Composites: Part A 42 (2011) 14321437

Contents lists available at ScienceDirect

Composites: Part A
journal homepage: www.elsevier.com/locate/compositesa

Properties of spin coated epoxy/silica thin lm composites: Effect

of nano- and micron-size llers
Evon Foo a, Mariatti Jaafar a,, Azizan Aziz a, Lim Chong Sim b
a
b

School of Materials and Mineral Resources Engineering, Engineering Campus, Universiti Sains Malaysia, 14300 Nibong Tebal, Seberang Perai Selatan, Pulau Pinang, Malaysia
Intel Technology Sdn. Bhd., Kulim Hi-Tech Park, 09000 Kulim, Kedah Darul Aman, Malaysia

a r t i c l e

i n f o

Article history:
Received 11 March 2011
Received in revised form 15 June 2011
Accepted 21 June 2011
Available online 28 June 2011
Keywords:
A. Nano-structures
A. Thin lms
B. Thermal properties
E. Thermosetting resin

a b s t r a c t
With the increasing interest in high density electronics packaging, dimensional scaling becomes the key
to evolution. Low coefcient of thermal expansion (CTE) thin lm composites with silica llers were fabricated using spin coating. In comparison with the conventional thin lm fabrication, spin coating has the
ability to control lm thickness and uniformity. In this paper, the mechanical and thermal properties of
the thin lm composites using micron-silica and nano-silica were compared. The 2 wt% nano-silica thin
lm composite was found to have the lowest CTE and is able to achieve an equivalent tensile strength
compared with the 15 wt% micron-silica thin lm composite. The 2 wt% nano-silica samples also gave
an equivalent thermal stability as compared with that of the 30 wt% micron-silica. Hence, with the higher
surface area to volume ratio, nano-silica shows its capability to achieve a substantial performance with a
lower weight fraction compared with l-Si.
2011 Elsevier Ltd. All rights reserved.

1. Introduction
Changes in the innovative material have become a potential
issue for scaling other than the changes in chip manufacturing. A
good packaging caters to the ever-increasing demand of the miniaturization in the electronics industry. Hence, the evolution of
packaging from bulk packaging to thin lm packaging takes place
in line with Moores law. According to ASTM D 882-02, a material
is considered a thin lm when its thickness is less than 0.25 mm.
With the easier processing of polymers, a exible and thin polymer
lms are made possible. Previously, polymer thin lms has only
been used in technological applications ranging from multicolor
photographic printing to paints, adhesives, index-matched optical
coatings and photoresists [1]. Apart from that, the compatibility
of polymers with different inorganic llers has made the composite
thin lm versatile in their electrical and thermal properties. The
reinforced composite thin lms had been widely used in the
electronic application such as sensor [2], solar panel [3] and touch
panel [4]. Other than that, the demand on low cost, exible and
light weight devices has also promoted the development of excircuit technology where the polymer thin lm used as printable
materials for electronic packaging [5].
In polymer thin lm fabrication, the conventional methods,
such as dip coating, solution casting, and hot press are widely used.
Although these methods involve a lower cost and a simpler
Corresponding author. Tel.: +60 4 5995262; fax: +60 4 5941011.
E-mail address: mariatti@eng.usm.my (M. Jaafar).
1359-835X/$ - see front matter 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.compositesa.2011.06.007

processing method, the lack of uniformity and the uncontrollable

lm thickness become an issue for precision fabrication. In line
with packaging development, the spin coating method, commonly
used in photoresist applications in the semiconductor industry, has
replaced the conventional method in thin lm fabrication. As
shown in the comparison table (Table 1), spin coating method is
more prominent in producing high uniformity lms with specic
thickness [69]. The lm in the range of micron to nanometers in
thickness can be easily produced by controlling the parameters
such as spin rate and viscosity.
As for the materials used in the electronics packaging, epoxy/silica composite has successfully replaced the usage of conventional
packaging materials such as ceramics and metals. This composite
is widely used in the underll and molding compound due to its
ease of processing, low cost, as well as its excellent chemical and
electrical properties [10,11]. Moreover, the high thermal stability
silica ller do not only reduce the coefcient of thermal expansion
(CTE) of the composite system, it also provides assistance in ame
retardancy [12]. The effect of ller loading as well as the particles
shape and treatment of the micron and submicron silica mechanical
and thermal performance of the composite are being studied by
current researchers [1315]. Silica is commonly known to have an
extremely low CTE due to the high bond energy of SiO. However,
upon addition to the polymer composite system, the micron- and
submicron-sized silica requires a very high loading of up to
95 vol% in order to obtain a composite with a CTE value below
10 ppm/C [16]. This will weaken the mechanical performance of
the composites especially those involving thin lm composites.

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E. Foo et al. / Composites: Part A 42 (2011) 14321437

Table 1
Comparison of thin lm fabrication methods [69].

Fabrication
control
Thickness
control
Thickness of
product
Substrate/
shape
Uniformity of
lm
Production
rate
Cost
Commercialize

Spin coating

Dip coating

Solution casting

Hot press

Complex (3 stages)

Complex (due to concentration control

and dipping rate)
Poor, concentration control with few
trial needed to get proper concentration

Simple

Simple

Poor, thickness according to

depth of dish and shrinkage

Good control

Nano to micron

Micron

Micron

Irregular shape, glass substrate is

preferable
Poor

Flat substrate

Flat substrate

Poor

Good

Slow (few trial to obtain required

thickness)
Less expensive
Difcult due to variability in thickness
uniformity

Fast

Slower than spin coating (resin need

to be coagulated before hot press)
Expensive
Difcult due to slow production rate

Good control with spin rate

(with spin coat calculation
model)
Nano to micron
Flat substrate
Good
Fast
Expensive
Easy due to controlled thickness
and production rate

The high loading of silica leads to the increase in the viscosity of the
system and causes difculty to the fabrication process. Additionally, the high loading of large size silica llers often result in rougher surface and lower lm exibility.
With the increasing interest in nanoscience and nanotechnology, there are footprints of polymer nanocomposites in the scientic research and engineering applications. Due to its extremely
small size and large surface to volume ratio, nano-sized llers
induce different properties compared with micron-sized llers of
the same chemical composition [17]. This broadened the application of nanocomposites in the microelectronics eld [18,19]. Moreover, the exibility of thin lm composites at a high loading of
nano-sized ller was reported to remain the same with the low
loading [5]. This results in the possibility of the fabrication of
epoxy/silica thin lm composites. In terms of thermal properties,
the smaller nano-sized inorganic llers show an improvement in
CTE compared with the micron-sized llers [20]. The high surface
area per unit volume of this nanocomposite shows a better efciency in reducing the CTE compared with the micron-composite.
However, reports on the fabrication of low CTE thin lm nanoand microcomposites are still lacking.
In this paper, low CTE thin lm epoxy composites were fabricated using the spin coating method. The tensile properties, CTE,
and thermal stability of the thin lm epoxy nano- and microcomposites were studied. The effect of the size of llers and its loading
towards the mechanical and thermal properties of thin lm composites were discussed.
2. Experimental work
2.1. Materials
The epoxy used in the thin lm composite fabrication was EPON
8281 from Hexion while the curing agent used was polyetheramine EC 301 from BASF. The spherical silica powder (l-Si) grade
SS-0020 with mean particle size of 4.83 lm was supplied by
KOSEM and the fumed nano-silica (n-Si) grade S5130 with a mean
size of 7 nm was supplied by Sigma Aldrich.

based on the previous work done by Leng et al. [21]. Hielscher

UP200S Ultrasonic Stirrer was used as a mixer for ease of llers dispersion. The epoxy was then added into the curing agent mixture
and ultrasonicated again to homogenize the mixture. In order to
prevent pin holes defect on the composite lm, all the entrapped
bubbles were removed in the vacuum oven before proceeding to
the spin coating process. For the spin coating process, the epoxy
mixtures were deposited on the at substrate or transparency
and spin coated at the rate of 1000 rpm for 30 s, followed by a second spin-up rate at 1500 rpm for 60 s. The composite lms were
then cured at 80 C for 2 h.
2.3. Characterization
The specic surface area (SSA) of the l-Si was determined by the
BET method using the Quantachrome Instruments Autosorb-1. Due
to the limitation of this machine in the determination of SSA for
nano-sized particles, the SSA value for the n-Si provided by the supplier was used as comparison.
In the comparison of the effect of nano- and micron-sized llers
towards the composites system, the interface area between the
epoxy and ller per volume unit (IA/V) is determined. It is commonly known that there will be an increase in IA/V with the reduction of particle size into the nanometric dimensions. Therefore, a
simple ball model of a particle-lled polymer that was proposed
by Henk et al. [22] was used in the illustration of the magnitude
order for the interparticle spacing and interface area. In this model,
all the particles are assumed to have the same diameter D and the
particles are also uniformly distributed. Each ball is assumed to
have six nearest neighbors at a volumetric ller loading fraction
(f). Hence, the mathematical model in Eqs. (1) and (2) can be
obtained:
Nearest neighbor spacing,

dn D

The l-Si and n-Si were dried in the oven at 110 oC for 2 h before
mixing with the curing agent. For the comparison between the effects of ller size, the loading of the l-Si in the epoxy resin was
varied from 5 wt% to 30 wt% while the n-Si was varied from
0.5 wt% to 6 wt%. These loadings are assumed to be comparable

"

6f

1=3

#
1

Polymer matrix/ller particle interface area per volume unit,

IA=V
2.2. Methods

Cheapest
Difcult due to difculty in
thickness control

6f
D

D is the mean particle size.

The tensile properties of the neat epoxy thin lm and epoxy/
silica thin lm composites were studied by Instron 3366 with the
crosshead speed of 1 mm/min. The fracture surface of the tensile
specimen was observed using Zeiss Supra 35VP Field Emission
Scanning Electron Microscope (FESEM). Meanwhile, for the

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E. Foo et al. / Composites: Part A 42 (2011) 14321437

thermal properties such as the CTE and thermal stability, the Perkin Elmer Thermomechanical Analyzer (TMA) Pyris 7 and Perkin
Elmer Thermogravimetric Analysis (TGA) Pyris 6 were used,
respectively. For the TMA test, a heating rate of 10 C/min under
a static force of 1.0 mN was used from room temperature to
300 C. For the TGA test, the neat epoxy thin lm and thin lm
composite samples were analyzed from room temperature to
600 C under a heating rate of 10 C/min.

3. Results and discussion

The tensile modulus (E) and tensile strength (TS) of the neat
epoxy thin lm and epoxy/silica thin lm composites for the different loadings of l-Si and n-Si are shown in Fig. 1. As expected, the E
for the epoxy/silica thin lm composite increases with the both
l-Si and n-Si loading. The E for n-Si lled thin lm composite
reaches the highest value which is 2.4 GPa at 6 wt%. Meanwhile,
for l-Si the E value increases to a saturated state which is approximately 2.5 GPa when the l-Si loading reaches 30 wt%. The comparison of the highest E value achieved by l-Si and n-Si shows
that low loading of n-Si (6 wt%) is capable to achieve the E which
almost equivalent to that of 30 wt% l-Si. This could be explained
by the effect of ller particle size as seen in Table 2. Based on the
values, the SSA for n-Si is approximately 14 times larger than the
SSA for l-Si. Meanwhile, the dn is smaller with the decrease in
the size of ller particles and the IA/V increased dramatically. Thus,
the n-Si in this thin lm composite system has a higher surface
interaction with the epoxy compared with the l-Si. According to

Fig. 1. Tensile modulus and strength for thin lm composites with different loading
of l-Si (5 wt%30 wt%) and n-Si (0.5 wt%6 wt%) llers. (For interpretation of the
references to colour in this gure legend, the reader is referred to the web version of
this article.)

Table 2
Specic surface area (SSA), calculated values of nearest neighbour spacing (dn) and
epoxy/ller interface area per volume unit (IA/V) for both l-Si and n-Si in thin lm
composites.

a
b

Fillers

SSA (m2/g)

fa

Db (m)

dn (m)

IA=V (km2/m3)

5 wt% l-Si
15 wt% l-Si
30 wt% l-Si
1 wt% n-Si
2 wt% n-Si
6 wt% n-Si

28.70
28.70
28.70
390 40
390 40
390 40

0.03
0.08
0.17
0.23
0.38
0.65

4.83E06
4.83E06
4.83E06
7.00E09
7.00E09
7.00E09

8.43E-06
4.20E06
2.19E06
2.21E09
1.89E10
13.6E10

0.03
0.10
0.21
197.14
325.71
557.14

Equivalent volume fraction.

Mean particle size.

Fu et al. [23], the addition of higher rigidity inorganic ller into

the polymeric matrix increases the modulus of the overall product
due to the increase of the rigidity. As there is higher surface interaction of n-Si with the epoxy resin, the mobility of the epoxy molecules reduces [24]. Hence, higher rigidity in the composite lled
with n-Si leads to a higher E value even at low loading.
A large drop in the TS value was observed when the loading of
the n-Si and l-Si increase to 6 wt% and 30 wt% respectively. From
the SEM images on tensile fracture surface of the thin lm samples
in Fig. 2e, it can be proven that the drop in the TS for high loading
l-Si is due to the presence of high aggregates density, or in order
words, agglomeration occurs when the loading of l-Si reaches
maximum. During the tensile stress, these aggregates acted as foreign bodies and initiated the cracks in the composites. Moreover,
the obvious phase separation on the llers surface was also
observed on the SEM image of the tensile fracture surface for the
l-Si thin lm (Fig. 2d and e). The l-Si llers were not perfectly
encapsulated with the matrix phase during the tensile test. This
shows the poor miscibility between the silica llers and epoxy matrix also contributing to the TS value drop for the thin lm at high
loading of l-Si. Meanwhile, the SEM images of the n-Si thin lm
fracture surface shows an increment in the quantity of voids with
the loading of n-Si. This will also contribute to the drop of TS value
at high loading of n-Si in thin lm composite apart from the
agglomeration that takes place.
From the comparison of TS value between the l-Si and n-Si in
Fig. 1, it was found that the TS for the thin lm obtained by
15 wt% l-Si was equivalent to the TS obtained by the addition of
merely 2 wt% of n-Si. This can be supported by the SSA value in
Table 2. The SSA value for the n-Si was 57% higher compared with
the l-Si. The higher surface area of the nano-sized ller tends to
have a better reinforcing efciency than a larger sized ller even
at a very low loading [25]. Hence, only small amounts of n-Si are
needed in order to achieve the equivalent tensile properties using
l-Si. However, due to the agglomeration tendency of the nanosized particles, n-Si was still unable to give a large increment in
TS value.
Table 3 shows the value of Tg, CTE before Tg (aG) and after Tg
(aR), which are analyzed from the TMA curves. It is observed that
there is only a slight increment in the Tg for the l-Si lled thin lm
composites, on the other hand there is no signicant trend indicated by n-Si composite system. It is reported that the chemical
bonding between the ller surface and the epoxy matrix is important and strongly inuence the crosslinking density and Tg of the
composite materials [26], however since untreated l-Si and n-Si
were used in this study, hence no signicant increment in Tg was
observed in the composite system.
While for the CTE value, aG decreased drastically with the
increased loading of l-Si and n-Si llers. The value aG for the
1 wt% n-Si thin lm composites was almost equivalent to the aG
for the 15 wt% l-Si thin lm composites. As reported by Popelar
[27], the optimum CTE for the epoxy/silica composite in the ip
chip underll application should be at around 14 ppm/C in order
to minimized the damage in the solder joint. As comparison with
the results in Table 3, the increase of the l-Si and n-Si loading
show their ability to achieve the required CTE value in the ip chip
application. Moreover, the 2 wt% n-Si thin lm composites have
the lowest CTE value and reach the saturation stage in the CTE
value with the continue increase in n-Si to 6 wt%. The low loading
of n-Si was more effective in the CTE reduction compared with the
high loading l-Si. In correlation with the IA/V that was calculated in
Table 2, the IA/V for the n-Si was larger compared with the l-Si. The
larger IA/V of n-Si indicates a larger interface of ller particles and
resin matrix constricting the expansion of the resin matrix
[28,29]. The dn for n-Si is also smaller, which means that the n-Si
particles are more closely-packed in the composite system

E. Foo et al. / Composites: Part A 42 (2011) 14321437

1435

Fig. 2. SEM image of tensile fracture surface for thin lm composite with (a) 0 wt% or neat epoxy, (b) 2 wt% n-Si, (c) 6 wt% n-Si, (d) 15 wt% l-Si, (e) 30 wt% l-Si (SEM, 2500
for (a) and 30,000 for (b), (c) and 5000 for (d), (e)).

Table 3
Coefcient of thermal expansion (CTE) and glass transition temperature (Tg) for neat
epoxy thin lm and different loading of l-Si and n-Si thin lm composites.
Sample

Tg (C)

Neat epoxy (0 wt%)

5 wt% l-Si
15 wt% l-Si
30 wt% l-Si
1 wt% n-Si
2 wt% n-Si
6 wt% n-Si

85.4
87.12
95.0
103.0
89.3
86.2
82.85

Coefcient of thermal expansion, CTE

Before Tg (ppm/C)

After Tg (ppm/C)

47.5
42.5
17.7
15.1
18.3
6.7
6.9

352.4
339.7
70.5
96.1
192.2
177.7
169.4

compared with the l-Si. The expansion of the matrix is constrained

more effectively by the closely-packed n-Si. Hence, the expansion
of the total composite system was greatly reduced by the incorporation of n-Si compared with the l-Si even at a lower weight
fraction.
However, at a temperature above Tg, l-Si thin lm composites
achieve a lower aR compared with the n-Si thin lm composites.
As the temperature increases above Tg, the expansion of the matrix
is mainly due to the molecular mobility of the polymer chains
where the glassy solid transforms into viscous liquid [30]. In comparison with the l-Si thin lm composites, the weight fraction of

the matrix in the n-Si thin lm composites was higher. Hence,

the molecular mobility of the polymer chains in the n-Si thin lm
composites become more dominant than the expansion constriction by the small amount of n-Si llers. However, the electronics
application of the thin lm is only towards below the Tg condition
and therefore aG is a greater concern than aR [31].
Fig. 3 shows the TGA thermogram for the neat epoxy thin lm
and epoxy/silica thin lm composites that was characterized by
Perkin Elmer TGA. The TGA thermogram was analyzed and the
initial decomposition temperature (IDT) was taken at the temperature in which the sample achieved a 5% weight loss. With temperature at the maximum rate of weight loss (Tmax), these values were
tabulated in Table 4 and the thermal stability of the thin lm composites was determined. The Tmax value was obtained at the point
where the peak of the DTG curve is registered. In comparison with
the neat epoxy (0 wt%), the incorporation of l-Si and n-Si causes
the small positive shift in IDT. This small increment in IDT of the
composite is due to the presence of the relatively higher thermal
stability of the silica compared with the epoxy resin [32]. Based
on observations, the IDT value for the 2 wt% and 6 wt% n-Si loading
are almost equivalent to that with 30 wt% l-Si. According to Kuljanin et al. [33], the thermal stability increment for the ller reinforced polymers is due to the adsorption of polymer chains on
the ller surface, which partially altered the molecular mobility
of the chains. As in Table 2, n-Si has a higher SSA, which attaches

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E. Foo et al. / Composites: Part A 42 (2011) 14321437

Fig. 3. TGA thermogram together with enlarged TGA thermogram from 340 C to 420 C for different loading of l-Si (5 wt%30 wt%) and n-Si (1 wt%6 wt%) thin lm
composites. (For interpretation of the references to colour in this gure legend, the reader is referred to the web version of this article.)

Table 4
Initial decomposition temperature (IDT) and temperature at maximum rate of weight
loss (Tmax) for neat epoxy thin lm and different loading of l-Si and n-Si thin lm
composites.
Sample

IDT (C)

Tmax (C)

Neat epoxy (0 wt%)

5 wt% l-Si
15 wt% l-Si
30 wt% l-Si
1 wt% n-Si
2 wt% n-Si
6 wt% n-Si

334
350
349
360
323
360
359

390
391
389
392
385
392
390

more polymer segments. There will be more restriction of the polymer segment motions in the n-Si thin lm composites and the
chain transfer reaction will be suppressed. Even a small amount
of the n-Si are also able to produce better stability of the lled
composite. However, there is no signicant increment in the Tmax
for all the l-Si and n-Si thin lm composites due to the absence
of the strong chemical bonding between the inorganic ller and
the polymer chain. The silica ller was only physically adsorbed
to the epoxy resins, which is proven in the SEM image of the tensile
fracture surface in Fig. 2.
4. Conclusion
Low CTE thin lm composite was successfully fabricated using
the spin coating method. With the incorporation of silica llers,
the tensile and thermal properties of the thin lm composites
can be enhanced. Small amounts of n-Si can achieve a similar TS
with those of l-Si. For example, the 2 wt% n-Si thin lm composite
and the 15 wt% l-Si thin lm composite recorded approximately a
38% rise in their TS compared with the neat epoxy thin lm. In
comparison with the neat epoxy thin lm, 2 wt% and 6 wt% n-Si
thin lm composites obtain lower aG value with a drop of 86%
while the aG for the 30 wt% l-Si thin lm composite is only able
to decrease by 68%. Thus, n-Si proved its ability to achieve substantial mechanical and thermal properties at a lower weight fraction
compared with the l-Si. As for the thermal stability, both the maximum loading of l-Si and n-Si thin lm composites show a small

positive shift in IDT from 334 C to 359 C. However, the Tmax did
not increase signicantly. The overall thermal stability of the
epoxy/silica thin lm composite did not effectively enhance without the presence of a coupling agent.
Acknowledgments
The authors gratefully acknowledges Intel Technology (M) Sdn.
Bhd. for awarding the Intel Research Grant (Grant No.: 6050175)
and Universiti Sains Malaysia for providing the Postgraduate
Research University Grant (Grant No.: 8043020) that made this
study possible. The main author would like to thank Intel Technology (M) Sdn. Bhd. for granting her the Intel fellowship.
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