given in Eqs. (34) and (35). Using theexpression of Fourier series, the uniformly distributed load q0 (x, y) canbe obtained as follows,

== =

xq(x, y) Q sin sin ym 1 n 1

mn(50)

with

=w(x, y) Qd

andmn

mn

where

= =Q16q

mnm, n 1, 3, 5, ......mn

02 (51a)

= + + +db

D ma

D nb

2(D 2D ) mnabmn

411

412

412 66

2

(51b)

Substituting Eqs. (49)–(50) into Eq. (48), we can derive the solution

for the SS nanoplate to obtain its transverse deflection.

=+ + += … = … { }( ) ( ) ( )

w(x, y)16q sin x sin y

mn D D 2(D 2D )0

6m 1,3,5 n 1,3,5 11

ma

412

nb

412 66

mnab

2

(52)

3.3. Exact solution for dynamic response of GRNC nanoplates

Using Eq. (46), the governing equation for the GRNC nanoplate canbe written as

+ + + + =D wx

wy

2(D 2D ) wx y

h wt

0114

4

4

4 12 664

2 2

2

2 (53)

Similar to the conventional plate model, the harmonic solution forw (x,y,t) is derived as

== =

w(x, y, t)sin n y

be

m 1 n 1

B sin m xa i t

mnmn

(54)

where Bmn is a constant indicating the mode shape amplitude; m and nare the half wave numbers; ωmn is the resonant frequency; and =i 1 .

Making use of Eq. (54) into Eq. (53) yields the nanoplate resonantfrequency; as follows:

+ + + =D ma

nb

2(D 2D ) ma

nb

h 0114 4

12 662 2

mn2

(55)

Henceforth, the resonant frequency for nanoplate can be obtainedfor different order numbers m and n as:

= + + +h

D ma

nb

2(D 2D ) ma

nbmn

2

114 4

12 662 2

(56)

From above it is clear that the resonant frequency can be de-termined using the traditional theory of piezoelectricity if the flexo-electric effect is neglected.

4. Elastic properties of graphene

In the literature, piezoelectric properties of graphene sheets con-taining non-centrosymmetric pores are available (Kundalwal et al.,2017) but their elastic properties need to be estimated. Therefore, wefirst determined the elastic properties of (i) pristine graphene sheet and(ii) defective graphene sheets containing 4.5% and 20% vacancies inform of non-centrosymmetric pores using MD simulations. Schematicsof such graphene layers are shown in Fig. 4. All MD simulations runswere conducted with large-scale atomic/molecular massively parallelsimulator (LAMMPS) (Plimpton 1995), and the molecular interactionsin CNTs are described in terms of Adaptive Intermolecular ReactiveEmpirical Bond Order (AIREBO) force fields (Stuart et al., 2000). Theatomic volume was determined from the relaxed graphene sheet withthe thickness (t) of 3.4 Å (Huang et al., 2006; Pei et al., 2010). Thestress in the graphene sheet was computed by averaging the obtainedstress of each carbon atom in it. Then, the stress-strain curves duringthe tensile loading were obtained, and Young's modulus (E) and Pois-son's ratio of pristine and defective graphene sheets were determined.Detailed procedure of MD simulations is described elsewhere(Kundalwal and Choyal, 2018). The predicted elastic properties ofgraphene are summarized in Table 1.

The predictions of pristine graphene agree well with the existingresults obtained by using different modeling techniques and potentialsas well as experimental estimates (Lee et al., 2008; Jing et al., 2012;Dewapriya et al., 2015). In case of defective graphene, we validated ourresults with those reported by Jing et al. (2012). They used COMPAASforce field to model the defective graphene sheets containing vacancies

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which were functionalized by hydrogen atoms on the dangling bonds.The percentage of reduction in Young's modulus ∼1.6% in case ofgraphene containing 6 carbon atom vacancies (that is, 4.5% vacancies)is found to be close with that reported by Jing et al. (2012). They re-ported the percentage of reduction ∼1.53% for functionalized gra-phene with 6 missing carbon atoms. In case of 20% vacancies, theelastic properties of graphene are not much significantly affected. Thisis attributed to the hydrogenation and saturation of the dangling bondsat the edges and porosity in graphene sheet (Jing et al., 2012).

5. Result and discussion

In this section, we discussed the numerical outcomes of effectivepiezoelastic and dielectric properties of GRNC estimated by means ofMOM and FE models developed in the previous sections. The piezo-electric properties of graphene sheets containing non-centrosymmetricpores were taken from Ref. Kundalwal et al. (2017). The graphene sheetunder consideration has 224 carbon atoms and accordingly, the normalpiezoelectric coefficient (e33) was determined as 0.221 C/m2 when thevalue of = 15.2Å. The material properties of graphene and polyimidematrix are summarized in Table 1.

Practically, the fiber volume fraction in the composite can varytypically from 0.2 to 0.7 and hence, this range was considered to ana-lyze the effect of graphene volume fraction on the piezoelastic and di-electric properties of GRNC. Unless otherwise mentioned, the pristinegraphene was considered to determine the piezoelastic and dielectricproperties of GRNC. First, the effective piezoelastic and dielectricproperties of GRNC were determined using the MOM and FE ap-proaches as shown in Figs. 5–10. In FE simulations, the governingequations were solved by using a linear perturbation for piezoelectricanalysis and the sparse direct solver was used for structural analysis.First, the FE mesh convergence was carried out to study the effect ofelement size on the effective properties of GRNC for obtaining the re-liable results.

Fig. 5 demonstrates the variation of effective elastic constant C11NC of

the GRNC against the volume fraction of graphene (vg). It may be ob-served that the values of C11

NC are overestimated by the MOM modelcompared to the FE results, especially for higher values of vg. The sametrends of results were obtained for the values of C12

NC but are not shownhere for the sake of brevity; some predictions of C12

NC are summarized inTable 2. It is well known fact that the transverse elastic properties ofcomposite are mostly the function of matrix material properties,therefore, the predictions of both the models are in good agreement forthe lower values of vg or higher values of vm. The calculated values ofC22

NC are found to be identical to those of C11NCand are not shown here.

This is attributed to the fact that the constructional feature of GRNCdemonstrates the transversely isotropic behavior with the axis of sym-metry along the 3-direction. Fig. 6 shows the variation of effectiveelastic constant C23

NC of the GRNC against the volume fraction of gra-phene (vg). The predicted values of C23

NC by the MOM approach are

slightly lower than that of predictions by FE model and this indicatesthat the Poisson's effect in GRNC is accurately captured by the former.Due to the exerted load along the axis of symmetry (i.e., 3-direction),the extension-extension coupling occurs between the different normalstress (σ33) and normal strain (ɛ22), and FE simulations captured suchcoupling accurately. The predictions of values of C13

NC are found to besame as those of C23

NC and are not shown here for the sake of brevity.It may be observed from Figs. 5 and 6 that the predictions by both

the models differ as the graphene volume fraction increases. Such dis-crepancy exists because the transverse properties of composite arematrix dependent and hence the discrepancy between the predictionsby models increases as the matrix volume fraction decreases. Thisclearly indicates that the MOM model cannot accurately model isostressconditions (Eq. (5)) applied to the RVE of GRNC. Likewise, other re-searchers also observed the discrepancy in the predictions of transverseproperties of composite (Pettermann and Suresh, 2000; Odegard,2004). Fig. 7 depicts the variation of effective axial elastic constant C33

NC

of the GRNC with the volume fraction of graphene (vg). It can be ob-served that the values of C33

NC vary almost linearly with the values of vg

and both the models predict indistinguishable results. This comparisonalso ensures the validity of rules of mixture as well as the assumptionsadopted to develop MOM model, especially the isostrain condition. Theexisting experimental studies also reported the same for the axialproperties of graphene-based nanocomposite (Zhao et al., 2010; Khanet al., 2012; Ji et al., 2016; García-Macías et al., 2018). Note that theeffective longitudinal or axial elastic constant is usually estimated byusing the isostrain condition, which models actual experiments almostexactly, along the axis of symmetry and therefore, the predictions ofvalues of C33

NC are identical to that of Voigt-upper bound predictions. Itcan be observed from Figs. 5 and 7 that the magnitude of values of C33

NC

is significantly higher than that of the values of C11NC for a given value

of vg. This indicates that the axial stiffness of GRNC lamina is enhancedby aligning the graphene layer in the same direction. The effectiveelastic constant C66

NC is a function of elastic constants C11NC and C12

NC andhence the predictions C66

NC are not shown here.Figs. 8–10 demonstrate the variations of effective piezoelectric

coefficients e31NC and e33

NC as well as the axial dielectric constant 33NC of

GRNC against the volume fraction of graphene (vg). It can be observedfrom Fig. 8 that the value of e31

NC increases with the increase in thegraphene volume fraction. Since the GRNC is transversely isotropicmaterial with the axis of symmetry being aligned along the 3-direction,the values of e32

NC of the GRNC are found to be identical those of e31NC. It

can be seen from Figs. 9 and 10 that both the models predict almostidentical and linear estimates for the values of e33

NCand 33NC for a vast

range of volume fraction of graphene, respectively. Comparison of re-sults obtained by the MOM and FE models reveals that the formermodel yields conservative predictions for the most of the piezoelasticproperties of GRNC. Therefore, we considered the properties of GRNC(with 0.5 graphene volume fraction) predicted by the MOM model insubsequent sections to investigate the static and dynamic response of

Fig. 4. Armchair graphene sheet with trapezoidal pore subjected to axial stress: (a) 4.5% and (b) 20% vacancies.

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GRNC nanoplates.To investigate the effect of flexoelectricity on the electromechanical

response of GRNC nanoplates, we considered both pristine and defectedTable1

Mat

eria

lpro

pert

ies

ofgr

aphe

nela

yer

and

poly

imid

em

atri

x.

Mat

eria

lE

(GPa

e 31

(C/m

2 )e 3

3(C

/m2 )

33(F

/m)

Pris

tine

Gra

phen

e98

5(p

rese

nt)

0.26

5(p

rese

nt)

−0.

221

(Kun

dalw

alet

al.,

2017

)0.

221

(Kun

dalw

alet

al.,

2017

)1.

106

x10

−10

(Muñ

oz-H

erná

ndez

etal

.,20

17)

Gra

phen

ew

ith4.

5%va

canc

y96

9(p

rese

nt)

0.26

5(p

rese

nt)

−0.

027

(Kun

dalw

alet

al.,

2017

)0.

027

(Kun

dalw

alet

al.,

2017

)1.

106

×10

−10

Gra

phen

ew

ith20

%va

canc

y89

0(p

rese

nt)

0.26

5(p

rese

nt)

−0.

12(K

unda

lwal

etal

.,20

17)

0.12

(Kun

dalw

alet

al.,

2017

)1.

106

×10

−10

Poly

imid

e4.

2(O

dega

rdet

al.,

2005

)0.

4(O

dega

rdet

al.,

2005

)–

–3.

009

×10

−11

(Lie

tal

.,20

15)

Fig. 5. Variation of effective elastic constant (C11NC) of the GRNC with the gra-

phene volume fraction (vg).

Fig. 6. Variation of effective elastic constant (C23NC) of the GRNC with the gra-

phene volume fraction (vg).

Fig. 7. Variation of effective elastic constant (C33NC) of the GRNC with the gra-

phene volume fraction (vg).

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graphene (with 4.5% and 20% vacancies) sheets. Considering the vo-lume fraction of graphene as 0.5, the effective properties of GRNC weredetermined using the MOM approach, as summarized in Table 2.

The mass density of the GRNC (ρnc) is calculated using the simplerules of mixture: = +( v ) ( v )nc g g m m . We have taken the values of ρgand ρm as 2200 kg/m3 and 1330 kg/m3, respectively (Yolshina et al.,2016; Odegard et al., 2005), and the calculated ρnc is 1765 kg/m3. Themagnitude of the applied uniformly distributed load on the GRNC na-noplate is taken as =q 0.050 MPa. Recent experimental studies reportedthat the flexoelectric coefficients of certain ceramics and polymers aremuch larger than the previous estimates. However, in experimentalmeasurements of certain crystals, elastomers, polymers and ceramics,the predicted flexoelectric coefficient was found to be in the range of10 10 C/m6 10 ; where e is the electron charge and a is the latticeconstant (Kogan, 1963; Ma and Cross, 2003; Nguyen et al., 2013). Forinstance, the experimentally predicted values of flexoelectric coeffi-cients of polymers are found to be in the range from 10−8 to 10−9 C/m(Chu and Salem, 2012; Jiang et al., 2013; Zhang et al., 2015). Hence,unless otherwise mentioned, we considered the flexoelectric coefficient10–9 C/m for our calculations.

5.1. Effect of flexoelectricity on static response of GRNC nanoplate

The variation of normalized bending stiffness (D /D11 110 ) of GRNC

nanoplate with respect to its thickness (h) is plotted in Fig. 11, whereD11 and D11

0 are the bending stiffnesses of GRNC nanoplate with andwithout flexoelectric effect, respectively. Note that the value of D11

depends only on the thickness of nanoplate and is independent of its in-plane dimensions, as seen from Eq. (47). Fig. 11 reveals that thebending stiffness of GRNC nanoplate with flexoelectric effect is ∼10times higher than that of the conventional nanoplate (i.e., withoutflexoelectric effect) when the value of h is 1 nm. This difference is no-ticeable and cannot be ignored for predicting the electromechanicalresponse of thin nanostructures. As the thickness of nanoplate increases,the effect of flexoelectricity starts diminishing and this finding agreewell with the results obtained by Zhou et al. (2016). From this, it can beconcluded that the stiffness of nanoplate depends on the size or shape ofnanostructure (constant or varying cross section). As expected, thenormalized bending stiffness approaches unity when the fldepends oneffect vanishes. It may also be observed from Fig. 11 that the effect offlexoelectricity on the normalized bending stiffness of GRNC nanoplateis size dependent as it can be clearly seen from the Eq. (47).

The effect of flexoelectricity on the static bending of GRNC nano-plate is examined here. Figs. 12 and 13 demonstrate the variation oftransverse deflections of SS GRNC nanoplates with and without flexo-electric effect. The dimensions of the square GRNC nanoplate are takenas: =h 4 nm, and = =a b 50 h. Our selection of in-plane dimensions ofnanoplate is based on the fact that the theory of Kirchhoff plate pro-vides better results when the aspect ratio of a plate is in the range of5–80 (Yang et al., 2015). It can be observed from Figs. 12 and 13 thatthe maximum deflection of the GRNC nanoplate occurs at its center i.e.,at =x a/2 and =y b/2 for both the cases (with and without flexo-electric effect). The maximum deflection of GRNC nanoplate increasesif its in-plane dimensions are increased (a= b= 60 h). It may also beobserved that the deflection of GRNC nanoplate with flexoelectric effectis lower than that of the conventional plate for both the cases of in-plane dimensions. In addition, Figs. 12(a) and (b) represent the 3-Drepresentation of deflection of GRNC nanoplate with and withoutflexoelectric effect. The stiffness of GRNC nanoplate significantly im-proves due to the incorporation of flexoelectric effect over that ofconventional nanoplate. These results clearly demonstrate the im-portance of flexoelectricity in the static bending of GRNC nanoplateswhich cannot be neglected at nanoscale level.

In the previous sets of results, the static response of GRNC nano-plates subjected to the UDL is studied. However, the different types ofloadings may influence the deflection behavior of nanoplates.Therefore, three different cases were considered for GRNC nanoplateunder: (i) hydrostatic load (UVL), (ii) point load, and (iii) inline load.

Fig. 8. Variation of effective piezoelectric constant (e31NC) of the GRNC with the

graphene volume fraction (vg).

Fig. 9. Variation of effective piezoelectric constant (e33NC) of the GRNC with the

graphene volume fraction (vg).

Fig. 10. Variation of effective dielectric constant ( 33NC) of the GRNC with the

graphene volume fraction (vg).

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These cases represent the practical situation of different types of load-ings applied to the thin plates. We considered the equivalent magnitudeof loading in all situations. Table 3 illustrates the effect of three types ofloading conditions on the deflection of GRNC nanoplates. As expected,the maximum deflection of the nanoplate occurs at its center irrespec-tive of the type of loading in both the cases (with and without flex-oelectricity). It is evident from this table that the consideration offlexoelectric effect results in the lowering the deflection of GRNC na-noplates compared to that of conventional plates. For example, thereduction in the static deflection of GRNC nanoplate having 4 nmthickness is found to be ∼38.0% in all the loading cases. As expected,the maximum deflection of nanoplate occurs in case of the application

of point load on it; the magnitude of maximum deflection of GRNCnanoplate observed in the following order: Point load > In-lineload > UDL > VDL.

So far, the deflection characteristics of SS GRNC nanoplate werestudied by considering its thickness as 4 nm. To explore the effect ofthickness of GRNC nanoplate on its static behavior, once again the fourdiscrete types of loading conditions are considered: UDL, VDL, inlineload, and point load. Table 4 summarizes the values of maximum de-flections of GRNC nanoplates. The reductions in static deflections ofGRNC nanoplates, irrespective of the type of loading, are found to be∼71.0%, ∼37.0%, ∼21.0%, ∼13%, and ∼9.0% corresponding to2 nm, 4 nm, 6 nm, 8 nm, and 10 nm thicknesses of nanoplate. It can be

Table 2Effective properties of GRNC (vg = 0.5).

Material C11(GPa) C12(GPa) C66(GPa) e31(C/m2) e33(C/m2) 33(F/m)

Pristine Graphene 17.853 11.876 2.988 −0.0019 0.167 7.026 × 10−11

Graphene with 4.5% vacancy 17.851 11.874 2.988 −0.0002 0.0204 7.034 × 10−11

Graphene with 20% vacancy 17.838 11.863 2.987 −0.0011 0.0910 7.029 × 10−11

Fig. 11. Effect of variation of plate thickness on the normalized bending stiff-ness (D /D )11 11

0 of GRNC nanoplate under UDL.

Fig. 12. Effect of variation of plate aspect ratios (x/a and y/b) on the deflection of GRNC nanoplate: (a) without flexoelectricity and (b) with flexoelectricity underUDL = = =h a b( 4 nm; 50 h).

Fig. 13. Effect of variation of plate aspect ratio (x/a) on the deflection of GRNCnanoplate under UDL = = =h a b( 4 nm; 50 h and 60 h).

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clearly seen that the influence of flexoelectricity on the maximum de-flection of a nanoplate diminishes as its thickness increases and tends toapproach the results of maximum deflection of the conventional GRNCnanoplate indicating that the flexoelectric effect is size dependent. It

can be concluded from the above discussion that the effect of flex-oelectricity is more prominent for thin plates and this finding agree wellwith the results obtained by other researchers (Yan and Jiang, 2012;Zhang and Jiang, 2014). In the literature, nanofabrication techniques

Table 3Effect of flexoelectricity on the central deflection of GRNC nanoplate under different loadings = = =h a b( 4 nm; 50 h).

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such as layer-by-layer assembly and dispersion method, which mainlydeal with interaction between cation and anions of adjacent graphenelayers, are commonly used to fabricate graphene-based thin films(Gamboa et al., 2010). Using these techniques, the fabrication of thingraphene-based nanocomposite film can be achieved and its thicknesson the order of nm can be tailored by varying the number of graphenelayers (Yang et al., 2013; Prolongo et al., 2014 and 2018; Tzeng et al.,2015; Prolongo et al., 2018). Some challenges are associated with thesetechniques such as in every step of LBL technique the layered graphenestructure is required to be rinsed with deionized water followed by thedrying for a specific time that may lead to error and non-uniform de-position. Mature fabrication techniques have been evolving as the ap-plications of 2D graphene sheets became more defined and thin struc-tures made of their layers are being fabricated at relatively low-cost.

Fig. 14 shows the effect of variation of plate aspect ratio (a/h) onthe maximum deflection of GRNC nanoplates for different flexoelectriccoefficients. We kept thickness of GRNC nanoplate constant to study theeffect of its aspect ratio. It can be observed from Fig. 14(c) that theflexoelectric effect is more prominent when the values of aspect ratio ofplate and flexoelectric are 40 and 10–9 C/m, respectively. When thevalue of flexoelectric coefficient is 10–10 C/m then both the cases pro-vide almost same results (Fig. 14d). On the other hand, the flexoelectriceffect on the deflection behavior of nanoplates is negligible when thevalues of flexoelectric coefficients are 10–7 C/m and 10–8 C/m (Fig. 14aand b). It can also be observed that the flexoelectricity plays an im-portant role when the in-plane dimensions of the plates are on the orderof nm. However, flexoelectricity does not much influence the staticbehavior of nanoplate when its aspect ratio is less than 30 demon-strating the strong size-dependent behavior. We considered the value offlexoelectric coefficient as 10–9 C/m to study the effect of flexoelec-tricity on the dynamic response of GRNC nanoplates.

5.2. Effect of flexoelectricity on dynamic response of GRNC nanoplate

In this section, the investigations are carried out to study the effectof flexoelectricity on the dynamic response of GRNC nanoplates.Figs. 15 illustrates the effect of flexoelectricity on the resonant fre-quency of mode (1,1) of GRNC nanoplates against the plate aspect ratio.We kept the in-plane dimensions of plates constant (a= b= 100 and150 nm) and varied their thickness. It can be observed that the resonantfrequency is higher for the flexoelectric nanoplate over that of theconventional plate when the plate thickness is less than 3 nm. Theflexoelectricity does not much influence the resonant frequencies ofnanoplates having larger thickness (>4 nm) and this is due to the factthat the effect of size dependent flexoelectricity diminishes as thethickness of nanoplate increases. This figure also reveals that the re-sonant frequency is largely depends on the in-plane dimensions of na-noplate; resonant frequency of the nanoplate diminishes as its in-planedimensions increase.

So far, the effect of flexoelectricity on the resonant frequencies of

GRNC nanoplate was studied by varying its thickness from 1 to 15(Fig. 15). Here, the parametric results of resonant frequencies of GRNCnanoplates are presented to investigate the effect of flexoelectricityconsidering the plate thicknesses as 1 nm and 2 nm. Fig. 16 demon-strates the effect of flexoelectricity on the resonant frequency of GRNCnanoplate with mode (1,1). It can be observed that the resonant fre-quency decreases as the aspect ratio of plate increases. The effect offlexoelectricity is noteworthy in case of thin plate. For instance, re-sonant frequencies of GRNC nanoplate with flexoelectricity are en-hanced by ∼225% for the plate aspect ratios of 10 to 30 when the platethickness is 1 nm. On the contrary, when the aspect ratio is sufficientlylarge, the difference between the resonant frequencies is very small,therefore the flexoelectric effect can be neglected. The results shown inFigs. 15 and 16 are significant which indicate that the flexoelectricityplays an important role in the dynamics of thin plates and needs to beaccounted properly. It is observed from Figs. 11–16 that as the thick-ness of nanostructure increases the flexoelectric effect starts dimin-ishing, and this finding agree well with the results obtained by otherresearchers (Su et al., 2018; Shi and Wang, 2019; Yang, 2019).

6. Conclusions

Static and dynamic behaviors of graphene reinforced nanocompo-site (GRNC) plates with flexoelectric effect were investigated for thefirst time in the literature. First, we determined the elastic properties ofpristine and defective graphene sheets using MD simulations and theobtained results are found in good agreement with the existing ex-perimental and numerical results. Second, we developed the mechanicsof materials (MOM) and finite element (FE) models to predict the ef-fective piezoelastic and dielectric properties of GRNC. The MOM modelwas derived using the isofield conditions and rules of mixture. Goodagreements between the MOM and FE results were obtained as long asthe graphene volume fraction is small. Finally, we derived the exactsolutions for flexoelectric GRNC nanoplate based on Kirchhoff's platetheory, Navier's solution and extended linear theory of piezoelectricity.Based on this, the static and dynamic behaviors of simply supportedGRNC nanoplates under different types of loadings were investigated tostudy the role of flexoelectricity. It is found that the bending stiffness ofnanoplates having thickness less than 5 nm increases significantly dueto the incorporation of flexoelectric effect and such effect cannot beneglected for predicting static response of thin structures. Similarly, thedynamics response of GRNC nanoplates is enhanced due to the flexo-electric effect as the plate thickness reduces. Resonant frequencies ofGRNC nanoplates are enhanced by ∼225% for the plate aspect ratios of10–30 when the plate thickness is 1 nm. Our results indicate that theflexoelectricity plays an important role in the static and dynamics be-haviors of thin plates and needs to be accounted properly while mod-eling 2D nanostructures.

Table 4Effect of flexoelectricity on the maximum deflection of GRNC nanoplate subjected to different types of loading conditions.

Thickness h (nm) Maximum deflection

UDL (nm) VDL (nm) Point load (nm) In-line load (nm)

2 with flexoelectricity 0.5155 0.2578 1.2720 0.8098w/o flexoelectricity 1.7478 0.8739 4.3125 2.7454

4 with flexoelectricity 2.1881 1.0940 5.3989 3.4370w/o flexoelectricity 3.4956 1.7478 8.6250 5.4908

6 with flexoelectricity 4.1431 2.0715 10.2226 6.5079w/o flexoelectricity 5.2434 2.6217 12.9375 8.2362

8 with flexoelectricity 6.0825 3.0412 15.0079 9.5544w/o flexoelectricity 6.9911 3.4956 17.2499 10.9816

10 with flexoelectricity 7.9763 3.9882 19.6808 12.5292w/o flexoelectricity 8.7389 4.3695 21.5624 13.7271

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Acknowledgments

This work was generously supported by the CSIR Senior ResearchFellowship awarded to the first author from the Council of Scientific &Industrial Research (CSIR) of India (141200/2K18/1).

Supplementary materials

Supplementary material associated with this article can be found, inthe online version, at doi:10.1016/j.mechmat.2019.04.006.

Fig. 14. Effect of variation of plate aspect ratio (a/h) on the maximum deflection of GRNC nanoplate, with fixed in-plane dimensions, considering differentflexoelectric coefficients: (a) 10–7 C/m (b) 10–8 C/m (c) 10–9 C/m and (d) 10–10 C/m.

Fig. 15. Effect of variation of plate thickness =h a( /x) on the resonant fre-quency of GRNC nanoplate.

Fig. 16. Effect of variation of plate aspect ratio =a( hx) on the resonant fre-quency of GRNC nanoplate =h( 1 nm and 2 nm).

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