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A study on mechanical, thermal, and electrical properties of glass fiber-


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DOI: 10.1177/0021998313506242

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A study on mechanical, thermal, and electrical properties of glass fiber-reinforced epoxy hybrid
composites filled with plasma-synthesized AlN
Pravuram Panda, Gopa Mishra, Sisir Mantry, Saroj Kumar Singh and Swami Prasad Sinha
Journal of Composite Materials published online 15 October 2013
DOI: 10.1177/0021998313506242

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A study on mechanical, thermal, Reprints and permissions:
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and electrical properties of glass DOI: 10.1177/0021998313506242
jcm.sagepub.com
fiber-reinforced epoxy hybrid composites
filled with plasma-synthesized AlN

Pravuram Panda1, Gopa Mishra2, Sisir Mantry3,


Saroj Kumar Singh2 and Swami Prasad Sinha1

Abstract
Glass fiber-reinforced epoxy resin (GFRE) composites filled with aluminum nitride (AlN) powder were fabricated, and
their thermal and electrical properties were investigated. It is observed that with the increasing percentage of AlN
particles, there is a significant enhancement in thermal conductivity and micro-hardness, but there is a decline in tensile
strength. Experimental results demonstrate that the GFRE composites with 10 wt% of AlN loading show maximum
dielectric breakdown strength of 30.26 kV/mm with minimum volume resistivity of 7.5  1014
cm and thermal con-
ductivity value of 0.300 W/mK. Scanning electron microscopy studies were conducted to observe the voids and distri-
bution of filler in composites.

Keywords
Epoxy resin, plasma-synthesized AlN, glass fiber, hand-lay-up technique, GFRE composites

reduces compressive and shear forces on the surface of


Introduction the semiconductor. Very large-scale integration semi-
Polymer matrix composite (PMC) materials having conductor devices produce heat when they operate.
good mechanical strength and thermal conductivity To remove this heat, silica-filled epoxy resins are not
are widely used in various fields. Materials added to desirable for the encapsulation of silicon integrated cir-
the matrix help improving operating properties of a cuit (IC) chips because of low thermal conductivity of
composite. Glass fiber-reinforced polymer (GFRP) silica (1.4 W/mK); hence higher thermal conductivity
composites due to their high specific strength, stiff- fillers are being developed.9 Again, inclusion of glass
ness, corrosion resistance, and good dielectric fiber to the PMC enhances the mechanical, electrical,
properties have become attractive materials in aero- and thermal properties of the system significantly.10–13
space, automobile industries, marine, armor, microelec- Recently, aluminum nitride (AlN) has attracted much
tronic packaging, electronic circuit board, civil attention because of its unique combination of proper-
engineering structures, railways, sports goods, etc.1–6 ties like high thermal conductivity (320 W/mK),
Thermosetting epoxy resin based composites have
taken much attention because of its high thermal sta- 1
School of Applied Sciences (Physics), KIIT University, India
bility, moisture resistance, and low cost. Unfortunately, 2
Advanced Materials Technology Department, CSIR-Institute of Minerals
cured epoxy has low thermal conductivity and high and Materials Technology, India
coefficient of thermal expansion coefficient (CTE).7 3
Surface Engineering Department, CSIR-Institute of Minerals and
Generally, thermal expansion of epoxy is lowered by Materials Technology, India
reinforcing ceramic powders such as fused silica or
Corresponding author:
quartz to more closely match that of the encapsulated Pravuram Panda, School of Applied Sciences (Physics), KIIT University,
metal lead frames and semiconductor dies.8 This pre- Patia, Bhubaneswar 751024, India.
vents damage to the device from thermal cycling and Email: pravuram.panda@gmail.com
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2 Journal of Composite Materials 0(0)

high dielectric breakdown strength, high electrical Table 1. Plasma operating parameters adopted in
resistivity (>1016 Vm), low dielectric constant (8.8 at extended arc thermal plasma reactor.
1 MHz), and low CTE which is close to that of silicon
Plasma operating parameters
and good corrosion resistance.14,15 Hence, the use of
AlN powder in glass fiber-reinforced epoxy resin DC load voltage (V) 50
(GFRE) composite enhances its thermal, electrical, Arc current (Ampere) 300
and mechanical properties to a large extent. NH3 gas flow rate (l/min) 2
Considerable work has been reported by many Ar gas flow rate (l/min) 1
researchers based on the study of thermal, mechanical, Reaction time (min) 25
and electrical properties of epoxy composites filled with Electrode spacing (cm) 5
nano- or micron-sized AlN filler.9,16–21 Rarely work
was explored on the same study about the glass fiber-
reinforced epoxy/AlN hybrid composite. The cost of
nano AlN powder in the international market is also atmosphere of ammonia (2 l/min) and argon (1 l/min)
too high, hence designing PMC using micron-sized cer- in an extended arc DC thermal plasma reactor (50 kW)
amic powder with good physical, mechanical, and elec- for a pre-optimized time of 25 min. The adopted plasma
trical properties is a challenge. operating condition was given in Table 1. The length of
In view of above, in our laboratory, we synthesized the arc was adjusted by moving the top electrode
fine AlN powders using thermal plasma technology via (anode) up and down by a rack and pinion arrange-
carbothermal reduction–nitridation process in an indi- ment. Ar gas helps in the formation and stabilization of
genously developed extended arc thermal plasma reac- plasma arc, and it also maintained in a protective
tor. Using the plasma-synthesized AlN powder, GFRE atmosphere inside the hearth. The gas flow was contin-
composite slabs were fabricated by conventional hand- ued even after the plasma treatment of the granules till
lay-up technique followed by light compression mould- the hearth was sufficiently cooled to prevent oxidation
ing technique. The main objective of the present study of the product. The solid–solid reaction between
is to develop the mechanical, thermal, and electrical a-Al2O3 and activated charcoal in NH3 plasma via car-
properties of GFRE resin composite using plasma- bothermal reduction process resulted fine AlN powder
derived fine AlN powder as filler material. with little unreacted carbon. After the synthesis of AlN
powder, unreacted free carbon was removed by heating
the plasma yield product in a muffle furnace at 700 C
Experimental procedures for 2 h in air. The detail of the powder synthesis method
and reaction mechanism involved was described in
Materials detail elsewhere.22
Low temperature curing epoxy resin (DGEBA, grade-
LY 556, density 1.15 gm/cc at 25 C), an aliphatic
Composite slab fabrication
amine-based hardener (HY951, Triethelene Tetra
Amine, density 0.98 gm/cc at 25 C, supplied by Ciba A weighed amount of epoxy resin and plasma-
Geigy Ltd., India), and bi-directional woven roving synthesized AlN powders were taken in a beaker and
E-glass fibers (having modulus 72.5 GPa, density mixed thoroughly with the help of a high speed stirrer
2.59 gm/cc at 25 C, Saint Gobain Ltd., India) were before the respective fiber mats were reinforced into the
used for the preparation of GFRP matrix composite matrix body. The mixture was kept in a vacuum oven at
system. Alumina (a-Al2O3, purity—99.5%, Median 30 C for 30 min to avoid air trapped into the mixture.
diameter—4 mm, Grade-NSPL 20, NALCO, India) Then a hardener was added to the mixture at 1:10
and activated charcoal (Carbon content—81.3%, weight ratio of the resin, as recommended.23
MERCK, India) were used for the preparation of Composite slabs with particulate fillers (AlN) of three
AlN powder in our laboratory. different amounts (5, 10, and 15 wt%, respectively) with
fixed glass-fiber loading (50 wt%) were fabricated by
conventional hand-lay-up technique followed by light
Preparation of AlN from alumina compression moulding technique. A stainless steel
Alumina (a-Al2O3) and activated charcoal powders mould having dimension of 210  210  40 mm3 was
were mixed in the weight ratio of 5:3 with dextrin as used. The cast of each composite was cured under a
a binder and small granules (1–3 mm diameter) were load of 50 kg for 24 h before it was removed from the
prepared. The moisture present in granules was then mould. In order to achieve further better performance,
removed by heating at 100 C for 5 h on a hot plate. the composites were then post cured at 80 C for 2 h and
The dried granules were plasma-treated in the 100 C for 4 h in an oven and allowed to cool gradually
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Panda et al. 3

The uniaxial tensile test was performed on flat spe-


cimens (dog-bone specimen and straight side specimen
with end tabs) as per ASTM standard D 3039-76. The
dimension of the test section was 200  10  3 mm.
The tensile test was performed in the universal testing
machine (UTM) Instron 1195.
The differential scanning calorimeter (Model:
MDSC Q100, TA, USA), was used to analyze the influ-
ence of AlN content on the glass transition temperature
(Tg) of the GFRE composite samples. The measure-
ments were conducted in a N2 atmosphere (flow
rate—50 ml/min), varying temperature from 20 C to
300 C at a heating rate of 10 C/min using a standard
aluminum pan.
Thermal conductivity was measured using Unitherm
Model 2022, Anter Corporation, Pittsburgh, PA, USA.
The thermal conductivity of samples was measured at
Figure 1. X-ray diffraction of fine AlN particle synthesized by
room temperature in the air following ASTM E1530
themal plasma process.
standard. The specimens for thermal conductivity
measurement were made in the form of circular discs
to room temperature. Specimens of suitable dimension with 3 mm in thickness and 50 mm in diameter.
were cut using a diamond cutter for physical character- Thermo gravimetric analysis was carried out by
ization and mechanical testing. Utmost care was taken using TGA/SDTA 851 e, METTLER TOLEDO to
to maintain the uniformity and homogeneity of the dif- analyze the influence of AlN content on the thermal
ferent specimens of the composites. stability of the GFRE composite samples. The meas-
urements were carried out in air/N2 atmosphere from
28 C to 700 C, at a heating rate of 20 C/min.
Characterization
The AC dielectric breakdown strength was measured
The phase and crystallinity of the as-synthesized prod- using OTS-100 AF/2, alternating current dielectric
uct was determined by X-ray diffraction with mono- strength tester (Meggera OTS, UK) in accordance
chromatic Cu Ka radiation with Ni filter (Phillips, with ASTM D 149-2004. Specimen of 50 mm diameter
Model: PW 3020). The X-ray diffraction pattern of and 3 mm thickness was placed between two 10-mm
carbon free AlN powder is given in Figure 1. The diameter copper ball electrodes. The electrode system
microstructure and elemental analysis of the obtained containing the specimen was immersed in the pure sili-
powder was performed by FE-SEM equipped with cone oil to prevent the surface flashover. The test volt-
EDAX (ZEISS SUPRA 55) as shown in Figure 2. age was applied across two ball-typed electrodes and
The densities of the composites were measured by was increased until the sample was punctured. Five
adopting simple water immersion technology which is breakdown tests were repeatedly performed on each
depicted in Table 2. specimen. Voltage breakdown values were measured
Micro hardness measurement was carried out using and printed at a resolution of 0.1 kV. All of the meas-
a Leco micro hardness tester. A diamond indenter, in urements were performed under the same humidity and
the form of a right pyramid with a square base and an room temperature.
angle 136 between opposite faces, was forced into the The DC volume resistivity measurements are per-
material under a load F. The two diagonals X and Y of formed using Ultra Megaohm Meter (SM-8220,
the indentation left on the surface of the material after HIOKI Corporation, Japan) by supplying 1 kV for
removal of the load were measured, and their arith- 60 s using in accordance with ASTM D 257. Square
metic mean L was calculated. In this study, the load samples of 100  100  8 mm3 were taken for measure-
considered F ¼ 0.5 N and Vickers hardness number ment of the resistivity in the samples. Five tests were
was calculated using the following equation. repeatedly conducted for each specimen. All the tests
were conducted at room temperature and same humid-
HV ¼ 1:889ðF=L2 Þ ð1Þ ity. The corresponding resistivity was calculated using
the formula:
where L ¼ (X þ Y)/2, F is the applied load (N), L is the
diagonal of square impression (mm), X is the horizontal
length (mm), and Y is the vertical length (mm). rv ¼ ð19:6  Rv Þ=t ð2Þ
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4 Journal of Composite Materials 0(0)

Figure 2. FESEM image and its corresponding EDAX spectrum of plasma synthesized hexagonal AlN powder.

Table 2. Density and void volume fraction of the PMCs filled with glass fiber and different wt% of
plasma-synthesized AlN powder.

Measured Theoretical Volume


density density fraction of
Composition (gm/cc) (gm/cc) voids (%)

Neat epoxy 1.150 1.150 0


Epoxy þ 50 wt% glass fiber 1.535 1.544 0.56
Epoxy þ 5 wt% AlN þ 50 wt% glass fiber 1.591 1.619 1.75
Epoxy þ 10 wt% AlN þ 50 wt% glass fiber 1.660 1.702 2.50
Epoxy þ 15 wt% AlN þ 50 wt% glass fiber 1.733 1.794 3.50

where, rv, Rv, t, and 19.6 are volume resistivity in


cm, Results and discussion
corresponding volume resistance in
, average thick- Structural and morphology of plasma-synthesized
ness of specimen in cm, and constant for the apparatus,
AlN powder
respectively.
The morphology and distribution of filler particles in Figure 1 shows the XRD pattern of AlN powder
the fractured surface of tensile samples of GFRE com- synthesized in thermal plasma. All the peaks are attrib-
posites were carried out on scanning electron micro- uted to hexagonal AlN and good agreement with
scope (SEM) (Model: JSM-7000F, JEOL, Japan). The JCPDS index card no. 25-1133. The degree of crystal-
fracture surfaces were cleaned with alcohol in order to linity of the plasma-synthesized product is high as all
eliminate impurities such as dust before test. In order to the diffraction peaks are sharper with high intensity.
improve conductivity, the samples were sputtered with FESEM picture shows (Figure 2) that the synthesized
gold in vacuum prior to observation. The observation AlN particles are fine, spherical shaped, well faceted,
was carried out to study the distribution of filler par- and loosely agglomerated. The EDS profile of the as-
ticles in GFRP matrix. produced AlN powder shows the presence of aluminum
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Panda et al. 5

and nitrogen at 1.5 and 0.4 keV, respectively. A small


peak at 0.5 keV shows very little oxygen impurity,
which may come from the surface contamination with
moisture present in the air.

Density of composites
The density of a composite depends on the relative
proportion of matrix and reinforcing materials,
and this is one of the most important factors determin-
ing the properties of the composites. The theoretical
densities of samples were calculated based on the dens-
ity of AlN, epoxy, and glass fiber as 3.255, 1.15, and
2.590 g/cm3, respectively, according to the following
equation: Figure 3. Variation of density and void fraction in composites
with different wt% of plasma synthesized AlN powder.
1
ct ¼ w w wp ð3Þ
f m
þ þ
f m p

where W and  represent the weight fraction and dens-


ity, respectively. The suffix f, m, ct, and p stand for the
fiber, matrix, composite materials, and particulate filler
materials, respectively. The actual density ce of the
composite, however, can be determined experimentally
by simple water-immersion technique. The volume frac-
tion of voids Vv in the composites was calculated using
the following equation:

ct  ce
Vv ¼ ct
ð4Þ

The theoretical and measured densities of the compos-


Figure 4. Variation of micro-hardness and tensile strength of
ites along with the corresponding volume fraction of the GFRE composites filled with with different wt% of plasma
voids are presented in Table 2. It is clearly seen that synthesized AlN powder.
the incorporation of glass fiber in the neat epoxy creates
the void fraction in the composite. With the addition of
AlN as the filler material, more voids are found in the
composites. As the filler content increases from 5 wt%
Micro-hardness and tensile strength of GFRE matrix
to 15 wt%, the volume fraction of voids is found to be The variation of micro-hardness and tensile strength of
increased. The void content is the cause for the differ- GFRE composites as a function of weight fraction of
ence between the values of measured density and the AlN particulates is given in Figure 4. It was observed
theoretically calculated one. It has also been clearly that, with the incorporation of filler particulates into
seen in Figure 3 that, with the increase in filler content, the composites, the mean hardness improves signifi-
there is an increase in density. However, more addition cantly. Neat epoxy shows the average hardness of
of filler to matrix may create more voids, which may 13.7 HV. As the percentage of AlN increases, the hard-
affect on the mechanical, thermal, and electrical proper- ness of composite increases signiEcantly and 15 wt% of
ties of composites. The knowledge of void content is AlN-Elled epoxy composite shows the maximum hard-
desirable for estimation of the quality of the compos- ness of 35 HV. This may be attributed to the pressing of
ites. It is understandable that a good composite should hard AlN particles into polymeric matrix phase and
have fewer voids. Higher void contents usually mean making intimate contact with each other so that the
lower fatigue resistance, weathering, and greater sus- interface can transfer load more effectively. Moreover,
ceptibility to water penetration.24 However, the pres- relatively uniform distribution of AlN particles and
ence of void is unavoidable in composites especially decrease in inter particle distance with increasing par-
made by the hand-lay-up technique. ticle loading in the matrix results in an increase of
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6 Journal of Composite Materials 0(0)

resistance to indentation of epoxy matrix. This can also


be attributed to the surface coating of AlN particles
with a Elm of the matrix which prevents the direct par-
ticle–particle contact.
It was observed that as the content of the AlN par-
ticles increases, the tensile strength of composite
declines gradually. There can be two reasons for this
decline in the strength of these particulate filled com-
posites. One is that interfacial adhesion between AlN
particles and the matrix may be too weak to transfer
the tensile stress; the other is that the irregular shaped
AlN particles act as stress raisers in the polymer matrix.
Further, it can be explained as follows: under the action
of tensile force, the Eller matrix interface is vulnerable
to bonding, depending on interfacial bond strength and
this may lead to a break in the composite.

Thermal conductivity, glass transition temperature


(Tg) and thermal stability
The thermal conductivity values of GFRE composite
are shown in Figure 5(a). It shows that with the inclu-
sion of plasma-synthesized AlN filler in GFRE com-
posites, the thermal conductivity value increases
significantly. At 5 wt% of AlN filler loading, the ther-
mal conductivity of GFRP composite shows 0.241 W/
mK and it increases to 0.300 W/mK at 10 wt% of load-
ing, which is 2.11 times of neat epoxy and it subse-
Figure 5. Variation of (a) Thermal conductivity and (b) flow of
quently increases to 0.322 W/mK with 15 wt% of AlN
heat in PMC filled with glass fiber and different wt% of plasma
loading, which is 2.25 times of neat epoxy. The filler
synthesized AlN filler.
particles with low volume fraction may disperse ran-
domly into epoxy matrix resulting weak interaction
that leads to have marginal increase in thermal con- The TGA curves for GFRP composite are illustrated
ductivity. As the Eller loading increases, the particles in Figure 6. There is an obvious increase in the thermal
begin to touch each other and form a partial conductive stability of epoxy with increasing AlN concentration.
path or network which enhances heat conductance. The reason may be ascribed to the higher heat capacity
Thermal conductivity of glass fiber is larger than the 0.738 Jg1 C1 of AlN, as compared to epoxy resin and
epoxy.25 The direction and length of glass fiber also high thermal conductivity of 170 W/mK, compared to
make a continuous path for phonons to transfer heat. 0.142 W/mK of neat epoxy. The inclusion of high ther-
Hence, reinforcement of glass fiber not only increases mal conductive AlN and glass fiber in epoxy is used to
mechanical properties but thermal conductivity too. absorb the heat. So, this will result in epoxy chains
The DSC curves of neat epoxy, glass fiber-reinforced starting to degrade at a higher temperature.
epoxy composite, and GFRE matrix with different wt %
AlN filler (5, 10, and 15 wt%) composites are plotted in
Dielectric breakdown strength
Figure 5(b). The thermogram shows the endothermic
glass transition temperature of neat epoxy at 66.53 C. Dielectric breakdown strength is defined as the highest
It can be observed that reinforcement of glass fiber and voltage which samples can stand before they fail elec-
AlN powder into epoxy does not seem to have appre- trically, divided by sample thickness. Break down of
ciable inFuence on the Tg. However, at 15 wt% AlN polymer dielectrics is affected by several factors such
loading, Tg reduced to 64.8 C. The decrease in Tg may as degree of crystallinity, accumulation of bulk
be due to the decrease in the polymer matrix interaction charge, interfacial area, temperature, types of bonding,
and formation of agglomeration of AlN particles in the and free volume.27 Figure 7 shows the AC dielectric
composites.26 The agglomeration or cluster formation breakdown strength of neat epoxy and GFRE compos-
occurs at higher filler loading which is visible in SEM ites at variable AlN loading. It is evident that break-
micrograph (Figure 9d) of composites. down strength of neat epoxy varies accordingly with the
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Panda et al. 7

Figure 6. TGA curves of neat epoxy and GFRE composites Figure 8. Variation of volume resistivity of PMC filled with glass
filled with different wt% of plasma synthesized AlN powder. fiber and plasma synthesized AlN powder with different wt%.

field at any point and alteration of space charge distri-


bution.28 The bonding between filler particles and
epoxy matrix would lead to form denser structure,
which might limit the mobility of matrix backbone
leading to increase in the dielectric breakdown
strength.20 Here, the number of particles in the com-
posite is more, resulting in smaller inter-particle dis-
tance; hence, the volume fraction of loose polymer
layer reduces and the particles themselves act as bar-
riers to flow of current between the electrodes. These
factors contribute to oppose in the flow of current
in the composite, resulting in higher break down
voltage.18 At higher filler content, i.e. 15 wt% of AlN
loading, the dielectric breakdown strength again
decreases marginally to 22.34 kV. This may be attribu-
Figure 7. Variation of dielectric breakdown strength of PMC ted to the formation of agglomeration of fine AlN par-
filled with glass fiber and plasma synthesized AlN powder with ticles in the GFRE composites that result in defects
different wt%. such as voids.17

reinforcement of glass fiber and AlN powder. At


50 wt% of glass fiber loading, the breakdown strength
Volume resistivity
increases marginally up to 20.55 kV, whereas neat Figure 8 shows the variation in the DC volume resist-
epoxy shows only 11.88 kV. However, at filler concen- ivity of neat epoxy and GFRE composites at variable
tration of 5 wt%, the break down strength of the com- wt% of AlN filler. Neat epoxy shows a resistivity value
posite remains almost the same as the GFRE of 3.31  1015 V cm which decreases with the incorpor-
composite. This behavior is probably because at lower ation of glass fiber and plasma-synthesized fine AlN
concentration of filler, the number of AlN particles is powder. As glass fiber sheets were layer wise sand-
less, the interparticle distances are more, and the wiched in epoxy, it does not significantly affect on the
volume fraction of the loose polymer layer is large volume resistivity, as the conduction path through the
under the condition of high electric stress, and a large epoxy is obstructed by laminated glass fiber sheets
fraction of those polymer layer allows the transfer of which result in a small increase in volume resistivity.29
charge carrier between the electrodes thereby loading to The 50 wt% of glass fiber reinforcement in neat epoxy
lower or marginally same breakdown voltage as the shows the volume resistivity value of 8.51  1015
cm.
epoxy.18 At 10 wt% of AlN loading, the composite However, a 5 wt% incorporation of plasma-synthesized
shows maximum dielectric breakdown strength of fine AlN particles to the GFRE reduces the resistivity
30.26 kV. The reason may be due to high packing dens- value to 3.01  1014 V cm. This behavior indicates that
ity, reduced accumulated charge and reduced threshold at lower filler loading, the fraction of extended loose
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8 Journal of Composite Materials 0(0)

Figure 9. Microstructure of tensile fractured GFRE composites with (a) 0, (b) 5, (c) 10 and (d) 15 wt% of plasma synthesized AlN
powder.

polymer and glass fiber layers is high, which probably 15 wt% plasma-synthesized AlN powder, respectively.
allows the existence of free ions and also their unhin- It is evident from Figure 9(a) that the layers of polymer
dered transport through the bulk of the material result- and bidirectional glass fiber staked one over another
ing in an increase in the electrical conductivity through with good bonding. Lateral view of the tensile fractured
the volume of the material. However, with the increase glass fiber can be observed in Figure 9(a) and (b). It is
in AlN loading up to 10 wt%, immobilized polymer evident that glass fibers are well embedded in epoxy
chains act as ion traps, which inhibit the ion mobility which improves the mechanical properties of the com-
and the flow of electrons, thereby resulting in a decrease posites. There is no observation of AlN particles in the
in the overall conductivity values, i.e. an increase in micrograph of GFRE composite filled with 5 wt% of
volume resistivity.18 Furthermore, incorporation of AlN because of low filler concentration and well dis-
AlN (i.e. at 15 wt%) leads to the reduction in volume persion of the filler particles in epoxy. As the concen-
resistivity as filler makes partial interconnections tration of AlN increases up to 10 wt%, the formation of
between the particles lead to the margin decrease of voids started (Shown in Figure 9 (c)), which affects the
volume resistivity of GFRE composite system. Similar mechanical, electrical, and thermal properties of the
type of observation was observed in a previously composites. In 15 wt% of the AlN loading, agglomer-
reported paper related to the influence volume resistiv- ation/clusters of AlN particles were formed inside the
ity of epoxy/nano alumina composites on the filler composite which is shown in Figure 9(d). There is no
percentage.30 observation of particle-matrix debonding and micro-
cracks on the surface of the composites, which suggest
a relatively strong interfacial bonding and good com-
patibility of AlN particles with the epoxy matrix. This
Fracture surface morphology
further corroborates the enhancement of thermal con-
Figure 9(a) to (d) shows the morphology of the tensile ductivity, mechanical, and electrical property of GFRE
fractured GFRE matrix composite with 0, 5, 10, and matrix with AlN filler.
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3. Lu S, Ban J and Liu K. Preparation and characterization


Conclusions of liquid crystalline polyurethane/Al2O3/epoxy resin com-
The following conclusions may be summarized from posites for electronic packaging. Int J Polym Sci 2012;
the studies: 728235: 1–4.
4. He Y, Moreira BE, Overson A, et al. Thermal character-
ization of an epoxy-based underfill material for flip chip
1. The density and volume fraction of voids in the packaging. Thermochim Acta 2000; 357: 1–8.
GFRE composites increases simultaneously with 5. Ratna D, Chongdar TK and Chakraborty BC.
the incorporation of plasma-synthesized AlN Mechanical characterization of new glass fiber reinforced
powder. epoxy composites. Polym Comp 2004; 25: 165–171.
2. The hardness of GFRE composites increases with 6. Kchaou B, Turki C, Salvia M, et al. Dielectric and fric-
the inclusion of plasma-synthesized AlN filler, but tion behaviour of unidirectional glass fibre reinforced
the tensile strength decreases simultaneously. epoxy (GFRE). Wear 2008; 265: 763–771.
3. Inclusion of plasma-synthesized AlN particles into 7. Kim W, Bae JW, Choi ID, et al. Thermally conductive
GFRE composites improves its thermal stability sig- EMC for microelectronic encapsulation. Polym Eng Sci
nificantly, whereas no appreciable inFuence on the 1999; 39: 756–766.
8. Weltevreden ER, Tesarski SJ, Wymyslowski A, et al.
glass transition temperature of epoxy.
A multi-scale approach of the thermo-mechanical proper-
4. Thermal conductivity of the GFRE composites
ties of silica-filled epoxies used in electronic packaging.
increases up to 0.300 W/mK at 10 wt% of AlN Microelectron Reliab 2012; 52: 1300–1305.
filler loading with good mechanical and electrical 9. Lee ES, Lee SM, ShaneEeldz DJ, et al. Enhanced thermal
properties. conductivity of polymer matrix composite via high solids
5. The dielectric breakdown strength increases grad- loading of aluminum nitride in epoxy resin. J Am Ceram
ually up to 30.26 kV at 10 wt% of AlN loading in Soc 2008; 91: 1169–1174.
GFRE composites. 10. Kchaou B, Turki C, Salvia M, et al. Role of fibre–matrix
6. The volume resistivity of GFRE composites increase interface and fibre direction on dielectric behaviour of
with the reinforcement of glass fiber but decreases epoxy composites. Compos Sci Technol 2004; 64:
with loading of AlN filler up to 5 wt% and again it 1467–1475.
11. Kechaou B, Salvia M, Benzarti K, et al. Fiber-reinforced
increases marginally up to 10 wt% of loading. At 15
epoxy composites role of fiber/matrix interphases on
and 5 wt% of AlN filler loading, the volume resist-
dielectric, friction, and mechanical properties of glass.
ivity values are approximately same. J Compos Mater 2011; 46: 131–144.
12. Fouad Y, El-Meniawi M and AEE A. Erosion behaviour
of epoxy based unidirectional (GFRP) composite mater-
Acknowledgements ials. Alexan Eng J 2011; 50: 29–34.
This work was supported by the Institute of Minerals and 13. Cugnet D, Hauviller C, Kuijper A, et al. Thermal con-
Materials Technology (CSIR), Bhubaneswar and KIIT ductivity of structural glass/fibre epoxy composite as a
University, Bhubaneswar. The authors are grateful to the function of fibre orientation. In: 19th international cryo-
Director, IMMT, Bhubaneswar, India and Vice-Chancellor, genic engineering conference (ICEC 19), European
KIIT University, Bhubaneswar, India for providing research, Organization for Nuclear Research. Large Hadron
library, and computational facilities. Collider Project Report, Report no. 613, Grenoble,
France, 2002.
Funding 14. Mussler BH. Advanced materials and powders–alumin-
ium nitride (AlN). Am Ceram Soc Bull 2000; 79: 45–47.
This research received no specific grant from any funding
15. Molisani AL and Yoshimura HN. Low-temperature
agency in the public, commercial, or not-for-profit sectors.
synthesis of AlN powder with multicomponent additive
systems by carbothermal reduction–nitridation method.
Conflict of Interest Mater Res Bull 2010; 45: 733–738.
None declared. 16. Xu Y and Chung DDL. Increasing the thermal conduct-
ivity of boron nitride and aluminium nitride particle
epoxy-matrix composites by particle surface treatments.
References Compos Interf 2000; 7: 243–256.
1. Yung KC, Zhu BL, Wu J, et al. Effect of AlN content on 17. Peng W, Huang X, Yu J, et al. Electrical and thermophy-
the performance of brominated epoxy resin for printed sical properties of epoxy/aluminum nitride nanocompo-
circuit board substrate. J Polym Sci Part B: Polym Phys sites: effect of nanoparticle surface modification. Compos
2007; 45: 1662–1674. Part A 2010; 41: 1201–1209.
2. Toldy A, Szolnoki B and Marosi GY. Flame retard- 18. Choudhury M, Mohanty S, Nayak SK, et al. Preparation
ancy of fibre-reinforced epoxy resin composites for and characterization of electrically and thermally con-
aerospace applications. Polym Degrad Stab 2011; 96: ductive polymeric nanocomposites. J Min Mater
371–376. Charact Eng 2012; 11: 744–756.
XML Template (2013) [8.10.2013–2:07pm] [1–10]
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10 Journal of Composite Materials 0(0)

19. Ma A, Chen W, Hou Y, et al. The preparation and 25. AL-Hassani ES. Effect of UV radiation on dielectric con-
cure kinetics researches of thermal conductivity stant and thermal conductivity in epoxy phenol blends.
epoxy/AlN composites. Polym-Plast Technol 2010; 49: Eng Tech J 2010; 28: 1982–1989.
354–358. 26. Vassileva E and Friedrich K. Epoxy/alumina nanoparti-
20. Wu CC, Chen YC, Yang CF, et al. The dielectric proper- cle composites. I. Dynamics mechanical behavior. J Appl
ties of epoxy/AlN composites. J Eur Ceram Soc 2007; 27: Polym Sci 2003; 89: 3774–3785.
3839–3842. 27. Sarathi R, Sahu RK and Rajeshkumar P. Understanding
21. Yu JH, Duan JK, Peng WY, et al. Influence of nano-AlN the thermal, mechanical and electrical properties of epoxy
particles on thermal conductivity, thermal stability and nanocomposites. Mater Sci Eng A 2007; 445–446:
cure behavior of cycloaliphatic epoxy/trimethacrylate 567–578.
system. eXPRESS Polym Lett 2011; 5: 132–141. 28. Mohanty A and Srivastava VK. Dielectric breakdown
22. Panda P, Singh SK and Sinha SP. Structural and optical performance of alumina/epoxy resin nanocomposites
properties of AlN synthesized by plasma technique. Inter under high voltage application. Mater Design 2013; 47:
J Mater Sci 2010; 5: 677–682. 711–716.
23. Jha AK, Mantry S, Satapathy A, et al. Erosive wear per- 29. Kupke M, Wentzel HP and Schulte K. Electrically con-
formance analysis of jute-epoxy-SiC hybrid composites. ductive glass fibre reinforced epoxy resin. Mater Res
J Comp Mater 2010; 44: 1623–1641. Innovat 1998; 2: 164–169.
24. Agarwal BD and Broutman LJ. Analysis and performance 30. Yu J, Huo R, Wu C, et al. Influence of interface structure
of fiber composite, 2nd ed. New York, NY: John Wiley on dielectric properties of epoxy/alumina nanocompo-
and Sons, Inc. sites. Macromol Res 2012; 20: 816–826.

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