scispace - formally typeset

Journal ArticleDOI

Effect of grain boundaries on the interfacial behaviour of graphene-polyethylene nanocomposite

15 Mar 2019-Applied Surface Science (North-Holland)-Vol. 470, pp 1085-1092

Abstract: Aim of this article was to investigate the effect of grain boundaries on the interfacial properties of bi-crystalline graphene/polyethylene based nanocomposites. Molecular dynamics based atomistic simulations were performed in conjunction with the reactive force field parameters to capture atomic interactions within graphene and polyethylene atoms, whereas non-bonded interactions were considered for the interfacial properties. Atoms at the higher energy state in bi-crystalline graphene helps in improving the interaction at the nanocomposite interphase. Geometrical imperfections such as wrinkles and ripples helps the bi-crystalline graphene in increasing the number of adhesion points between the nanofiller and matrix, which eventually improves the strength and toughness of nanocomposite. These outcomes will help in opening new opportunities for defective nanofillers in the development of nanocomposites for future applications.
Topics: Graphene (56%), Nanocomposite (52%), Grain boundary (51%)

Content maybe subject to copyright    Report

Accepted Manuscript
Full Length Article
Effect of grain boundaries on the interfacial behaviour of graphene-polyethylene
nanocomposite
Akarsh Verma, Avinash Parashar, M. Packirisamy
PII: S0169-4332(18)33297-5
DOI: https://doi.org/10.1016/j.apsusc.2018.11.218
Reference: APSUSC 41064
To appear in:
Applied Surface Science
Received Date: 24 October 2018
Revised Date: 24 November 2018
Accepted Date: 27 November 2018
Please cite this article as: A. Verma, A. Parashar, M. Packirisamy, Effect of grain boundaries on the interfacial
behaviour of graphene-polyethylene nanocomposite, Applied Surface Science (2018), doi: https://doi.org/10.1016/
j.apsusc.2018.11.218
This is a PDF file of an unedited manuscript that has been accepted for publication. As a service to our customers
we are providing this early version of the manuscript. The manuscript will undergo copyediting, typesetting, and
review of the resulting proof before it is published in its final form. Please note that during the production process
errors may be discovered which could affect the content, and all legal disclaimers that apply to the journal pertain.

*Corresponding author. E-mail: drap1fme@iitr.ac.in; Ph: +91-1332284801 (Avinash Parashar)
Effect of grain boundaries on the interfacial behaviour of graphene-
polyethylene nanocomposite
Akarsh Verma
a
, Avinash Parashar
a
* and M. Packirisamy
b
a
Department of Mechanical and Industrial Engineering, Indian Institute of Technology, Roorkee, India
b
Department of Mechanical, Industrial and Aerospace Engineering, Concordia University, Montreal, Canada
Abstract:
Aim of this article was to investigate the effect of grain boundaries on the interfacial
properties of bi-crystalline graphene/polyethylene based nanocomposites. Molecular
dynamics based atomistic simulations were performed in conjunction with the reactive force
field parameters to capture atomic interactions within graphene and polyethylene atoms,
whereas non-bonded interactions were considered for the interfacial properties. Atoms at the
higher energy state in bi-crystalline graphene helps in improving the interaction at the
nanocomposite interphase. Geometrical imperfections such as wrinkles and ripples helps the
bi-crystalline graphene in increasing the number of adhesion points between the nanofiller
and matrix, which eventually improves the strength and toughness of nanocomposite. These
outcomes will help in opening new opportunities for defective nanofillers in the development
of nanocomposites for future applications.
Keywords: Graphene, Grain boundaries, Polyethylene, Molecular dynamics, Reactive force
field, Nanocomposites

2
1. Introduction
Graphene is a two-dimensional (2D) nanomaterial with honeycomb crystal lattice domain [1,
2]. Due to exceptional mechanical, thermal and electrical properties, graphene is emerging as
a potential candidate for the reinforcement of nanocomposites [3-5]. In addition to structural
applications, graphene has wide range of application in the field of electronics [6],
biotechnology [7], desalination membrane [8], clean energy devices [9], photocatalyst [10]
and hydrogen storage [11].
In thermoplastic based nanocomposites, polyethylene (PE) is a leading matrix material with
low cost and average mechanical properties. Due to easy processability and insulating
behaviour, PE based composites are used for the manufacturing of armour materials, pipes,
packaging and also as biomaterial [12, 13]. Higher content of hydrogen (the element with
lowest atomic mass) in PE also helps in extending its application to space structures and for
radiation shielding [14, 15]. Molecular chain structure of PE contains both amorphous as well
as crystalline structure, which governs the increment in mechanical stiffness and flexibility
[13, 15]. These atomistic scale phenomena cannot be easily captured by conventional
experimental techniques. Atomistic modelling techniques such as molecular dynamics (MD)
have proved to be viable in simulating the nanoscale dynamics of intricate PE structure [16,
17].
Several computational studies on graphene/PE nanocomposites have already been reported in
the literature [18-26]. Jin et al. [24] revealed enhancement in interfacial mechanical
properties of functionalised graphene and PE based nanocomposite. They attributed higher
interfacial strength for relatively stronger covalent bonds formed by the functional groups as
compared to weak non-bonded van der Waals interactions. Li et al. [27, 28] reported that the
Stone-Thrower-Wales (STW) defects also helps in enhancing the interfacial shear strength

3
and thermal conductivity between defected graphene and epoxy. Ma et al. [29] chemically
functionalised the graphene with 4,4-diaminophenylsulfone and studied the mechanical and
fracture behaviour of epoxy based nanocomposite. Their simulations predicted that the
functionalised interface helps in improving young’s modulus and fracture release rate by
47.7% and 84.6%, respectively. Lv et al. [30] also captured the effect of chemical
functionalisation of interface between graphene/PE nanocomposite. They reported an overall
enhancement in the bonding energy and shear stress for the nanocomposite system. Ding et
al. [31] predicted a superior interfacial strength for graphene oxide based nanocomposites, as
compared to pristine form of graphene. Ramanathan et al. [32] experimentally described the
positive impact of functionalised graphene sheets on the mechanical and thermal behaviour of
poly(methyl methacrylate) composite. Liu et al. [33] concluded in their work that grafting of
graphene with polymer chains helps in improving the shear strength as well as graphene’s
dispersion in the polymer matrix. Recently in 2018, Rajesh and Avinash [12] performed
atomistic simulations to study the effect of defective h-BN nanosheets on the PE based
nanocomposites. An overall improvement in the interfacial strength as well as mechanical
properties of h-BN/PE nanocomposite was predicted in their computational work. Due to
limitations associated with the synthesising techniques, nanomaterials e.g. large size
graphene nanosheets are synthesised with geometrical defects such as vacancies, dislocations
and grain boundaries (GB) [34, 35]. Scanning tunneling microscopy and transmission
electron microscopy based experimental characterization of polycrystalline graphene reveals
that GB configuration is composed of pentagon-heptagon (57) rings [36, 37]. Several
computational and experimental works have already been performed to characterize the
mechanical properties of bi-crystalline graphene [38-42]. Xu et al. [38] predicted decline in
the mechanical properties of bi-crystalline graphene as compared to pristine counterpart.
Yang et al. [39] and Grantab et al. [40] employed the MD based atomistic simulations to

4
predict the brittle behavior of bi-crystalline graphene configurations. Recently, our research
with oxidized bi-crystalline graphene nanosheets have predicted a shift in the failure
morphology from brittle to ductile with specific spatial distribution of oxide groups [41, 42].
So far, research was mostly focused on using either pristine or chemically functionalised
graphene for the reinforcement of polymer based nanocomposites. But, larger size nanosheets
are considered as a better reinforcement for the nanocomposites. Chemical vapour deposition
is the most commonly used technique for synthesising larger size graphene, but it results in
polycrystalline structure. Literature is almost mute on the effect of grain boundaries on the
reinforcing capabilities of graphene for polymer based nanocomposites. So taking this as our
motivation and in order to fulfil this literature gap, herein this article, the authors have
attempted to elucidate the role of GB in graphene domain on the interfacial bonding
characteristics.
2. Modelling details
In this study, the classical mechanics based MD approach was used to perform all the
simulations. In order to capture the interatomic interactions between carbon in graphene and
carbon and hydrogen atoms in PE, reactive force field (ReaxFF) parameters proposed by
Chenoweth et al. [43] has been used; whereas, for the cross or interfacial (van der Waals)
interactions between graphene and PE, Lennard-Jones (LJ) potential parameters (refer Table
1) were employed from the literature work [44-46].

Citations
More filters

Steven J. Plimpton1Institutions (1)
01 May 1993-
TL;DR: Comparing the results to the fastest reported vectorized Cray Y-MP and C90 algorithm shows that the current generation of parallel machines is competitive with conventional vector supercomputers even for small problems.
Abstract: Three parallel algorithms for classical molecular dynamics are presented. The first assigns each processor a fixed subset of atoms; the second assigns each a fixed subset of inter-atomic forces to compute; the third assigns each a fixed spatial region. The algorithms are suitable for molecular dynamics models which can be difficult to parallelize efficiently—those with short-range forces where the neighbors of each atom change rapidly. They can be implemented on any distributed-memory parallel machine which allows for message-passing of data between independently executing processors. The algorithms are tested on a standard Lennard-Jones benchmark problem for system sizes ranging from 500 to 100,000,000 atoms on several parallel supercomputers--the nCUBE 2, Intel iPSC/860 and Paragon, and Cray T3D. Comparing the results to the fastest reported vectorized Cray Y-MP and C90 algorithm shows that the current generation of parallel machines is competitive with conventional vector supercomputers even for small problems. For large problems, the spatial algorithm achieves parallel efficiencies of 90% and a 1840-node Intel Paragon performs up to 165 faster than a single Cray C9O processor. Trade-offs between the three algorithms and guidelines for adapting them to more complex molecular dynamics simulations are also discussed.

24,496 citations


Journal Article
Abstract: This paper is concerned with the interfacial thermal resistance for polymer composites reinforced by various covalently functionalised graphene. By using molecular dynamics simulations, the obtained results show that the covalent functionalisation in graphene plays a significant role in reducing the graphene-paraffin interfacial thermal resistance. This reduction is dependent on the coverage and type of functional groups. Among the various functional groups, butyl is found to be the most effective in reducing the interfacial thermal resistance, followed by methyl, phenyl and formyl. The other functional groups under consideration such as carboxyl, hydroxyl and amines are found to produce negligible reduction in the interfacial thermal resistance. For multilayer graphene with a layer number up to four, the interfacial thermal resistance is insensitive to the layer number. The effects of the different functional groups and the layer number on the interfacial thermal resistance are also elaborated using the vibrational density of states of the graphene and the paraffin matrix. The present findings provide useful guidelines in the application of functionalised graphene for practical thermal management.

86 citations



Journal ArticleDOI
Bharat Sharma1, Avinash Parashar1Institutions (1)
Abstract: Due to outstanding properties, graphene and h-BN nanosheets are emerging as a potential candidate for wide spectrum of applications in the field of engineering and bio-medical science. Graphene and...

29 citations


Journal ArticleDOI
Abstract: In this article, experimental and classical mechanics-based approaches have been used to study the reinforcing capabilities of hexagonal boron nitride (h-BN) nanosheets for polyethylene (PE)-based nanocomposites. Experiments were performed with h-BN nanoflakes and high-density polyethylene-based nanocomposites. Experimental results reported 27.0 and 64.1% improvement in tensile strength and Young’s modulus for 5 wt % h-BN loading in PE, respectively. Experimental analysis helps in developing a micro- and macrolevel understanding of the mechanical behavior of BN/PE nanocomposites, whereas the strength of these nanocomposites is governed by interfacial properties. Interfacial properties can be easily captured using atomistic simulations such as molecular dynamics. Molecular dynamics-based atomistic models were developed to study the effect of aspect ratio, weight fraction, morphology, distribution of h-BN nanosheets, and strain rate loading on mechanical properties of the nanocomposite. A reactive force fie...

22 citations


References
More filters

Journal ArticleDOI
Steven J. Plimpton1Institutions (1)
Abstract: Three parallel algorithms for classical molecular dynamics are presented. The first assigns each processor a fixed subset of atoms; the second assigns each a fixed subset of inter-atomic forces to compute; the third assigns each a fixed spatial region. The algorithms are suitable for molecular dynamics models which can be difficult to parallelize efficiently—those with short-range forces where the neighbors of each atom change rapidly. They can be implemented on any distributed-memory parallel machine which allows for message-passing of data between independently executing processors. The algorithms are tested on a standard Lennard-Jones benchmark problem for system sizes ranging from 500 to 100,000,000 atoms on several parallel supercomputers--the nCUBE 2, Intel iPSC/860 and Paragon, and Cray T3D. Comparing the results to the fastest reported vectorized Cray Y-MP and C90 algorithm shows that the current generation of parallel machines is competitive with conventional vector supercomputers even for small problems. For large problems, the spatial algorithm achieves parallel efficiencies of 90% and a 1840-node Intel Paragon performs up to 165 faster than a single Cray C9O processor. Trade-offs between the three algorithms and guidelines for adapting them to more complex molecular dynamics simulations are also discussed.

26,738 citations


Steven J. Plimpton1Institutions (1)
01 May 1993-
TL;DR: Comparing the results to the fastest reported vectorized Cray Y-MP and C90 algorithm shows that the current generation of parallel machines is competitive with conventional vector supercomputers even for small problems.
Abstract: Three parallel algorithms for classical molecular dynamics are presented. The first assigns each processor a fixed subset of atoms; the second assigns each a fixed subset of inter-atomic forces to compute; the third assigns each a fixed spatial region. The algorithms are suitable for molecular dynamics models which can be difficult to parallelize efficiently—those with short-range forces where the neighbors of each atom change rapidly. They can be implemented on any distributed-memory parallel machine which allows for message-passing of data between independently executing processors. The algorithms are tested on a standard Lennard-Jones benchmark problem for system sizes ranging from 500 to 100,000,000 atoms on several parallel supercomputers--the nCUBE 2, Intel iPSC/860 and Paragon, and Cray T3D. Comparing the results to the fastest reported vectorized Cray Y-MP and C90 algorithm shows that the current generation of parallel machines is competitive with conventional vector supercomputers even for small problems. For large problems, the spatial algorithm achieves parallel efficiencies of 90% and a 1840-node Intel Paragon performs up to 165 faster than a single Cray C9O processor. Trade-offs between the three algorithms and guidelines for adapting them to more complex molecular dynamics simulations are also discussed.

24,496 citations


Journal ArticleDOI
Andre K. Geim1Institutions (1)
19 Jun 2009-Science
TL;DR: This review analyzes recent trends in graphene research and applications, and attempts to identify future directions in which the field is likely to develop.
Abstract: Graphene is a wonder material with many superlatives to its name. It is the thinnest known material in the universe and the strongest ever measured. Its charge carriers exhibit giant intrinsic mobility, have zero effective mass, and can travel for micrometers without scattering at room temperature. Graphene can sustain current densities six orders of magnitude higher than that of copper, shows record thermal conductivity and stiffness, is impermeable to gases, and reconciles such conflicting qualities as brittleness and ductility. Electron transport in graphene is described by a Dirac-like equation, which allows the investigation of relativistic quantum phenomena in a benchtop experiment. This review analyzes recent trends in graphene research and applications, and attempts to identify future directions in which the field is likely to develop.

10,893 citations


Journal ArticleDOI
Yanwu Zhu1, Shanthi Murali1, Weiwei Cai1, Xuesong Li1  +3 moreInstitutions (1)
15 Sep 2010-Advanced Materials
TL;DR: An overview of the synthesis, properties, and applications of graphene and related materials (primarily, graphite oxide and its colloidal suspensions and materials made from them), from a materials science perspective.
Abstract: There is intense interest in graphene in fields such as physics, chemistry, and materials science, among others. Interest in graphene's exceptional physical properties, chemical tunability, and potential for applications has generated thousands of publications and an accelerating pace of research, making review of such research timely. Here is an overview of the synthesis, properties, and applications of graphene and related materials (primarily, graphite oxide and its colloidal suspensions and materials made from them), from a materials science perspective.

7,753 citations


Journal ArticleDOI
11 Oct 2012-Nature
TL;DR: This work reviews recent progress in graphene research and in the development of production methods, and critically analyse the feasibility of various graphene applications.
Abstract: Recent years have witnessed many breakthroughs in research on graphene (the first two-dimensional atomic crystal) as well as a significant advance in the mass production of this material. This one-atom-thick fabric of carbon uniquely combines extreme mechanical strength, exceptionally high electronic and thermal conductivities, impermeability to gases, as well as many other supreme properties, all of which make it highly attractive for numerous applications. Here we review recent progress in graphene research and in the development of production methods, and critically analyse the feasibility of various graphene applications.

6,902 citations


Performance
Metrics
No. of citations received by the Paper in previous years
YearCitations
20221
202114
20208
20195
20151
19931