Application of Cold Plasma in Nanofillers Surface Modification For Enhancement of Insulation Characteristics of Polymer Nanocomposites: A Review

This article has been accepted for publication in a future issue of this journal, but has not been
fully edited. Content may change prior to final publication. Citation information: DOI
10.1109/ACCESS.2021.3085204, IEEE Access
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Application of Cold Plasma in Nanofillers

Surface Modification for Enhancement of
Insulation Characteristics of Polymer
Nanocomposites: A Review
N M Saman1, M H Ahmad1 and Z Buntat1
1
Institute of High Voltage and High Current (IVAT), School of Electrical Engineering, Faculty of Engineering, Universiti Teknologi Malaysia, Johor
Bahru, Johor, 81310 Malaysia.
Corresponding author: M H Ahmad (e-mail: [email protected]).

"The authors would like to acknowledge Universiti Teknologi Malaysia and Sriwijaya University for providing research grants; 01M73, 16J61, 4B383,
07G05, 04G81, 4B377, 4B340, 4B341, and 4B342. "
ABSTRACT Polymer nanocomposites have gained much attention among researchers due to their
excellent characteristics, such as high thermal resistivity and the ability to withstand higher electrical stress.
Introducing nanoparticles into the polymer matrix can further improve the insulation characteristics.
However, the effectiveness of nanocomposite polymer to suppress an electrical tree, enhancing the partial
discharge, and increase the breakdown strength is still a question mark due to the agglomeration issue of
nanoparticles, which causing the nanoparticle to be dispersed non-uniformly within the polymer matrix.
Plasma treatment is one of the methods that potentially replace conventional modification techniques such
as chemical functionalization and heat treatment to improve the dispersion of nanoparticles, nanocomposite
bonding, and the compatibility between polymer-nanoparticle interfaces. By altering the surface of
nanoparticles using cold plasma with a glow discharge mechanism, the surface morphology of
nanoparticles can be modified in terms of chemical structure, which indirectly solves the nanoparticle
agglomeration. This study presents a review on the application of cold plasma in surface modification to
enhance insulation characteristics of nanocomposite polymers. Various polymer hosts combined with
different untreated and plasma-treated nanofillers are also reviewed. The trends on nanomaterial surface
modification using the cold plasma technique based on its operating pressure to improve the dielectric
properties of nanocomposite polymers are also discussed accordingly.
INDEX TERMS Cold plasma, nanofillers surface modification, nanocomposites polymer, and plasma
treatment.
I. INTRODUCTION discharge resistance, and increase the dielectric breakdown

Recently, multiple studies and research of nanocomposites strength.
polymer have been conducted among the researchers to Nowadays, nanoparticles have become the size of choice
obtain the most usable and high-quality insulation medium for composites filler as they promise enhancement of the
for high and medium voltage application. insulator’s properties, and less amount is needed compared
Nanocomposites polymer combines a polymer matrix to micro-particles used in micro composites. Besides,
and inclusions with at least one dimension such as length, nanocomposites also exhibit better mechanical, electrical,
width, or/and thickness in the nano-meter size range known and thermal properties than micro composites [4][5].
as nanofillers [1]-[3]. Previously, micrometre size particles Based on previous research, the type of nanofiller used
have been employed by several researchers to be used as an has been varied in terms of material, quantity, and
additive material that combined with a pure polymer to mechanism of surface modification to obtain different
improve the quality of insulator in several aspects such as levels of electrical properties improvement. On the other
to suppress an electrical tree prolongation, enhance partial hand, several types of polymer host are generally used as a
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subject in the study of nanocomposites such as low-density Heat treatment is also used to alter the surface
polyethylene, high-density polyethylene, cross-linked morphology by drying the water molecule and moisture on
polyethylene, polypropylene, silicon rubber, and epoxy the nanofillers. The justification of this technique is to
resin. reduce the hydrogen and hydroxide ions on the surface of
However, nanofiller surfaces and polymer matrix the nanofiller to decrease the local electric field. This is
compatibility is the main issue due to the agglomeration of because hydrogen and hydroxide ions have higher
nanofiller [6]-[9]. Agglomeration of nanofiller formed due conductivity which may degrade the insulation
to the coarse accumulation of nanoparticles has affected the characteristics of nanocomposite polymers [25]. However,
homogeneity of nanoparticles dispersed within the polymer this technique has a drawback that can damage the
matrix. The dispersion of nanofiller into polymer matrices nanofiller’s surface structure, especially when the amount
became non-uniform due to the agglomeration of of heat exposed onto the nanofiller exceeding the minimum
nanofillers [10]-[14]. Uniform and homogenous dispersion amount of heat can be withstood by the nanofiller. Thus,
of nanofillers are crucial in enhancing nanocomposite cold plasma treatment seems to provide effective surface
polymers’ insulation characteristics such as dielectric modification on the nanofiller by providing a self-repelling
permittivity, space charge, direct current conductivity, process to overcome the agglomeration of nanofiller and
dielectric losses, partial discharge resistance, dielectric increase the hydrophilicity of nanofiller to enhance the
breakdown strength, and electrical tree endurance. dispersion uniformity.
In addition, the uniform dispersion of nanofillers into Besides, cold plasma can also provide anchoring sites to
polymer matrices is also influenced by the surface enable covalent bonds between the organic and inorganic
characteristic of nanoparticles. Numerous comprehensive phases [26]-[29]. The insulation characteristics of
studies have revealed that uniform dispersion can be nanocomposite polymers can be further improved by
achieved by increasing the surface hydrophilicity of the obtaining uniform and homogenous nanofiller dispersion in
nanoparticle [15]-[17]. Meanwhile, functionalizing a polymer matrices. Therefore, plasma treatment promises a
specific functional group such as carbonyl and carboxyl reliable result in improving the insulation characteristics by
onto the nanoparticle’s surface could increase the reducing nanofiller agglomeration, functionalizing certain
hydrophilicity of the nanoparticle, which leads to obtaining compatible functional groups, and strengthening the
better uniformity of dispersion. interfacial bonds.
Furthermore, the insulation characteristics of This paper reports a review on the application of cold
nanocomposite polymers are also influenced by the plasma treatment in nanofiller surface modification and the
characteristics of interfacial regions between organic and significant improvement of the insulation characteristics of
inorganic compounds. Other than uniformity of dispersion, nanocomposite polymer filled with plasma-treated
interfacial bonds’ strength is also the crucial factor in nanoparticles. The effectiveness of cold plasma treatment has
enhancing the insulation characteristics [18]-[20]. also been pointed out to give an overview sentiment for
Preparation of nanocomposite polymer by using a direct future study.
mixing process without introducing surface modification This scientific review began by describing the composition
technique might result in the formation of weak interfacial of polymer nanocomposites. The constituents, physical,
bonds and small deep trap sites, limiting the ability of chemical structures of the nanocomposites are also
organic-inorganic nanocomposites to suppress the space
dismantled to deliver the basic concept of nano-composition.
charge [21]-[24]. Thus, the insulation characteristics did not
Also, the classification of nanocomposites material based on
experience significant improvement compared to the pure
its natural characteristics of the compound has been
host polymer.
The study on surface modification techniques has been described with an appropriate example of each listed class.
intensively conducted since a few decades ago. The main The classification contents are structured in general so that a
purpose of those studies is to enhance the insulation clear picture of the potential of nanocomposites with
characteristics by overcoming the agglomeration issue, different classes, including their areas of application, can be
increase the hydrophilicity of nanofiller surfaces, and distinguished and explained in detail.
strengthen the interfacial bonds. Surface modification can This paper has been organized to describe the
be categorized into three techniques: chemical treatment, performances of dielectric insulations nanocomposites. In
heat treatment, and plasma treatment. Chemical treatment is detail, the performance of nanocomposites was discussed
the technique that uses chemical agents and/or solvents to according to the previous collective studies related to the
functionalize certain chemical functional groups on the investigation of electrical treeing prolongation, partial
nanofiller surfaces since chemical treatment required discharge endurance, and dielectric breakdown strength since
chemical solvent, which was difficult to be decomposed these properties are required to be considered in designing a
and toxicity in some cases. Thus, the trend of surface good insulation medium. The current limitation of the surface
modification study was shifted to heat and plasma modification technique was also included in this review’s
treatment. structure, which explains the limitation of chemical
functionalization and heat treatment technique in developing FIGURE 1. Composition of nanocomposites polymer.
effectively treated nanocomposites insulating materials.

The limitation of cold plasma treatment was also critically Generally, nanocomposites polymers have three main
constituents: polymer matrix, nanofiller, and interaction
reviewed at the culmination of this review based on
zone, as shown in Fig. 2. These three constituents are
justifications and claims made in the previous studies. The
required to be considered to understand the structure of
concept of cold plasma was also discussed as the main topic
polymer nanocomposites. Commonly, the nanofillers used
distinguished according to the operating condition of the to disperse into a polymer matrix consist of higher relative
plasma production. Besides, the effectiveness of cold plasma permittivity than the matrix substrate [32]. Besides, the
treatment as a surface modification technique to enhance interaction zone between the polymer matrix and
insulation properties of the nanocomposites was also nanofillers plays an important role in polymer property
presented so that the recent performance of cold plasma enhancement. Nanofillers also act as a barrier to the
treatment can be criticized scientifically. vibration of the polymer chain [33][34].
The critical review of the nanocomposites has been Theoretically, the polymer chains will vibrate when the
summarized in the table to determine the trend of research electrical stress is applied to the polymer insulation. The
regarding the insulation properties developed by using cold rapid vibration of polymer chains will initiate the sliding
plasma treatment concerning the technique of surface motion of chains, which causes the polymer chains to
modification. The climax of this review highlights the major collapse and excite the electron avalanche to form across
challenges and future directions of cold plasma as an points where electrical stress is applied. Introducing
intensive technique in enhancing the insulation properties of nanofiller into polymer matrices is a comprehensive
polymer nanocomposites. technique to reduce the vibration of polymer chains and
obtain better stability of polymer chains.
II. NANOCOMPOSITES POLYMER Besides, nanofillers also work as a barrier to the injection
of space charge to decrease the local electric field
A. CONSTITUENTS OF NANOCOMPOSITES POLYMER distortion. However, nanofillers’ compatibility and polymer
Particularly, nanocomposites polymers have received much matrix are crucial for obtaining a well and homogeneous
attention due to the addition of inorganic nanoparticles to nanofiller dispersion into the polymer matrix. Thus,
develop insulation materials with tailored properties. A multiple surface modification techniques have been
nanocomposite polymer is a composition that is formed by introduced to produce the most effective interaction zone,
dispersing a certain amount of nanometer-sized fillers within directly achieving a certain improvement level.
a polymer matrix [1]-[3][30][31]. Fig. 1 illustrates the basic
composition of nanocomposite polymers. The size of the
nanofiller is normally from a few nanometers to 100 nm. The
amount of the nanofiller distributed within the polymer
matrix can be determined based on a measurement parameter
known as weight percentages (wt%). Different amounts of
nanofiller (weight percentage) used will produce different
outcomes and change the properties of the nanocomposites.
The main purpose of introducing nanofiller into polymer
matrices is to enhance the insulation characteristics of
polymers [21][22][30][31]. The insulation characteristics
promoted to be enhanced including dielectric breakdown
strength, partial discharge resistance, dielectric losses,
electrical tree prolongation, and thermal conductivity.
FIGURE 2. Constituents of nanocomposites polymer [35].
B. PHYSICAL STRUCTURE OF NANOFILLERS

Nanofillers are essential in determining the physical
properties of nanocomposites polymers because they increase
the molecular weight and limit the translational motions of
the chains to each other [33]-[35].
Newly, the study on the type of nanofiller made from
various materials has been intensively conducted among
researchers worldwide to obtain the most effective
nanofiller that can be used to form high-quality
nanocomposites polymers. Generally, nanoparticles can be
classified based on their dimension: zero-dimensional, one-
3
dimensional, two-dimensional, or three-dimensional [36]. In contrast, graphene consists of a hexagonal

The illustration of nanofiller into those different dimensions arrangement of a single atomic thick sheet, in which the
is shown in Fig. 3. carbon atoms are covalently sp2-bonded [43]. The primitive
graphene cell comprises two non-equivalent atoms, and
these two sub-lattices are translated from each other with
1.44 Å of carbons distance [42]. The preparation of
graphene can be classified into several chemical
intercalated graphite methods by using thermal expansion
technique, the exfoliation of graphite using a
micromechanical process, deposition of chemical vapour,
FIGURE 3. Classification of nanofiller (a) zero-dimensional, (b) one- and chemical reduction of graphene oxide [44].
dimensional, (c) two-dimensional, (d) three-dimensional (nano-meter
sized of fillers which are less than 100 nm).
Nanoclays are also one of the types of nanofiller usually
used to be filled into the polymer matrix. Generally,
In zero-dimensional (0D) nanomaterials, all dimensions nanoclays are produced from layered silicates or mineral
are measured within the nanoscale (no dimensions are clays with traces of metal oxides and an organic compound.
larger than 100 nm). Most commonly, 0D nanomaterials are Hydrous aluminium phyllosilicates are a common type of
nanoparticles [36]. The characteristic of a one-dimensional clay mineral used as nanofillers with various iron, alkali
(1D) nanofiller refers typically to the thin platelet or metals, alkaline earth, magnesium, and other cations [45].
lamellar particles. Besides, two-dimensional (2D) nanofiller Montmorillonite, saponite, laponite, hectorite, sepiolite, and
are represented as rod or/and whisker particles, while vermiculite are examples of nanoclays that are often used
organic oxides in rectangular or spherical shapes can be comprehensively [45]. Montmorillonite (MMT) consists of
classified into three-dimensional (3D) nanofiller. an alumina octahedral sheet flanked by two layers of
As defined, the nanofillers added to the polymer matrices tetrahedral silica sheets, in which hydrated exchangeable
are very small in terms of quantity which is less than ten wt% cations occupy the spaces between the lattices. Regular van
compared to conventional microcomposites which, contain der Waals gap, known as an interlayer or gallery, is formed
50 wt% of micro fillers [4][5][37][38]. Thus, nanocomposites due to the stacking of clay layers. The isomorphic
polymer becomes selective due to the small quantity of substitution within the layers produced negative charges
nanofillers needed to obtain better properties enhancement counterbalanced by the earth alkaline and alkali cations
than micro composites. located inside the interlayers. The level of the negative
charge of the nanoclay is characterized according to the
C. CHEMICAL STRUCTURE OF NANOFILLERS capacity exchange of cation [46].
Chemically, nanofillers can be categorized according to the Porous and hollow nanoparticles also another type of
chemical identities of the compound. In general, the nanofillers that have been chosen to be dispersed into the
category of nanofillers consists of carbon-based nanofillers, polymer matrix to enhance the properties of nanocomposite
layered nanoclays, porous and hollow nanoparticles, polymers. Halloysite nanotube is a hollow micro and nano-
nanocellulose, and nanoparticles of metallic alloys. Carbon tubular structure of aluminosilicate [47]. Structurally,
nanotubes and graphene are among the types of carbon- halloysite nanotube more likely to the kaolinite, which
based nanofillers that are often used to be dispersed to form weakly held and led the intercalation of water molecules
comprehensive nanocomposite polymers. Carbon nanotubes monolayer. It is composed of SiO4 tetrahedral sheets with
consist of carbon fibres with nano-meter sized of diameter the shared edge of AlO6 octahedral sheets. Thus, the
and micro-meter sized of length. The structure of carbon chemical composition of the halloysite nanotube is almost
nanotubes consists of an enrolled graphitic sheet formed like nanoclays, while the geometry of the nanotubular is
through the planar-hexagonal arrangement of carbon atoms almost similar to carbon nanotubes. Halloysite nanotube
distributed in a honeycomb-like lattice [39]. tubularly formed with the nano-meter scale of diameter and
Carbon nanotubes can be classified depending on their micro-meter scale of length. Zeolite is a faujasite-type
preparation method. The classification of carbon nanotubes framework of aluminosilicate with 1.3 nm of cavities
is either single-walled carbon nanotube or multi-walled diameter interconnected to the 0.74 nm of pores. The cubic
carbon nanotube [40]. Single-walled carbon nanotube forms cell of the aluminosilicates unit is composed of 192 (Si,
by rolling up a single graphene layer into a seamless Al)O4 tetrahedrons [48]. Usually, only the large surface
cylinder [41]. In contrast, multi-walled carbon nanotube area of internal micro-porous of zeolites is considered,
forms by arranging two or more concentric cylindrical while the external surface area of micrometre-sized zeolites
shells of graphene sheets coaxially around a central hollow is neglected to design nanocomposite polymers [49].
core. The properties of both classes of carbon nanotubes Nanocellulose is a cellulose-derived material with at least
exhibit a strong covalent bond between carbon atoms and one of its dimensions in the nano-meter scale. Recently,
their arrangement in cylindrical nanostructures [42]. nano-cellulose has been listed as a comprehensive new bio-
4
nanomaterial to fill into a polymer matrix, which promises mechanical, and thermal properties. However, the prevalent
a significant enhancement in insulating properties. The acid issue that arises is the inappropriate nanofiller dispersion,
hydrolysis process is the key to form monocrystals which stifled the improvement of these properties. For
cellulose by isolating the crystalline cellulosic regions [50]. instance, carbon nanotubes are one of the nanoparticles that
Nanocellulose can be categorized into two chemical difficult to be dispersed into polymer matrices. The
identities such as nanofibril and nanocrystal celluloses. agglomeration of carbon nanotubes during the low
Nanofibrils can be produced by applying the mechanical polymer/carbon nanotube preparation process causes the
shearing force to a cellulosic fibre slurry. This process is interaction between both materials to become weaker [54].
called the de-structuration strategy. Generally, the Thus, this clearly proved that the processing technique and
mechanically induced de-structuration strategy is conditions influencing the dispersion state of carbon
implemented using different shearing equipment such as nanotubes within polymer matrices. Therefore, the state of
homogenizer, microfluidizer, or ultra-fine friction grinder. carbon nanotubes required to be modified to functionalize
Nano-fibrillated cellulose is usually obtained as an aqueous certain chemical functional groups. This indirectly able to
suspension [51]. The width of nano-fibrillated cellulose is improve interfacial interaction [54] [55].
lying up to 100 nm with higher than one μm of the length The chemical reactivity between the carbon nanotubes
depends on some factors such as the source of cellulose, and polymer matrix is increased by coating the chemical
defibrillation, and pre-treatment process [52]. functional group on the surface of carbon nanotubes. Thus,
In contrast, nano-crystallized cellulose is produced by the functionalized carbon nanotubes produced better
applying a controlled strong acid hydrolysis treatment interface regions, consequently forming a better self-
process to cellulosic fibres. This process will cause the mechanism of load transfer from the polymer matrix to the
dissolution of amorphous domains and longitudinally functionalized carbon nanotubes [42]. Chemical surface
cutting the microfibrils. Thus, this process is known as the functionalization is a comprehensive technique
chemically induced de-structuration strategy. Nano- implemented using nitric and sulfuric acids (HNO3/H2SO4).
crystallized cellulose was also obtained as an aqueous This is a promising technique to functionalize carboxylic
suspension [52]. Commonly, the nano-crystallized cellulose acid groups (-COOH) on the surface of carbon nanotubes
tends to form rod-like nanocrystals or also known as [42]. As a result, functionalizing carboxylic acid groups on
whiskers. The geometrical dimension of nano-crystallized carbon nanotubes surfaces can alter the surface nature of
cellulose is affected by the source of cellulose and its carbon nanotubes, creating significant compatibility
conditions of hydrolysis. The production of nano- between carbon nanotube and the polymer matrix [56].
crystallized cellulose can be prepared from sulfuric acid. In improving the insulation properties of nanocomposite
This process usually will form a sulphate functional group polymers, the employment of secondary particles such as
with negatively charged on the surface of nano-crystallized clay is also another technique used intensively to achieve
cellulose. The average length and width of nano- better dispersion of carbon nanotubes within polymer
crystallized cellulose dimensionally up to a few nanometers matrices [55]. Besides, instead of using a single type of
[52]. In the selection procedure of nanoparticles, the ratio of polymer matrix, introducing blending polymer/polymer as a
the length to the width of nano-crystallized cellulose being matrix also exhibits an excellent agreement to enhance the
the crucial parameter required to be considered to obtain a dispersion of carbon nanotubes. Polymer/polymer blends
high surface area reaction [51]. with carbon nanotubes have been observed to have better
Recently, the capability of metal hydrides alloys to electrical and thermal properties compared to unfilled
enhance the properties of nanocomposite polymers has polymer/polymer blends [57]. The strength of electrical
caused this type of nanofiller intensively used. The reversibly conductivity will be changed abruptly depending on the
chemical reaction between metal hydrides alloys and distribution and dispersion of carbon nanotubes within the
hydrogen causes this type of nanofiller to be utilized in the polymer matrix due to the formation of a three-dimensional
solid-state storage of the gas. Metal hydrides alloys subjected network of dispersed carbon nanotubes.
to repeated hydride/dehydration cycles suffer from a Literally, the electrical conductivity of nanocomposite
pulverization phenomenon caused by a significant difference polymers depends on the concentration of nanofillers. At
between hydride and the metallic compound [53]. Thus, the critical concentration of nanofiller, the electrical
repeated hydrogen loading/unloading cycles produce free conductivity of the nanocomposite polymers is increased,
metal powder particles on a nanometric scale. surprisingly. This critical concentration of nanofiller is also
inferred from the limit of the electrical percolation state.
D. CHEMICAL AND PHYSICAL COMPOSITION OF However, the further increases of carbon nanotubes
NANOFILLERS ON INSULATION CHARACTERISTICS dispersed within the polymer matrix exceed the critical
The incorporation of nanoparticles into polymer matrices concentration will cause a moderate increase in electrical
has been explored as a strategy to produce nanocomposite conductivity [56] [57]. The amount of carbon nanotubes
materials with the superior enhancement of electrical, required to achieve an electrical percolation state for
5
polymer/polymer blends usually less than the amount of barrier with only a small volume fraction of nanoparticles
carbon nanotubes needed to obtain the same state with a required [62]. Layered Nanoclays have proven effective in
single polymer matrix. However, the region where the reinforcing fillers for a single or blend polymer because of
carbon nanotubes are dispersed must be selectively in the their lamellar structure and high surface area with 750 m2g-1
matrix phase or between the polymer/polymer blend [58]. [63]. Generally, smectite clays or layered silicates have
The double phenomenon of electrical percolation can be been chosen to be dispersed into the polymer matrix due to
achieved by forming the polymer/polymer blend their superior properties such as swell, high cation
nanocomposites with co-continuous morphology. exchange capacities, and cost-effectiveness. Besides,
Collectively, the concentration of carbon nanotubes and the montmorillonite is another example of layered nanoclay
final morphology of the polymer/polymer blends are crucial that is intensively used to fill into the polymer matrix due to
factors to the limit of the electrical percolation state. Both this nanofiller’s beneficial properties, such as high surface
factors significantly act as a function of the nano- and reactive area chemically well-known intercalation or
composition, determination of processing conditions, and exfoliation process, and high availability potential [64].
compatibilizer steps [57]. Naturally, the surface morphology of montmorillonite is
One factor that drives graphene has been used intensively hydrophilic, while characteristic most of the polymers tend
as a nanofiller to be dispersed within the polymer matrix is to be hydrophobic. As a result, the dispersing process of
the extremely high surface area with 2630 m2g-1 [59]. montmorillonite into the polymer matrix is mismatched or
Besides, graphene is also a promising carbon-based incompatible, cause the nanofiller to agglomerate.
nanofiller due to the high thermal and electrical Therefore, the surface modification technique must be done
conductivity, such as 5000 Wm-1 and 6000 Scm-1, on the montmorillonite to form organophilic characteristics
respectively [59]. The nature of graphene with gas of nanoclay, which may improve the compatibility of
impermeability is also why this type of carbon-based nanocomposites mixture. Regularly, the surface
nanofiller has been chosen to improve the insulation modification technique executed to alter the surface
properties of the polymer. These properties are the primary morphology of layered nanoclays is the cations exchanging
consideration because graphene’s overall factors greatly process in the interaction regions by using alkylammonium
enhance the mechanical, electrical, thermal, and gas barrier or alkyl-phosphonium salts as dioctadecyl dimethyl
properties of polymer nanocomposites [59]. ammonium bromide. The exchange of inorganic cations
Chemically, graphene’s effectiveness as a nanofiller with organic ions on the surface galleries of layered
depends on the exfoliation process of bulk graphite to be nanoclays effectively extends the nanoclays exterior
translated into specific single sheets. The preparation corridor. As a result, the layered nanoclays will be
process of individual exfoliated graphene sheets can be intercalated easily into the polymer chains.
categorized into chemical and mechanical techniques such In addition, silanization is also a comprehensive
as chemical exfoliation, chemical vapour deposition, and modification technique used to alter the properties of
mechanical exfoliation [60]. The effectiveness of each layered nanoclays. This technique uses a reactive extrusion
technique can be evaluated according to the results of process to provide strong interactions between the nanoclay
chemical functional groups coated on the surface of and the polymer matrix through the fostered covalent bonds
graphene. However, graphene preparation usually involves during the modification process of nanoclay with
the chemical oxidation process to produce graphite oxide organosilanes. For instance, 3-aminopropyltrimethoxysilane
first, followed by the reduction and mechanical exfoliation (APTES) and vinyltrimethoxysilane (VTMS) are widely
process [61]. Based on the chemical behaviour of graphite used as silane agents to modify the surface galleries of
oxide, it is non-conductive and naturally will swell and layered nanoclays [65]. Consequently, the modified-layered
disperse in water due to the hydrophilicity characteristic of nanoclays to be dispersed into the polymer matrix will have
its morphology. This carbon-based nanofiller seems to be better insulation properties due to the formation of strong
modified by functionalizing the surface of graphene sheets covalent bonds and well-dispersion nanoclays, which may
with certain chemical functional groups to improve its improve insulation diagnosis properties as partial discharge
dispersibility in polymers and organic solvents [59]. Thus, endurance, dielectric field strength, and electrical treeing
the better dispersion of graphene nanofillers can be prolongation.
achieved by overcoming the agglomeration issue, in which Porous and hollow nanoparticles are also categorized as
avoiding the formation of large trap sites of space charge on good nanofillers since they promise innovative possibilities
the dielectric materials to strengthen the dielectric field for preparing nanocomposite polymers [66]. In
strength of nanocomposite polymers filled with nanometre- nanocomposite polymers, halloysite nanotube is one of the
sized graphene. fillers found to have a great potential to increase
Incorporating exfoliated nanoclays into the polymer mechanical, thermal, electrical, non-flammability
matrix leads to an increase in the insulating properties, such significantly [66]. Besides, halloysite nanotube is also being
as improving the stiffness, fire retardancy, and space charge used intensively in many applications by considering the
6
shape, surface area, size, and length to diameter ratio. In Inorganic material is a good component in terms of
addition, zeolite is another type of porous and hollow rigidity and thermal stability [68][69]. In comparison, the
nanoparticle that promotes an improvement on the organic polymer is an exciting material to be used as an
polymeric materials by enhancing the space of insulation medium due to its flexibility, ductility, and
intercrystalline, forming a better external and internal processability and can be an effective dielectric medium
surface area creating the volume and pores of the exposed [70][71]. Thus, introducing inorganic nanoscale fillers into
muzzles. As a result, the insulation properties of filled organic polymer hosts is intended to achieve both
polymeric materials experienced a significant improvement component properties’ advantages.
in terms of endurance, especially. Hectorite and montmorillonite are among the most
commonly used smectite-type layered silicates to prepare
The nanofibril and nanocrystal celluloses are the nano-
polymer/layered silicate nanocomposites. The main reason
compounds with such renewable, recyclable, non-toxic, and
why layered silicates are coated onto the nanofiller surfaces
sustainable properties because carbon footprints are low.
is that nanofiller’s hydrophilic characteristic in nature
Hence, both types of cellulose nanoparticles can be makes them difficult to disperse uniformly into a polymer
concluded as green nanofillers that significantly enhance matrix [72]. Thus, silicate layers coated onto nanofiller
polymeric materials. In nanoparticles of metallic alloys, the surfaces would result in better dispersion, enhancing the
fragmentation of particles conductively may increase the properties of this nanocomposite due to biocompatibility
surface area of the metal particles, and this consequently the between layered silicate nanofiller and polymer matrix [73].
properties of polymeric materials gaining a comprehensive Polymer/polymer nanocomposite is a composition that
improvement after dispersing this type of nanoparticle into combines two substrates of polymers. Commonly,
the matrix. polymer/polymer nanocomposites are prepared by using in
situ polymerization technique. The aims of producing this
E. CLASSIFICATION OF NANOCOMPOSITES composition are to obtain a nanocomposite using both
MATERIAL polymer properties [74].
Nanocomposites can be categorized based on functional The study trend regarding this composition also focuses
materials such as electrical, thermal, optical, on confining the polymerized phase to the nanoscale
electrochemical, and catalytic behaviours. However, in domain and characterizing the dispersion. Recent progress
certain cases, nanocomposites can also be categorized demonstrates polymer blends and interpenetrating networks
based on the structure of the materials, which contribute via supercritical carbon dioxide substrates such as
more to their mechanical properties. Different component polystyrene-based. However, this composition is slightly
materials of nanocomposites would obtain different more challenging to prepare due to the larger polymer chain
functional determination. size and higher mobility of the product due to stronger
Another way to classify nanocomposites is through the interactions with the matrix phase.
identity of composition materials. Nanocomposites can be Recently, inorganic/organic hybrid nanocomposites have
classified into several classes: polymer/ceramic drawn special attention due to their extraordinary properties
nanocomposite, inorganic/organic polymer nanocomposite, and widespread applications in diverse fields such as
inorganic/organic hybrid nanocomposite, polymer/layered dielectric insulation, cell imaging, drug delivery, photo-
silicate nanocomposite, polymer/polymer nanocomposite, thermal therapy, bio-sensing, catalysis, energy storage, and
and bio-nanocomposite. gas sensing. In some literature, inorganic/organic hybrid
Polymer/ceramic nanocomposite comprises ceramic nanocomposites are also referred to as nanocomposite
materials such as silica and bioactive glasses used as polymers that are filled by two or more types of nanofillers
nanofillers dispersed within the pure polymer. For instance, [75]-[78]. The main purpose of this composition is to obtain
low-density polyethylene/silica nanocomposite and K- a better performance of dielectric insulation depending on
carrageenan/calcium phosphate nanocomposite is the the properties of multiple types of nanofillers used to be
polymer/ceramic nanocomposite that shows properties dispersed into the matrix. For instance, Chao et al. has used
intermediate between organic and inorganic polymers silicon nanoparticles-modified epoxy as a dispersing agent
ceramics. The primary goal of preparing polymer/ceramic to obtain a uniform dispersion of silver nanowires into the
nanocomposite is to achieve combinations of properties epoxy matrix [75]. Inorganic/organic hybrid
from polymer and ceramic components [67]. nanocomposites are promising nanocomposite polymers,
Besides, inorganic/organic polymer nanocomposite consisting of great properties such as high thermal
comprises a polymeric matrix and a plurality of metal conductivity, high glass transition temperature, high
nanoparticles. Epoxy/clay nanocomposite is an example of electrical insulation, and low viscosity [75][76]. However,
inorganic/organic polymer nanocomposite. Generally, the this category of nanocomposite polymers is rarely used in
organic component is referred to as the polymer host, and designing dielectric insulations. In addition,
the inorganic component is referred to as the nanoscale inorganic/organic hybrid nanocomposites also appeared as
materials. This combination brings together the advantages active layers for electronic devices, such as memristor and
of both components. transistor. The term ‘hybrid’ refers to the combination of
inorganic and organic components that form a single Xing et al. pointed out that bio-nanocomposite material
material called nanocomposite with improved and unique system has been applied in various areas, including resistive
properties than the individual components. The purpose of memory, flash memory, nano-biotechnology, biosensors,
this combination is also to obtain a composition with both biofuel cells, artificial organs, and artificial synapses, and
component properties. Graphene is the most recognized as artificial neural network simulation [84]. In fact,
one of the potential organic components, whereas silica is a introducing nanoparticles into bio-hybrid systems may
popular material of inorganic components for generate new mutant materials and add new perspectives to
inorganic/organic hybrid nanocomposites. Ziyu et al. [79] the development of materials science and organic
have introduced benign carbon dots/silk protein hybrid electronics [84].
nanocomposites as a phototunable carrier trapping to
fabricate an optical transistor synapse, which provides a III. DIELECTRIC INSULATION OF NANOCOMPOSITES
comprehensive avenue for bio-inspired neuromorphic POLYMER
computing. The study revealed that after doping carbon Based on the previous research that has been conducted
dots into silk film, the potential value of the non-projected regarding the nanocomposites study. The most common
zone has decreased, and the potential change induced by nanoparticle used as a filler in nanocomposites for electrical
electron injection has increased, implying that the carbon insulation is carbon nanotubes, silicon dioxide, nanoclay
dots play a vital role in the carbon dots/silk hybrid (i.e., montmorillonite, organomodified nanoclay, sepiolite,
nanocomposites which work as a mechanism of charge- etc.), and metallic oxides (i.e., zinc oxide, alumina titanium
trapping in the development of phototunable bio-electronic oxide, etc.).
memory devices [79][80]. In another study, Ziyu et al. also Calebrese et al. [85] reported that silica nanofillers had
pointed out that inorganic/organic hybrid nanocomposites been used widely together with numerous polymer
such as all-inorganic caesium lead bromide (CsPbBr3) matrices, and the composition has shown positive
perovskite quantum dots/poly-methyl methacrylate improvement significantly. Besides silica, the other
(PMMA) hybrid nanocomposites film effectively trap nanoparticle that can be categorized into metallic oxide is
charge to dominate the properties of the photonic synapse also used as a nanofiller to develop dielectric nanostructure
[81]. materials. Metal oxide can be considered a good nanofiller
Like other types of nanocomposites, the properties of an to be merged within a polymer matrix since they have good
inorganic/organic hybrid nanocomposite are also dependent electrical insulating behaviour and can be dispersed easily
upon the particle morphology and interfacial region formed due to their hydrophilic characteristic [86][87].
between both components [82]. Thus, the study trend Metal oxide is a group of nanoparticles that consist of a
regarding this nanocomposite class focuses on the synthesis combination of metal (positively charged ion, cation) and
and surface modification approach to obtain a compatible oxygen (negatively charged ion, anion) elements. The most
mixture between organic and inorganic compounds. common metal oxide used as a nanofiller is magnesium
Bio-nanocomposite is also one of the nanocomposites oxide, zinc oxide, and alumina. Those metal oxides usually
developed for application in dielectric insulation, food can be produced into both quasi-spherical shapes and
packaging, biomedical, and pharmaceutical. In the last few whisker particles. The metal element and oxygen element are
decades, nano cellulose-based bio-nanocomposite has a chemically bonded as an ionic bond in terms of the chemical
great potential to incorporate with polymer matrix, which bond. Based on previous research, metal oxide has promising
promises an effective improvement of insulation endurance. improvement in thermal conductivity, whereas the
Aulia et al. conducted a study to identify the tensile nanocomposite’s ability to sustain the high operating
properties of bio-nanocomposites polymer by dispersing temperature of medium and high voltage cable [88][89].
two types of nanofillers which is nano-silica and nano-
alumina powder, into bio-polymeric materials produced by A. ELECTRICAL TREEING
blending low-density polyethylene and silicone rubber, in In the study of electrical trees, the historical development of
which the results obtained exhibits the addition of electrical insulation has mainly been based on the
nanofillers into bio-polymeric insulator resulted into stiffer introduction of polymeric materials, which often contain
than unfilled composition [83]. For instance, bio- various additives. Nanocomposite polymer is another
nanocomposite can be prepared by mixing the bio-polymer initiative to improve the performance of polymer insulation
and solution of swollen nanoparticles. Through that, the [21]-[24] [30][31]. Recent research showed that the
polymer chains will intercalate and displacing the solvent nanofiller with appropriate surface compatibility with
with the interlayer of the silicate. Upon solvent removal, the polymer matrices could improve the performance of
intercalated structure remains, forming a biopolymer insulation, especially in terms of electrical tree
polymer/layered silicate bio-nanocomposite. Same as prolongation.
previous, bio-nanocomposite polymers are also rarely Zheng et al. [23] employed a density functional theory
chosen as insulation material compared to other classes. In method in their study to investigate the significant role of
addition, the bio-nanocomposite is an ecological strategy nanometer-sized silica as a voltage stabilizer for power
for a greener electronic and dielectric insulation medium. cable insulation. The study was found that the nano-silica
8
additive can restrict the movement of the polyethylene Alapati et al. [93] performed electrical treeing studies in
chain through Van Der Waals physical interaction. In polymer nanocomposites. In the study, epoxy resin was
addition, the particular modified surface of silica, such as chosen as a host polymer, while nano-silica was used to fill
incompletely hydroxylated, boron-doped, and oxygen within the epoxy resin matrix. Treeing experiments were
vacancy defect on the top layer of nanosilica, could induce performed at a constant alternating current voltage of 20kV,
the migration reaction and consequently affecting electrical 50Hz on epoxy samples without any fillers and silica/epoxy
tree growth in the cross-linked polyethylene chain [23]. nanocomposites with 1% by weight nano-silica. Times for
The nanoscale additives can effectively suppress the tree inception and tree growth patterns were studied. The
space charge accumulation and inhibit the electrical tree results show that adding a small amount (1% by weight) of
growth of power cable insulation by constraining the nano-silica particles in the epoxy resin can improve the
movement of the polymer chain and trapping hot electrons treeing resistance by delaying the tree inception time and
[23][24]. Hot electrons are usually formed due to the the time required by the tree to reach the opposite electrode
energy conversion from kinetic energy (movement of a [93].
polymer chain) to heat [23][24]. In this study, nitrogen- The initiation of electrical trees usually formed due to the
doped silica with a completely hydroxylated surface, such existence of the void, crack, or/and inclusion between the
as shown in Fig. 4, is the most promising additive due to its surface of needle tip and nanocomposites polymer [93]-
strongest adsorption abilities to cross-linked polyethylene [95]. After the initiation of the tree, it starts to grow through
and transferring charge as well as the weakest chemical the base polymer and continues to propagate towards the
activity. nanoparticle due to the local enhancement in the electric
field [93]-[95]. The presence of hydroxyl groups on the
nanoparticle surface forms hydrogen bonding with the polar
groups present on the base polymer. It has been reported
that hydrogen bonding forms a weak chemical bond with
conductive nature because of polar groups [93]. The
interfacial region between the nanoparticle and polymer
matrix has higher conductivity than the polymer base or the
nanofiller because the density of hydrogen bond forms near
the nanoparticle surface is higher than in the other region
[93].
Once the tree channel reaches the nanoparticle, it
propagates through the interfacial region due to the
conductive nature of that region. After propagating along
FIGURE 4. The nanosilica model with nitrogen-doped and complete
surface hydroxylation [23]. the interfacial region, the tree channel continuously
propagates to another nanofiller through the polymer base.
Du et al. [90] also conducted an extensive study to Thus, the pattern of tree propagation tends to be more
identify tree characteristics in silica/silicone rubber zigzag and slow down the tree propagation with a greater
nanocomposites under low temperatures. The study number of branches, as shown in Fig. 5. The tree channel
reported that the addition of nanoparticles into silicone propagates around the nanoparticles and erodes the polymer
rubber could improve the insulating properties compared region around the nanoparticles due to continuous
with undoped material. The samples were prepared by discharges inside the tree channel [93]. When the tree
mixing nano-silica into room temperature vulcanized channel diameter reaches the inter-particle distance, the
(RTV) silicone rubber, containing 0, 0.5, 1.0, 1.5, and 2.0 nanoparticles enter the tree channel. The ingress of
wt%. The experiment was conducted in the range of nanoparticles further delays the tree propagation by
temperature from -30 °C to -90 °C. Alternating current obstructing the discharge avalanche inside the tree channel
voltage with a frequency of 50 Hz was applied between a [93]-[95].
pair of needle-plate electrodes to initiate the electrical tree
at different experiment temperatures. The experiment
results indicated that both nanoparticles and low
temperature are important factors of the treeing process in
silica/silicone rubber nanocomposites [90]-[92]. The
distribution of tree structures depends on the content of
nanoparticles and temperature [90]-[92]. Nano-silica can
effectively repress tree growth, and the optimum content
with the lowest tree growth speed is 1.5 wt% [90].
Crystallization caused by the changing temperature also
influences the treeing process [90]-[92].
organic modification and solubilization methods. In the

study, frequency accelerated partial discharge ageing of
epoxy nanocomposite with 5 wt% additions of clay was
investigated compared to epoxy without clay in partial
discharge erosion depth. Layered silicate (LS) or clay is
organically modified through hydrochloric acid processing
and ion exchange processing by organic modification or
solubilization methods. In the organic modification method,
layered clay is organically modified with octa-decyl amine
without a swelling process added and dispersed to neat
epoxy.
On the contrary, organically modified clay is swollen in
dimethylacetamide (DMAc) to be added into neat epoxy in
the solubilization method. Scanning electron microscopy
observation was made to evaluate the degree of dispersion
of layered clay in nanocomposite specimens prepared by
the solubilization method. In the scanning electron
microscopy photo, nanofillers did not agglomerate in
FIGURE 5. Physical model of electrical tree growth in nanocomposites
structure and were comparatively homogeneously dispersed
polymer [93]. [98]. The surface of the specimen is eroded due to partial
discharge exposure, and erosion depth is selected as a
B. PARTIAL DISCHARGE measure of partial discharge resistance. The result
Polymer nanocomposites have recently attracted attention confirmed that even the small content like 2 wt% would
among researchers in electrical insulating applications from work well against partial discharge degradation [98]. It was
energy storage to power delivery. However, the partial shown that the highest partial discharge resistance was
discharge has always been a predecessor to major faults and indicated by micro-nano mixed epoxy nanocomposite
problems in this field. In addition, there is a lot more to followed by solubilization method nanocomposite and
explore, as neither the partial discharge characteristic in organic modification method nanocomposite. While pure
nanocomposites nor their electrical properties are not epoxy (reference erosion depth) showed the lowest partial
clearly understood. For instance, nanofillers in discharge resistance.
nanocomposites such as silica, alumina, and Titania play a Nanoparticles consist of three-layered cores with
significant role in providing a good approach to increase the different characteristics and morphology compared to
partial discharge resistance of nanocomposites [96]. polymer matrices. Each core has different roles, but only
Tanaka et al. [97] carried out a comprehensive two roles are distinctive and prominent for the
experimental investigation of cross-linked polyethylene and characteristics of partial discharge resistance. The first role
its nanocomposite with fumed silica in the CIGRE Working indicates the direct process where the base polymers are
Group D1.24 cooperative tests conducted by members segmented into three-dimensional nano-meter scales by the
covering partial discharge resistance. The experiment was nanofillers [97][98].
set up to measure the erosion speed due to partial discharge The second role indicates an indirect process and an
events. A voltage of 10 kVrms (250 Hz) was applied to important process where the ability of nanofillers to hold
three kinds of cross-linked polyethylene samples of 1 mm physical tightness with pure polymer matrix and apparent
thickness for time up to 750 h (50 Hz equivalent time). enlarged volume due to the formation of interaction zones
Applied voltage corresponds to 5 times partial discharge [97][98]. Both aspects (refer to the first and second roles)
inception threshold. A needle-plane electrode system with must be mutually coordinated to increase partial discharge
an air gap of 0.1 mm and a tungsten needle electrode of 1 resistance. The formation of three cores would reduce the
mmφ diameter for partial discharge erosion evaluation. The interstices between neighbouring fillers [97][98].
result obtained in this study showed that filled cross-linked Consequently, the strength of nanocomposite polymers in
polyethylene exhibits much-improved endurance to partial terms of partial discharge endurance can intensify.
discharge (i.e., 0.001 mm2/h of average erosion speed) than The erosion mainly happens in the polymer region of
unfilled cross-linked polyethylene (i.e., 0.0016 mm2/h of nanocomposite substances. This is because inorganic
average erosion speed), and the best performance was nanofillers are far more partial discharge resistive than
possessed by cross-linked polyethylene filled with surface- organic polymers [97][98]. Thus, the partial discharge will
heat treated filler (i.e., 0.0006 mm2/h of average erosion attack pure organic polymer regions preferentially. Through
speed) [97]. that, the segmentation of organic substances (pure polymer)
In another study, Tanaka et al. [98] also performed into many small areas and volume is effective against
research to enhance partial discharge resistance of partial discharge attack [97][98]. This configuration will
epoxy/clay nanocomposite prepared by newly developed help to increase partial discharge resistance.
10
C. DIELECTRIC BREAKDOWN STRENGTH to-volume ratio [104]. As a result, the insulation properties
As mentioned, dielectric breakdown strength is one of the of the nanocomposites polymer will further extend to the
most important properties of insulation material. The comprehensive level.
dielectric breakdown strength of nanocomposites depends The interfacial region formed through the incorporating
heavily on the nanofiller content, and even small quantities process act as a barrier to the transported charge. Charge
can cause improvement [99][100]. This is linked to the transportation is an important aspect required to enhance
maximum interface volume achieved already at low the dielectric field strength and the electrical erosion of the
nanofiller concentrations. Homogeneous nano-dispersion is nanocomposites polymer [105]-[106]. This has been proven
the key for dielectric breakdown strength increase and by Montanari et al. [107] that pointed out that the new
reliable results [99][100]. Often the most profitable relaxation process has occurred related to the charge
nanofiller quantities are below 5 wt% [99]. The same kind trapping at the interfacial region. Consequently, reducing
of behaviour can be seen with different voltage shapes, but the transportation charge due to the formation of the
the increase is more significant with direct current voltage. interfacial region also affects the magnitude of interfacial
Dielectric breakdown strength has a maximum value charge by exhibiting fewer charge forms in the
concerning the nanofiller amount (below 5 wt%) and nanocomposites polymer [102]. Besides, the decay of
decreases after that. Filler quantities around 5 wt% and dynamic charges faster in the nanocomposites polymer than
even lower are the most attractive considering the dielectric the pure polymer due to the formation of the interfacial
breakdown strength of nanocomposites [99]. region effectively serves as a barrier to the charge carried in
Tanaka et al. [97] experimented with investigating the the insulation materials [102]. Besides, the existence of
dielectric breakdown strength of cross-linked nanofillers in the polymer matrix also makes the space
polyethylene/silica nanocomposites. Alternating current charge accumulated on the nanocomposites polymer
dielectric breakdown strength tests were performed using a become lower and redistributed due to the presence of
test cell with 2 spherical electrodes (diameter 30 mm) in homopolar charge adjacent to the cathode [108]. This could
silicone oil at room temperature. Data were obtained in the be why nano-meter scale fillers are introduced to replace
form of two parameters of the Weibull distribution (i.e., the micro-meter scale fillers since space charge accumulation is
scale parameter and the shape parameter). They represent higher and not redistributed due to the charge adjacent to
the breakdown strength α [kVrms/mm] and the data scatter the cathode being heteropolar.
β, respectively. The applied voltage was increased at the However, the concentration of nanofillers is required to
rate of 500 Vrms/s (60 Hz). About 40 numbers of be considered to produce optimum and comprehensive
breakdown measurements were made on each of the 3 enhancement of insulation properties. As referring to the
samples (~1 mm thick), and data outliers were removed physical conception, the interfacial region being the crucial
from statistics. The results obtained showed that the highest constituent in producing the most effective composition of
alternating current breakdown strength was obtained with nanocomposites polymer. In fact, the concentration or
cross-linked polyethylene filled by functionalized nanofiller amount of nanofillers incorporated into the polymer matrix
after heat treatment [97]. affected the interfacial region formed. The higher the
amount of nanofillers dispersed into the polymer matrix, the
IV. RELATIONSHIP BETWEEN THE PHYSICAL AND larger specific interfacial area will be formed. However,
CHEMICAL COMPOSITIONS OF NANOCOMPOSITES there is a specific limit of the amount of nanofillers called
POLYMER AND INSULATION CHARACTERISTICS critical loading, which indicates the maximum amount of
A. PHYSICAL COMPOSITIONS OF NANOCOMPOSITES nanofillers that need to be adhered to obtain an
POLYMER improvement in the insulating properties effectively.
The main purpose of incorporating the nanofillers into the Previously, in some literature, the critical amount of
polymer matrix is to combine insulation properties in nanofillers defined as not to exceed 10 wt% because the
between the nanofillers and the neat polymer. Hence, the further increase might cause an adverse effect to the
enhancement of insulation properties promised by adding properties [109]. Related to the interfacial regions,
the nanofillers into the matrix must be understood dispersing more than 10 wt% of nanofillers might cause the
physically. A few physical factors must be considered to nanofillers distributed too close to one another. This might
produce a better performance of insulation properties, cause the self-agglomeration of filled nanoparticles and
especially in terms of electrical properties. Structurally, consequently reducing the specific interfacial region.
interfacial regions formed in between the nanofillers and Worse, this may destroy the natural properties of
polymer matrix is the crucial factor that contributes to the nanocomposites polymer as insulators because reducing
significant improvement of insulating properties [101]- interfacial region will cause the mechanism of trapping
[103]. This is related to the radius size of the fillers, in charge to occur ineffectively as compared to larger
which reducing the size of the fillers forms a larger specific interfacial region formed with the loading of nanofiller less
surface area, and this physically will increase the formation than 10 wt%.
of interfacial area. Thus, the interfacial area between the In addition, the agglomeration of nanofiller also occurs
nanofillers and polymer matrix will have a higher surface- due to the imperfection of the processing/dispersion
11
technique [110]. The agglomeration of nanofillers in a interaction region by using chemical pre-treated nanofillers
polymer matrix will cause the formation of the interfacial can be done by functionalizing modifiers containing
region to reduce, usually indicated by the decrement of reactive groups. This technique effectively constructs
surface area to volume ratio significantly. This also might chemical bonding between the nanofillers and the polymer
compromise the unique nanofiller properties in the matrix, indirectly strengthening the merging mechanism of
polymer. Therefore, the processing technique needs to be the nanocomposites mixture [113]. The coupling agent is
executed in detail by considering mechanical mixing and the most intensive treatment used to enhance the
ultrasonication-mechanical mixing technique in a high compatibility between inorganic fillers and organic
shear force mechanical mixer [110]. Follow by the second matrices. The ubiquitous coupling agents used for this
stage of dispersion by using ultrasonic agitation. The purpose are silane, titanite, and zirconate. Collectively, the
trapped air bubbles and moisture also need to be removed attachment of silanes on the nanofillers offers the reduction
through the degassing process [110]. Furthermore, of hydrophilic properties of the nanofillers [65][114]. In
nanofillers' agglomeration can also be resolved using the addition, grafting macromolecules onto inorganic particles
surface functionalization technique discussed is also a technique implemented to alter the interfacial
comprehensively in this review. characteristics between treated nanofillers and the polymer
The interfacial region has been pointed out as a key in matrix. The grafted polymer properties can be strategized
improving insulating properties due to its role in trapping depending on the graft monomers' species and the grafting
the charges distributed in the nanocomposites polymer. The process's condition. Furthermore, the grafting technique
trapping charge mechanism will reduce the accumulation of also capable of strengthening the fragile agglomerated
space charge and minimize the distortion of the local nanoparticles and forms a microstructure of
electric field. This brings positive implications to the nanocomposites that consists of nanofillers and homo-
insulation properties, such as improving the relative polymerized polymer.
permittivity, dielectric losses, dielectric breakdown The compatibility of nanofillers and polymer matrix also
strength, dissipation factor, partial discharge, surface can be achieved by functionalizing a chemical functional
tracking, erosion resistance, and electrical treeing group on the surface of nanofillers such as hydroxyl (OH-)
prolongation. and carboxyl (C(=O)OH) functional group [23][115]. This
technique can be done by using either chemical
B. CHEMICAL COMPOSITIONS OF NANOCOMPOSITES functionalization or plasma treatment. The functionalized
POLYMER chemical groups will further strengthen the interfacial
The chemical composition of nanocomposites polymer is region between the nanofillers and polymer matrix by
closely related to its physical composition. As highlighted, forming covalent bonds; thus, a rigid interfacial region can
the agglomeration of nanofillers in a polymer matrix being be produced to maximize the trapping charge mechanism
a major factor stifling the improvement of insulation [110]. Hence, improve the insulation properties by
properties of nanocomposites polymer. Commonly, the minimizing the distortion of the local electric field on the
agglomeration of nanofillers is happened due to the nanocomposites polymer.
incompatibility between the surface of nanofiller and
polymer matrix chemically [6]-[14]. Naturally, most V. LIMITATION OF SURFACE MODIFICATION
nanofillers' surface morphology is hydrophilic, while most TECHNIQUES
of the polymers tend to be hydrophobic [53]. Hydrophilic is Surface modification is one of the subjects required to be
a characteristic or entity of a molecule that chemically considered to obtain effective insulation performance of
reactive to the water molecules and tends to be dissolved by nanocomposite polymer regardless of the types of polymer
water molecule [15]-[17][72][86][87]. At the same time, host and nanofiller used to form the nanocomposites.
hydrophobic is a property of a molecule that chemically not Several surface modification techniques are currently used
undergoing a reaction with water molecule [111][112]. to alter nanofillers' surface morphology, such as surface
Thus, the dispersing process of nanofillers into the polymer functionalization, coupling agent, intercalation, heat
matrix is mismatched or incompatible, cause the nanofiller treatment, plasma polymerization, and plasma treatment.
to agglomerate. Organophilic represents the molecules on The purpose of all techniques is to enhance nanofiller
which the surface consists of covalently linked organic surface structure by overcoming the agglomeration of
moieties [53]. Hence, the surface modification technique nanofiller and incompatibility between nanofiller and base
must be done on the nanofillers to form organophilic polymer surfaces.
characteristics, which may improve the compatibility of Fig. 6 shows the model of agglomerated nanocomposite
nanocomposites polymer mixture [53]. polymers. Specifically, the enhancement of insulation
Chemical modification is a comprehensive technique performance can be achieved by resolving agglomeration
widely used since this technique significantly improves the issues and creating compatible surface structures between
insulation properties of nanocomposites polymer through nanofiller-base polymers [6]-[14]. Fig. 7 shows the model
the covalent attachment modifier that prevents desorption of a compatible mixture between surface-treated nanofillers
from the particle surface [113]. The modification of the and polymer matrices. For instance, the insulation
characteristics promising improvement through surface
12
modification techniques are partial discharge, dielectric self-repelling process, high effectiveness, effective to form
breakdown strength, electrical tree, space charge, etc. and strengthen interfacial covalent bonds but has not been
explored thoroughly in this regard [114][120][121].
C. LIMITATION OF PLASMA TREATMENT

Dealing with the limitation of plasma treatment systems is a
challenging task when choosing plasma treatment as a
nanofiller surface modification technique. Cold plasma has
been practiced widely in the study of nanofiller surface
modification. However, the previous collective studies only
highlighted the duration of treatment with filamentary
plasma discharge. Only a limited number of studies are
concerned about the discharge mechanism toward the
FIGURE 6. The model of agglomerated nanocomposites polymer filled effectiveness of insulation performances. Glow plasma
with untreated nanomaterials.
discharge is a uniform discharge, while filamentary plasma
discharge is a non-uniform discharge of gases [122].
Uniform discharge is expected to overcome incompatibility
issues effectively compared to non-uniform discharge.
Nowadays, plasma technology has been chosen as an
alternative method to improve the uniformity of
nanoparticle dispersion within polymer matrices. Plasma
treatment also helps to improve the molecular structure of
nanofillers so that the distribution of nanoparticles within
the polymer matrices is dispersed homogeneously
[114][120][121]. As per our knowledge, the specific design
of the cold plasma system for this purpose still has not
existed yet. Therefore, the most effective cold plasma
FIGURE 7. The model of compatible nanocomposites polymer filled system with a glow discharge mechanism must be designed
with surface treated nanomaterials.
and developed by concerning any other factors such as
optimum voltage and frequency of plasma generation and
A. LIMITATION OF CHEMICAL FUNCTIONALIZATION
the structure of the plasma chamber.
Surface functionalization, coupling agent, intercalation, and
Plasma surface treatment is also being employed in
plasma polymerization are techniques that use chemical
numerous researches to modify the structural surface of
agents and/or solvents to functionalize certain chemical
nanoparticles. However, a limited study was conducted
functional groups on the nanofiller surfaces [116]-[118].
which employed cold plasma with a glow discharge
Since this method required chemical solvent, which is
mechanism to treat nanofiller, which were next to be merged
difficult to decompose and toxic in some cases, surface
within the polymer matrix. Therefore, a specific cold plasma
functionalization methods are not suggested to be
reactor needs to be used to treat the surface of a nanofiller
implemented, especially in the manufacturing industry of
before it is dispersed within the polymer matrix.
cable. Besides, the by-products formed during the chemical
reaction of those techniques are not guaranteed either VI. COLD PLASMA
harmful or not to the human and eco-environment. Thus, heat Plasma is a state of an ionized gaseous substance that
treatment and plasma treatment have been introduced to becomes highly electrically conductive to the point that
replace those techniques which are more eco-friendly. having long-range electric and magnetic fields dominates
the substance’s behaviour. Plasma is a technology that can
B. LIMITATION OF HEAT TREATMENT be used to treat a certain condition of the chemical
Heat treatment is also one of the techniques used to alter the phenomenon to improve the properties of the system [123].
surface morphology of the nanofiller. This is intended to In other words, plasma treatments are useful for
obtain a uniform dispersion of nanofiller within the modification and treatment processes towards a certain
polymer matrix. However, this technique has a drawback mechanism, system, chemical structure, chemical process,
that can damage the nanofiller’s surface structure, etc.
especially when the amount of heat exposure on the Interestingly, plasma treatment can be applied to improve
nanofiller exceeds the minimum amount of heat that can be the dispersion of the nanoparticle, nanocomposite bonding,
detained by the nanofiller [119]. Thus, an alternative to and the compatibility surface between polymer matrices and
those techniques explained above is plasma treatment nanoparticles [114][121]. However, several factors such as
which deemed to provide an effective surface modification suitability, types of plasma, and harmful sub-product
process on the nanofiller due to eco-friendly, providing a generated from the plasma treatment process need to be
13
considered before carrying out the treatment process. As several drawbacks, such as requiring complicated and
mentioned, plasma treatment is an alternative method that is expensive vacuum systems. Besides that, the vacuum
useful to modify the surface of the nanoparticles. Thus, this system also often requires a maintenance process which
section discusses the behaviour of cold plasma based on low means consuming high expenditure. On top of that, the
and atmospheric pressure discharge conditions. capacity and size of the nanofiller to undergo treatment are
also limited by the size and capacity of the vacuum
A. LOW-PRESSURE PLASMA chamber. On the other hand, a low-pressure plasma reactor
Low-pressure plasma is discharges made under low gas is not applicable to be practiced at the industrial levels as it
pressures compared to the gas at atmospheric pressure. Fig. requires a low controlled pressure system to achieve the
8 illustrates the setup diagram for plasma production under plasma discharge state due to higher cost and great
low-pressure conditions. This type of discharge benefits difficulty to operate as a continuous process.
from less power requirement of sustenance of the discharge
as the rate of volume-recombination is low [124]. At low B. ATMOSPHERIC PRESSURE PLASMA
pressure of gases, it is easier to achieve uniform discharges Atmospheric pressure plasma is one of the plasma
at once to produce a better quality of plasma [124][125]. categories that discharge under atmospheric pressure (i.e.,
Thus, the materials processing proceeds at the same rate 1.01325 x105 Pa). In order to overcome the drawbacks of
over large substrate areas. In addition, low-pressure plasma low-pressure plasma reactors, atmospheric pressure plasma
also produces high concentrations of reactive species that has been introduced since it promised the solution over
can etch and deposit into thin films [125]. low-pressure plasma drawbacks. The main advantages
provided by this type of plasma discharge are the
elimination of vacuum systems, reduced operation and
maintenance cost as well as possibility to be employed in
the continuous treatment system. The type of atmospheric
pressure plasma discharge can be categorized into two main
regimes: filamentary or micro-discharge plasma and
atmospheric pressure glow (APG) discharge [128]. Micro-
discharges are obtained either by using a corona system,
dielectric barrier discharge, or plasma jet configuration
[129].
One of the reactors to produce plasma discharge at
atmospheric pressure is dielectric barrier discharge (DBD).
Fig. 9 shows the structure of a dielectric barrier discharge
reactor to produce cold plasma at atmospheric pressure
FIGURE 8. Setup diagram for plasma system under low-pressure conditions. Dielectric barrier discharge has been used
conditions. widely in ozone production, surface treatment, and
nanofiller treatment to improve insulating materials.
Usually, the prevalent background gas used is argon Dielectric barrier discharge consists of two parallel plate
since it has a low potential of ionization in which it is easier electrodes, with at least one of these electrodes covered by
to initiate and sustain the discharge process. The thermal- a dielectric layer made up of insulating materials. The
sensitive substrate also does minor damage since it is distance between the electrodes is maintained and limited to
unreactive, monatomic, and extremely low boiling point certain millimetres in width for a stable plasma production
[126]. The ions produced in the plasma discharge will [130]-[132].
accelerate toward a substrate to make a directional etching
of submicron features. In the other study, the various uses
of low-pressure plasma reactors can change gas feed ratios,
gas flow, time of treatment process, and power density. Due
to those benefits, low-pressure plasma is the most common
type of plasma discharge widely employed in industrial
applications such as semiconductor manufacturing and
material processing.
The frequency of low-pressure plasma reactors usually
depends on the geometric properties of the reactor itself.
However, the very common low-pressure plasma reactors
are using microwaves at 2.53 GHz. This is because
microwaves can operate at lower pressures and produce
higher plasma densities [127]. Even though low-pressure
plasma promises a good plasma treatment for this
application, operating the plasma at reduced pressure has
14
FIGURE 9. The basic structure of the dielectric barrier discharge FIGURE 10. The classification of plasma discharge is based on the
reactor operated under atmospheric pressure conditions. density of electron bombardment and electron temperature [138].
Dielectric barrier discharge can be ignited by using either Plasma treatment is also chosen to be one of the
a sinusoidal or pulsed power generator. The type of processes that promise enhancement on the characteristic of
discharge in this configuration could be glowing or the insulation. For surface modification, plasma treatment
filamentary depends on the gas composition, voltage, and has promoted modification of wettability, printability, and
frequency excitation. As mentioned, filamentary discharge adhesion of the treated materials [139]-[141]. Plasma
is formed by micro-discharges that are statistically treatment also can be used to treat the structure of the
developed on the surface of the dielectric layer while using nanofiller surface, which indirectly improves the
an inert gas such as helium as plasma gas may produce effectiveness of nanocomposite polymers as an insulation
glow discharge [133]. medium.
The dielectric layer plays an important part in limiting The type of plasma used for the treatment must be
the discharge current and preventing the arc transition chosen based on the suitability and effectiveness offered by
enabling the system to operate with a continuous or pulsed that particular plasma. The most effective form of plasma
mode. This layer contribution ensures the streamers are used for surface modification on nanofillers is glow
distributed randomly and equally on the surface of the discharge and radio frequency (RF) discharges [142].
electrode so that the homogeneous treatment can be However, plasma characteristics must also be studied to
achieved. The streamers are produced from the identify which type of plasma can work effectively for this
accumulation of an electron on the dielectric layer treatment. In this section, the treatment of nanofiller
[134][135]. surfaces using cold plasma is discussed based on the
pressure of the discharge process.
VII. SURFACE TREATMENT OF NANOFILLER BY COLD Low-pressure plasma treatment can be done by exposing
PLASMA the nanofillers to the plasma plume produced under a low-
Plasma is a form of matter in which many electrons wander pressure condition, usually operated inside a closed vacuum
freely around the nuclei of an atom. The plasma properties system. In contrast, atmospheric pressure plasma treatment
are changed in electronic density or temperature depending is executed by exposing the nanofillers to the plasma plume
on the energy supply and the amounts of energy transferred forms under atmospheric pressure conditions. Usually, the
to the plasma [136]. Plasma can be categorized into certain duration of plasma treatment, type and flow rate of
categories based on these two parameters: electron density discharge gases, voltage, and frequency of supply are
and electron temperature [136][137]. Fig. 10 shows the varied to obtain different plasma treatment mechanisms on
characteristic of plasma discharge. the surface of nanofillers. The treated nanofillers under the
different configurations of plasma production are then
placed inside an airtight container, and then all the samples
are characterized by using spectroscopy instruments such as
X-ray Photoelectron Spectroscopy (XPS) and Fourier
Transform Infrared Spectroscopy (FTIR). The waveform of
voltage supply and discharge current was also recorded to
characterize the mechanism of plasma discharge during the
treatment process. Voltage-discharge current and Lissajous
15
figure waveforms are usually used to characterize the organometallic compound decomposition and the size and
plasma discharge. Besides, optical emission spectroscopy is the oxidation state of the homogeneously dispersed nickel
another equipment used to characterize plasma discharge nanoparticles, which obtained through a low-pressure
according to the spectrum of discharge species that plasma processing technique [144].
occurred through the plasma discharge process. The treated Introducing plasma treatment also helped increase the
nanofillers then dispersed in a polymer matrix using flux, whereas doping modified the surface properties of the
appropriate processing techniques such as direct mixing to nanoparticle [145]. Meanwhile, plasma treatment can
form nanocomposites polymer. increase the porosity and roughness of nanoparticles.
Agrawal et al. [145] applied low-pressure plasma treatment
A. LOW-PRESSURE PLASMA TREATMENT with a glow discharge mechanism to coat and modify the
In 2010, Hody et al. [143] conducted a comprehensive surface of nano-cobalt. The absorption bands of C-O and
study to functionalize silicon carbide nanofiller with C=O are attributed to the creation of unsaturated -C=C-
carboxylic groups by synthesis it is using low pressure (i.e., bonds after plasma treatment [145]. C-C and C-H bands’
40 Pa) plasma at radio frequency (i.e., 13.56 MHz) intensity also decreases, which represents the cross-linking
discharge. A magnetic stirrer was used to make sure the phenomenon enhanced after plasma treatment. This
surfaces of the nanofiller are treated uniformly. The coating indicates the successful process of surface functionalizing
process was handled in an O2/hexamethyldisilazane on the nanofiller by improving the hydrophilicity of
(HMDSN) mixture. The x-ray photoelectron spectroscopy nanofiller surfaces. Thus, the synthesis of polymer
(XPS) analysis showed that the O2/ hexamethyldisilazane nanocomposites using nano-cobalt and polymethyl-
working gas resulted in a coating evolving from a polymer- methacrylate (PMMA) formed effective and homogeneous
like structure to a more inorganic SiOx-like structure as the nanofiller dispersion into polymer matrices [145].
oxygen ratio increased. Jiansirisomboon et al. [146] experimented with
The result showed that coated silicon carbides are investigating the effect of low-pressure plasma sprayed on
suitable to be further dispersed within the polymer host due alumina/silicon carbide nanocomposite. Plasma spray
to the surface morphology of silicon carbide after coatings are useful to provide surface resistance to
undergoing a low-pressure plasma coating process were corrosion. Low-pressure plasma spray is also considered a
being more inorganic SiOx-like structure. This indicates comprehensive technique to coat and transform nano-scale
that the nanofiller and polymer host’s surface compatibility substrates into equilibrium metastable nanocomposite
can be enhanced by coating the carboxylic functional group [146]. The study also revealed that the area percentage of
on the surface of the nanofiller [143]. nanofiller porosity and surface roughness could be further
Compatible surfaces between nanofiller and polymer increased by using low-pressure plasma spray [145][146].
host will further be formed homogeneous and uniform Indirectly, this might improve the surface morphology of
dispersion of nanofiller into a polymer matrix, thus forms nanofiller and form compatible interfaces between hybrid
effective deep trap sites to reduce the local electric field on nanofiller and polymer matrices.
the nanocomposite polymer filled with coated nanomaterial Besides, low-pressure plasma is also efficient in
[21]-[24][143]. Therefore, the insulation properties such as providing significant oxidation that resulted in nanofiller
dielectric breakdown strength, partial discharge, and surfaces with high hydrophilicity [147]. Norrman et al.
electrical tree are compromising to be enhanced by [147] pointed out that exposing polyphenyl-sulfone
introducing this alteration technique. surfaces to low-pressure plasma at 5 x 10-3 Torr will result
Low-pressure plasma is also effective in obtaining in the maximal occurrence of the oxidation process on the
homogenous dispersion of nanoparticles with a polymer surfaces of nanofiller. The oxidation reaction consists of
host. Haye et al. [144] employed low-pressure plasma with two oxidation products which are C=O and (C=O)-O.
discharge at radio frequency to synthesize nickel/carbon Both oxidation products are readily formed at 500W and
nanocatalysts from solid precursors. Three combinations of increase slightly for harsher plasma conditions. The
mixing working gas were used containing argon: nitrogen formation of both oxidation products on the surface of the
(Ar: N2, 5:2 sccm), argon: ammonia (Ar: NH3, 5:4 sccm), nanofiller may increase the surface hydrophilicity and
and argon: oxygen (Ar: O2, 5:2 sccm) with different flow wettability of the nanofiller, which enhances the
rate ratio to determine the most effective synthesize of compatibility between nanofiller and polymer host
nickel/carbon nanocatalysts under different plasma interfaces [139]-[141][147]. Therefore, the low-pressure
chemistries. Low-pressure plasma is also used to plasma-treated nanofiller is expected to be dispersed
functionalize carbon substrates such as carboxyl (-COOH), uniformly better than the dispersion of untreated nanofiller
carbonyl (C=O), and cyanide (C≡N) functional group on into polymer matrices.
nanofiller surfaces [144]. Xu et al. [111] reported that low-pressure plasma with
The radio frequency power was varied between 90 to particular functional monomers could obtain stable and
200W to obtain a complete process of plasma effective modification techniques to functionalize chemical
decomposition. The result was revealed that plasma bonds. Low-pressure plasma is also useful to alter the
chemistry and conditions strongly influence the surface roughness of nanofiller [111][145][146].
16
Spyrides et al. [148] used low-pressure plasma with the industrial level since it is not cost-effective to produce
argon and oxygen as a discharge gas to alter the surface mass products with a large-scale vacuum system. Thus, the
roughness of ultra-high molecular weight polyethylene. In plasma discharge at atmospheric pressure seems to need to be
addition, low-pressure plasma is also used to improve the explored to counter back the drawbacks of low-pressure
adhesion properties of polymers [148]. plasma and enhance nanofiller’s surface morphology to form
In fact, the wettability, chemical species, and surface a compatible and well-dispersed nanofiller into a polymer
morphology of polymer materials can also be modified matrix.
using plasma treatment at low-pressure discharge
conditions [149]. Mandofino et al. [149] revealed that low- B. ATMOSPHERIC PRESSURE PLASMA TREATMENT
pressure plasma treatment is an effective technique for the Atmospheric pressure plasma is preferred among
surface preparation of polymers to create bonded joints. researchers rather than low-pressure plasma because of the
The surface morphology of treating polymers was simple process of this system. In other words, the process
affected by the plasma power, exposure time, and type of of nanoparticle treatment becomes more accessible and
working gas [150]-[152]. In terms of surface morphology, more applicable by using atmospheric pressure plasma. The
carbonyl, carboxyl, and hydroxyl are the possible polar untreated nanofiller will be exposed to the plasma until the
groups introduced in the outermost layers of the surface by particle is homogeneously exposed and coated to become a
reactions with plasma species. All the polar groups treated nanofiller. The treated nanofiller is then mixed
functionalized on the surface of the polymer would affect within the polymer matrix by using multiple stages of a
the character of the treated surfaces, which increases the conventional method.
hydrophilicity of the surface. Recently, Yan et al. [114][156]-[161] reported the study
Low-pressure plasma also significantly decreased the of plasma application in high voltage insulations.
water contact angle of the polymer surfaces, especially Specifically, the study was conducted regarding the
pronounced for specific parameter sets. Consequently, low- improvement in terms of an electrical tree. In the study,
pressure plasma can increase the surface free energy of custom designs of atmospheric-pressure plasma reactors
polymers compared to untreated polymers [153][154]. have been employed to treat nano-silica, which exists as a
Increasing surface free energy occurred due to the nanofiller. The specimen configuration was designed by
functionalization of polar groups on the surface of low- placing 2 mm of tin-coated copper coil electrode above the
pressure plasma-treated polymers. top of the nanoparticle sample while the ground electrode
For instance, oxygen-containing functional groups were was placed under the reactor to form a dielectric barrier
formed on the treated surfaces due to the ionization of discharge system.
working gas, which is the principal cause of the enhanced Cold atmospheric-pressure plasma was generated for the
wettability. Furthermore, the strength of chemical bonds on plasma generation part using a 350 kHz radio frequency
the nanofiller surface is also a crucial aspect that needs to (RF) power supply with a maximum 5 kV peak-to-peak
be considered to obtain sufficient adhesive bond strength output voltage. However, the ideal specification of the
with relatively high surface energy. Iqbal et al. [155] plasma generator used in this study is 4 kV peak-to-peak
revealed that low-pressure plasma had effectively radio frequency voltage. The working gas used for the
functionalized dispersive components on the treated discharge medium is helium since it can decompose to
surfaces. However, identical polar groups forming on the discharge uniformly. To obtain a reliable outcome, the
low-pressure plasma-treated surfaces are not nanofillers were treated by exposing the sample of the
comprehensive as atmospheric pressure plasma treatment. nanofiller for 30 minutes until it was homogeneously
Since there are many advantages and impressive coated before mixed within an epoxy resin chain.
modification mechanisms provided by plasma treatment As expected, the studies also revealed that plasma
operated at low-pressure conditions, the low-pressure treatment enhanced the compatibility and the properties of
plasma becomes progressively common as the new surface interfacial regions between epoxy resins filled with nano-
modification technique. Indeed, plasma surface silica. In terms of modification, the treatments were
modification is also not required for water and chemical improved to increase the strength of chemical bonds and
solutions because the chemical reaction produced from the reduced the presence of weak chemical bonds while
ionization of discharge gases is developed from an maintaining excellent uniformity of dispersion [114][156]-
electrical streamer discharge. [161]. Therefore, the properties of nanocomposite improved
As mentioned, low-pressure plasma also has certain even with the low percentage weight of nanofiller.
drawbacks, which are criticized and highlighted in some In organic-inorganic nanocomposites, interfacial regions
studies. Iqbal et al. [155] claimed that low-pressure plasma are primarily influenced by the dispersion uniformity of
treatment is less effective than atmospheric pressure plasma nanoparticles and the strength of interfacial bonds between
treatment to improve surface energy and bonded joint the nanoparticles and the polymer matrix [161]. The
strength. Besides, low-pressure plasma also required a insulating performance of organic-inorganic dielectric
complex vacuum system, difficult and complicated to nanocomposites is highly influenced by the characteristics
control. Hence, low-pressure plasma is also not applicable to of interfacial regions [161].
17
In a study by Yan et al. [157], polyethylene oxide (PEO)- displacement caused by partial discharge activities is
like functional layers were prepared on silica nanoparticles detected with measurement impedance or quadripole (Zm).
through plasma polymerization. Silica/epoxy resin The result obtained in this study has shown that plasma-
nanocomposites are subsequently synthesized with these treated nano-silica, where dispersed within an epoxy resin
plasma-polymerized nanoparticles. Uniform atmospheric matrix, can suppress the partial discharge activities [156].
pressure plasma was generated with 5 kV peak-to-peak of The partial discharge level curve was categorized into three
applied voltage and 350 kHz of operating frequency. The stages in the electrical treeing process, namely 1-void
untreated nanosilica is then exposed to the plasma plume to formation, 2-tree propagation, and 3-ultimate breakdown.
treat the nanoparticles. Based on the results, the The partial discharge levels of the endurance test of
concentration of each bond in the epoxy resin untreated and treated nano-silica were measured and
nanocomposites filled with untreated nanosilica remained confirmed the time of void formation, time of tree
similar to pure epoxy resin. propagation. A lifetime of the plasma-treated nano-
This mainly indicates the nanosilica was dispersed silica/epoxy resin nanocomposite sample is prolonged (i.e.,
ineffectively within the epoxy resin matrix and failed to 19 hours of a lifetime) compared to untreated nano-silica /
improve the interfacial structure of the nanocomposite due epoxy resin nanocomposite sample (i.e., 14.7 hours of a
to the poor filler-matrix interaction [156][157]. However, lifetime) [156].
the concentration of each bond contained in the epoxy resin Awang et al. [163] reported a comprehensive study on
nanocomposite filled with plasma-treated nano-silica shows the effect of atmospheric pressure plasma-treated boron
significant changes. nitride on partial discharge characteristics of low-density
For instance, the concentration of C-O bonds of the polyethylene. The purpose of this study was to improve the
nanocomposites with plasma polymer coated nano-silica performance of the low-density polyethylene insulation
increases dramatically (i.e., 36.15 %) than nanocomposites against partial discharge by adding plasma-treated nano-
filled with untreated nanosilica (i.e., 16.14%). This boron nitride into the low-density polyethylene matrix. This
enhancement happens due to the nucleophilic substitution study was performed by following CIGRE Method II at 7
reaction between the surface oxygen-containing functional kVrms applied voltage. The results revealed that the partial
groups on the nanoparticles and the epoxide rings in the discharge resistance of low-density polyethylene
pre-polymer resin [156][157]. nanocomposite was highly achieved by treating the
In the same study, it is found that plasma at low power nanofillers with cold plasma compared with the untreated
(i.e., 10 W) can significantly increase the concentration of boron nitride nanofillers. It is showed where the magnitude
C–O bonds on the surface of silica nanoparticles. This of partial discharge of sample low-density polyethylene/5
plasma polymerized thin layer not only improves the wt% of plasma-treated boron nitride nanocomposite is
dispersion uniformity by increasing the hydrophilicity of lowest (i.e. ≈ 2 pC at 600 s) followed by low-density
the nanoparticles but also provides anchoring sites to enable polyethylene/5 wt% untreated boron nitride nanocomposite
the formation of covalent bonds between the organic and (i.e. ≈ 8 pC at 600 s) and pure low-density polyethylene
inorganic phases [156]-[158][160][161]. Result obtained in (i.e. ≈ 27 pC at 600 s) [163].
this study was to reveal the improvement of electrical Yan et al. [156] also conducted a comprehensive study to
treeing resistance. investigate the dielectric breakdown strength of epoxy resin
Musa et al. [162] investigated the electrical tree filled with atmospheric pressure plasma-treated nano-silica.
performance and the effect of filler concentration of The configuration of the electrodes and the samples are
silicone rubber nanocomposites filled with atmospheric designed based on ASTM Standard D149.
pressure plasma-treated nanosilica. Atmospheric-pressure As mentioned, homogeneous nano-dispersion is the key
plasma was used to treat the silica nanofiller surfaces to for dielectric breakdown strength increase and reliable
enhance compatibility between the nanofiller and the results. Therefore, the primary purpose of plasma treatment
silicone rubber matrix. The result showed that plasma- is to improve the homogeneity dispersion of nano-silica
treated silica nanoparticles were uniformly well dispersed within the epoxy resin matrix by altering the surface
and formed strong covalent bonds with the molecules of the morphology of the nanofiller. Based on results, epoxy resin
silicone rubber [162]. The plasma-treated nanocomposites filled with plasma-treated nano-silica showed the highest
were able to resist the electrical treeing better than the breakdown strength at 63.2% of probability failure with 150
untreated nanocomposites. kV/mm breakdown strength, followed by epoxy resin filled
Yan et al. [156] experimented with investigating partial with untreated nano-silica (i.e., 125 kV/mm). In contrast,
discharge (PD) characteristics of epoxy resin the breakdown strength of unfilled epoxy resin is 55
nanocomposites filled with atmospheric pressure plasma- kV/mm [156].
treated nanosilica. Electrical tests showed improved partial Awang et al. [164] also studied the effect of alternating
discharge characteristics with plasma-modified nanofillers. current breakdown strength enhancement of low-density
In their study, partial discharge was measured using the polyethylene nanocomposites using atmospheric pressure
direct coupling detection method, where the charge plasma. In this study, the surfaces of boron nitride
nanoparticles were treated with atmospheric pressure
18
plasma discharge to strengthen the interface between the characteristic to improve the compatibility, which means
low-density polyethylene matrices and boron nitride overcoming the agglomeration issue. The hydrophilic
nanoparticles. The treatment of boron nitride nanofillers characteristic of nanoparticles can be obtained by treating the
was done in the plasma chamber, which applied a dielectric nanoparticle surfaces using plasma treatment. In fact, the
barrier discharge configuration system. The gap spacing effectiveness of this method still has not been emphasized by
was kept at 3 mm, and it was generated by a 50 Hz of any researchers in detail.
alternating current power supply with a maximum applied
voltage between 7 to 8.5 kVrms. Helium gas was used as
discharge gas with a flow rate of 1 litre/min, which was
applied inside the plasma chamber. The plasma power was
consumed at 3 to 15 W. The obtained results were analyzed
with 2-parameter Weibull distribution. Results showed that
the alternating current breakdown strength of the low-
density polyethylene nanocomposites is improved when the
nanofillers were modified using plasma treatment (i.e., 173
kV/mm at 63.2% of probability failure) as compared to the
untreated samples (i.e., 158 kV/mm at 63.2% of probability
failure) [164].
C. SUMMARY ON PLASMA MODIFICATION TECHNIQUE

TO ENHANCE INSULATION PROPERTIES
Based on the analysis of the various technical publications
presented in the previous section, a few conclusions
regarding the nanocomposite materials and plasma
treatment are drawn as follows in Table I. The majority of
presented studies focus on improving the insulation
properties of nanocomposite by manipulating the type and
percentage weight of nanoparticles. Thus, a promising
approach for the improvement purpose of nanocomposites
polymer is still required in terms of electrical tree
prolongation, partial discharge resistance, and breakdown
strength enhancement.
Despite various configurations of composition that have
been performed to investigate the insulation properties of
nanocomposite polymer, there is still a limited number of
publications, mainly using plasma treatment as an
alternative method to modify the molecular surface of
nanoparticles. It is only limited to intercalation and
coupling agent methods. Less attention is paid to plasma
treatment methods that can modify the surface morphology
of nanoparticles.
Existing plasma systems used to treat nanoparticle
surfaces are based on dielectric barrier discharge
configurations. This configuration is inefficient and not
suitable because it requires a complicated control system of
discharge gas. As many nanoparticles also flow out of the
treatment chamber with the flow of working gas, therefore
the quantity of remaining treated nanoparticles in the
treatment chamber would decrease. This drawback
indicates that the existing configuration of dielectric barrier
discharge is inefficient and needs to be improved.
Recently, research showed that the nanofiller with
appropriate compatibility of polymer matrices could improve
the performance of the nanocomposite insulation, especially
in terms of electrical tree prolongation, partial discharge
resistance, and dielectric strength enhancement. Thus, the
surface of nanoparticles should have a hydrophilic
19
20
TABLE I
SUMMARY STUDIES CONDUCTED TO ENHANCE INSULATION PROPERTIES OF NANOCOMPOSITES POLYMERS USING COLD PLASMA TECHNIQUE
Researchers (Polymer Host/ Nanofiller) Type of modification Type of experiment conducted Significant improvement
Friedrich et al. No Filler Low-pressure plasma with Material characterization - Maximum adhesion.
[165] -Polyethylene. a glow discharge - Able to functionalize C=C, C-O-, C-OH, C=O, and COOH
(1993) -Polypropylene. functional groups.
Shi et al. [166] No Polymer Plasma polymerization Surface morphology - Energetically stable polymorph.
(2002) Alumina coated ultra-thin Pyrrole.
Sanchis et al. [115] No Filler Low-pressure plasma Material characterization, ageing - Longer lifetime.
(2006) Low-density polyethylene test, crystallinity, & degradation - No significant effect on crystallinity.
temperature - Improve degradation temperature.
- Improve wettability.
- Promote polar species (Carbonyl, Carboxyl, & Hydroxyl).
Hosseini et al. Polyvinyl chloride: styrene- Plasma treatment Surface morphology & surface - Increase density of deposited nano-silver.
[167] butadiene (95:5)/Silver (Tetrahydrofuran) charge density - Highly uniform distribution of nano-silver.
(2010) - Enhance membrane potential, surface charge density, transport
number, perm selectivity.
Mukheriee et al. Epoxy resin/barium nitrate Plasma treatment Surface morphology - Improve interfacial region between inorganic (nanofiller) – organic
[168] (polymer matrix).
(2010) - Sufficiently strong to permit synthesis between inorganic-organic
compounds.
Huang et al. [169] Epoxy resin/ Plasma treatment Thermal conductivity - Increase thermal conductivity.
(2010) Mn3(Cu0.6Si0.15Ge0.25)N - Improve thermal stability.
Yan et al. [114] Epoxy resin/silane-coated silica Atmospheric pressure Dielectric strength & Electrical - Increase dielectric strength.
(2010) plasma treatment ageing - Extended electrical ageing.
Yan et al. [156] Epoxy resin/silica Low-pressure plasma Partial discharge, dielectric - Improve partial discharge endurance.
(2013) treatment strength, electrical ageing - Increase dielectric strength.
resistance, space charge, - Extended electrical ageing.
dielectric constant, & electrical - Reduce space charge accumulation.
treeing. - Increase dielectric constant.
- Reduce the rate of growth of electrical treeing.
Yan et al. [157] Epoxy resin/silica Plasma polymerization Electrical ageing, electrical - Longer endurance against electrical ageing.
(2013) coated by poly(ethylene treeing, dielectric constant, & - Delay initiation electrical treeing.
oxide) like film surface morphology. - Radial extent electrical treeing.
- Reduce dielectric constant over a wide range frequency.
- Better dispersion due to formation of C-O bond on filler-matrix.
Yan et al. [158] Epoxy resin/silica Atmospheric pressure Dielectric constant, dielectric - Lower dielectric constant at high frequency.
(2013) plasma treatment strength, & Electrical ageing. - Increase dielectric strength.
- Prolonged lifetime under high electrical stress.
21
Yan et al. [160] Epoxy resin/silica Plasma polymerization Surface morphology, electrical - Increase hydrophilicity.
(2014) coated by Poly(ethylene treeing, & dielectric constant - Improve dispersion uniformity.
oxide) like film - Enable anchoring sites to form covalent bonds between inorganic &
organic phases.
- Increase C-O bond on the nanofiller surface.
- Improve electrical treeing.
- Decrease dielectric constant.
Yan et al. [161] Epoxy resin/silica Plasma polymerization Electrical ageing, dielectric - Better resistance against electrical ageing.
(2014) coated by Poly(ethylene constant, & space charge. - Decrease dielectric constant.
oxide) like film - Mitigate space charge to built-up.
Musa et al. [162] Silicone rubber/silica Atmospheric pressure Electrical treeing & surface - Improve electrical treeing resistance.
(2016) plasma (dielectric barrier morphology. - Enhance compatibility between nanofiller-polymer matrices.
discharge) filamentary - Formed a strong covalent bond between nanofiller & polymer
molecules.
Kumar et al. [112] Ultra-high molecular weight Plasma treatment Surface morphology - Transform hydrophobic to hydrophilic due to carboxyl groups
(2016) polyethylene/multiwalled carbon (dielectric barrier bonded on nanofiller surfaces.
nanotube discharge) - Hydrophobic results in less contact with biological fluids during
physiological interaction.
- Reduce surface roughness.
Liu et al. Poly(3,4- Atmospheric pressure plasma. Surface morphology. - Reduce agglomeration.
[19] ethylenedioxythiophene)- Synthesize in an aqueous - Improve dispersibility and stability.
(2016) poly(styrene sulfonate)/titania solution.
Awang et al. [163] Low-density polyethylene/boron Plasma (dielectric barrier Partial discharge (CIGRE - Improve partial discharge (lower partial discharge magnitude).
(2017) nitride discharge) filamentary Method II)
Awang et al. [163] Low-density polyethylene/boron Plasma (dielectric barrier Alternating current dielectric - Increase alternating current dielectric breakdown strength.
(2017) nitride discharge) filamentary breakdown strength
Mathioudaki et al. No Polymer Low-pressure plasma Surface morphology - Reduce agglomeration.
[170] Zinc oxide, alumina Polymerization - More polarizable.
(2018) (Cyclopropylamine) - High hydrogen bond.
- Weaker electronegativity.
Awang et al. [164] Low-density polyethylene/boron Plasma (dielectric barrier Partial discharge & dielectric - Reduce the magnitude of average discharge.
(2019) nitride discharge) filamentary breakdown strength - Reduce the number of partial discharges.
- Increase dielectric breakdown strength.
VIII. CONCLUSION agglomeration issues as filamentary discharge, which directly

Plasma treatment is one of the methods that can be used to improves the insulation properties of nanocomposite
improve the dispersion of nanoparticles, nanocomposite polymers. However, producing cold plasma with a glow
bonding, and the compatible surface between polymer discharge mechanism is one of the major challenges in
matrices and nanoparticles. Incompatibility of molecular implementing plasma treatment. This is because various
surface between nanoparticle and polymer matrix causing factors need to be considered, especially producing a glow
the structure of nanocomposites to become weak, thus plasma discharge under atmospheric pressure conditions.
reducing the effectiveness of the merging process. The Therefore, an appropriate cold plasma system specifically
studies conducted in which employed the cold plasma
used to treat the surface of nanofiller is required to be
treatment on nanofiller surface highlighted the significant
developed by considering a few parameters such as optimum
improvement of insulation properties of nanocomposite
voltage, operation frequency, type and flow rate of discharge
polymers. Meanwhile, insulation properties of
nanocomposite polymer filled with plasma-treated gas, and the geometrical structure of atmospheric pressure
nanofillers compromising a better dielectric performance plasma reactor together with the treatment chamber.
compared to nanocomposite polymer filled with untreated Meanwhile, all configuration of parameters is important to
nanofiller. determine the type of plasma discharge, effectiveness, and
Besides, the ability of cold plasma to replace efficiency of plasma treatment on the surface of nanoparticles
conventional technique such as chemical functionalization in terms of qualitative and quantitative. In addition, cost-
and heat treatment seems to have a good potential due to effectiveness in developing a cold plasma system also needs
the impressive result and outcomes from the cold plasma to be considered since this system requires a disposable
treatment that almost hit the same and even better level of material that is a gas discharge to encourage the ionization
effectiveness in altering the surface morphology of process to occur.
nanofiller to overcome the agglomeration issue. Another challenge of the plasma release process is the lack
Specifically, the space charge, treeing lifetime (rate growth of previous reports related to the by-product formed from
of electrical tree), partial discharge resistance, and ionization of discharge gas, which may decompose to form
breakdown strength are the parameters promoted to be harmful molecules. Thus, this could be one of the trends for
enhanced through the surface modification of nanofiller future research directions on cold plasma in producing an
using cold plasma. All the characteristics of insulation eco-friendly surface modification technique.
mentioned are proven improved by introducing cold plasma Besides, there is still no subsequent study to identify a
treatment with filamentary and glow discharge mechanism comprehensive technique to control the coating process in
as a surface modification technique. terms of the type of chemical functional group that will be
In terms of discharge conditions, atmospheric pressure
functionalized through a particular specification of cold
plasma provides better effectiveness to functionalize
plasma treatment and its significant role in enhancing
chemical polar groups on the surface of nanofillers
insulation properties. Therefore, all the related factors, such
compared to low-pressure plasma. Previous studies have
as the type of discharge gas used, need to be acknowledged
shown that atmospheric pressure plasma treatment
successfully coats and functionalizes certain chemical so that the type of chemical functional group coated on the
functional groups such as the carbonyl and carboxyl groups. surface of nanofillers can be inferred based on the
In addition, atmospheric pressure plasma is preferred to be composition of discharge gas manipulated.
implemented, especially on the industrial scale, compared Furthermore, the future direction of cold plasma treatment
to low-pressure plasma due to the unnecessary vacuum in improving nanocomposite polymers also tends to
system. determine the most effective duration of plasma treatment,
The main challenges detailed out in this review are which is required to optimize the plasma time exposure.
performance-related issues that arise in the cold plasma to However, it depends upon the aims and objectives to be hit in
improve the insulating properties of polymer nanocomposites its application. Introducing cold plasma treatment on
as manuscripts were reviewed revealed the ability of cold nanocomposite technology also opens up the proliferation of
plasma in improving compatibility between nanoparticles research related to the type and optimum amount of plasma-
and the polymer matrix through the process of coating a treated nanofillers required to enhance the properties of nano-
certain chemical functional group on the surface of nanofiller composition based on its utilization.
before dispersing it into the polymer matrix. The
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coated on Nanoparticles to Improve Dielectric and Electrical
Insulation Properties of Nanocomposites,” IEEE Transactions on MOHD HAFIZI AHMAD is currently working as
Dielectrics and Electrical Insulation, vol. 21, no. 2, pp. 548–555, a senior lecturer and researcher at the Institute of
2014. High Voltage and High Current (IVAT), Universiti
[159] W. Yan, Z. J. Han, W. Z. Liu, X. P. Lu, B. Toan Phung, and K. Teknologi Malaysia (UTM). In IVAT UTM, he
Ostrikov, “Designing atmospheric-pressure plasma sources for serves as testing and calibration manager, and he is
surface engineering of nanomaterials,” Plasma Chem. Plasma also involved in many calibrations and testing jobs
Process., vol. 33, no. 2, pp. 479–490, 2013. related to high voltage equipment. He is also a
[160] W. Yan, B. T. Phung, Z. J. Han, and K. Ostrikov, “Plasma senior technical advisor for Global Testing Services (M) Sdn. Bhd. He
functionalization of SiO2 nanoparticles for the synthesis of polymer obtained PhD degree in High Voltage Engineering from Universiti
nano-dielectrics,” 2012, pp. 1–4. Teknologi Malaysia. His PhD works are related to partial discharge
[161] W. Yan, Z. J. Han, B. T. Phung, F. Faupel, and K. Ostrikov, “High- measurement in insulation. He was formerly a visiting researcher at the
voltage insulation organic-inorganic nanocomposites by plasma University of Leicester, UK. Moreover, he has conducted several trainings
polymerization,” Materials (Basel), vol. 7, no. 1, pp. 563–575, 2014. and lectures on partial discharge fundamentals and measurement on
[162] F. Musa, N. Bashir, M. Ahmad, Z. Buntat, and M. Piah, primary electrical equipment for industries and universities. He has
“Investigating the influence of plasma-treated SiO2 nanofillers on conducted field and laboratory partial discharge measurements for
the electrical treeing performance of silicone-rubber,” Appl. Sci. transformer, switchgear, cable, and rotating machines using conventional
(Basel), vol. 6, no. 11, p. 348, 2016. and non-conventional methods. He is a member of IEEE, CIGRE, and IET
[163] N. A. Awang, M. H. Ahmad, Y. Z. Arief, I. H. Zakaria, and N. A. UK.
Ahmad, “The effect of plasma-treated boron nitride on partial
discharge characteristics of LDPE,” Int. J. Electr. Comput. Eng.
(IJECE), vol. 7, no. 2, p. 568, 2017.
[164] N. A. Awang et al., “AC breakdown strength enhancement of LDPE ZOLKAFLE BUNTAT was born in Pontian,
nanocomposites using atmospheric pressure plasma,” in 2017 Johor, on July 26, 1964. He is a Retired Professor
International Conference on Electrical Engineering and Computer at the School of Electrical Engineering, Universiti
Science (ICECOS), 2017. Teknologi Malaysia. He received the Diploma in
[165] J. F. Hall, “History and bibliography of polymeric insulators for Electrical (Communication) in 1985, B. Sc in
outdoor applications,” IEEE trans. power deliv., vol. 8, no. 1, pp. Electronics and Electrical. Eng. degree from
376–385, 1993. University of Strathclyde, United Kingdom in
[166] D. Shi et al., “Interfacial particle bonding via an ultrathin polymer 1988 and M.E.E in High Voltage Insulator study
film on Al2O3 nanoparticles by plasma polymerization,” J. Mater. from Universiti Teknologi Malaysia, in 1996. In February 2005, he
Res., vol. 17, no. 5, pp. 981–990, 2002. completed his PhD in High Voltage and Pulsed Power Engineering from
[167] S. M. Hosseini, S. S. Madaeni, A. R. Khodabakhshi, and A. Loughborough University, United Kingdom. His teaching and research
Zendehnam, “Preparation and surface modification of PVC/SBR responsibilities are in the areas of Electrical Power Engineering, High
heterogeneous cation exchange membrane with silver nanoparticles Voltage Technology, Electrical Discharges, and Ozone Generation and
by plasma treatment,” J. Memb. Sci., vol. 365, no. 1–2, pp. 438– Technology. He had also given lectures at many high voltage short courses
446, 2010. for industries. He had also published many research papers in indexed
[168] N. Mukherjee, D. Wavhal, and R. B. Timmons, “Composites of journals and conferences. He is now a member of the International Ozone
plasma surface functionalized barium titanate nanoparticles Association (IOA), International Water Association (IWA), and IEEE
covalently attached to epoxide matrices: synthesis and evaluation,” Nuclear and Plasma Sciences Society. He also a member of the SIRIM
ACS Appl. Mater. Interfaces, vol. 2, no. 2, pp. 397–407, 2010. Technical Committee for IEC, TC 115 High Voltage Direct Current
[169] R. Huang, Z. Chen, X. Chu, Z. Wu, and L. Li, “Preparation and (HVDC) Transmission for DC Voltages above 100 kV. His research
thermal properties of epoxy composites filled with negative thermal interests include the generation of electrical discharges operating at
expansion nanoparticles modified by a plasma treatment,” J. atmospheric pressure, ozone generation, ozone application in medical,
Compos. Mater., vol. 45, no. 16, pp. 1675–1682, 2011. water, and wastewater treatment, rainwater harvesting, removal of NOx
[170] S. Mathioudaki et al., “Plasma treatment of metal oxide and SOx from diesel engine vehicles, the process of agriculture
nanoparticles: Development of core–shell structures for a better and produce and non-thermal plasma applications in medicine, environmental
similar dispersibility,” ACS Appl. Nano Mater., vol. 1, no. 7, pp. and agriculture.
3464–3473, 2018.
NORHAFEZAIDI MAT SAMAN was born in

Ipoh, Perak, On July 10, 1995. He received the B.
Eng. degree in electrical engineering from
Universiti Teknologi Malaysia (UTM), Malaysia,
in 2018. Currently, he is pursuing his PhD degree
in Electrical Engineering at Universiti Teknologi
Malaysia, Johor, Malaysia. He is focusing on the
plasma applications field and nanocomposite
insulations. He also explores the insulation diagnostic study for medium
and high voltage applications.
27

Application of Cold Plasma in Nanofillers Surface Modification For Enhancement of Insulation Characteristics of Polymer Nanocomposites: A Review

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Application of Cold Plasma in Nanofillers Surface Modification For Enhancement of Insulation Characteristics of Polymer Nanocomposites: A Review

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This article has been accepted for publication in a future issue of this journal, but has not been

Application of Cold Plasma in Nanofillers

Corresponding author: M H Ahmad (e-mail: [email protected]).

I. INTRODUCTION discharge resistance, and increase the dielectric breakdown

effectively treated nanocomposites insulating materials.

B. PHYSICAL STRUCTURE OF NANOFILLERS

dimensional, two-dimensional, or three-dimensional [36]. In contrast, graphene consists of a hexagonal

organic modification and solubilization methods. In the

C. LIMITATION OF PLASMA TREATMENT

C. SUMMARY ON PLASMA MODIFICATION TECHNIQUE

VIII. CONCLUSION agglomeration issues as filamentary discharge, which directly

[158] W. Yan, B. T. Phung, Z. J. Han, and K. Ostrikov, “Plasma Polymer-

NORHAFEZAIDI MAT SAMAN was born in

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