Available online at www.sciencedirect.

com
COMPOSITES
SCIENCE AND
TECHNOLOGY
Composites Science and Technology 68 (2008) 346–353
www.elsevier.com/locate/compscitech

Effect of particle shape of silica mineral on the properties of

epoxy composites
Farrah Noor Ahmad, Mariatti Jaafar *, Samayamutthirian Palaniandy,
Khairun Azizi Mohd Azizli
School of Materials and Mineral Resources Engineering, Engineering Campus, Universiti Sains Malaysia, 14300 Nibong Tebal, Penang, Malaysia

Received 12 April 2007; received in revised form 26 July 2007; accepted 26 July 2007
Available online 3 August 2007

Abstract

This study was carried out to evaluate the performance of silica mineral composites in comparison with conventional fused silica com-
posites, which is commonly used as underfill material. The silica mineral was produced by fine grinding technique. Three different particle
shape type, namely angular, cubical and elongated shapes were obtained by varying the classifier speed of the grinder. In this study, the
effects of different percentage of filler loading and shapes of silica mineral particles on the mechanical and thermal properties of com-
posite systems were investigated. In general, it was found that the addition of particulate filler loading increased the tensile strength
and modulus, flexural strength and modulus, thermal stability and Tg. As expected, the addition of filler in epoxy reduced the coefficient
of thermal expansion (CTE) of the system. The study showed that elongated silica mineral particles exhibited higher flexural and tensile
properties and comparable CTE in comparison with fused silica filler composites.
 2007 Elsevier Ltd. All rights reserved.

Keywords: B. Strength; B. Mechanical properties; A. Polymer–matrix composites (PMC); A. Particle-reinforced composites; D. Scanning electron
microscopy (SEM)

1. Introduction
The introduction of well-dispersed inorganic particles
into a polymer–matrix has been demonstrated to be extre-
mely effective to improve the performance of the polymer
composites [1]. In microelectronic industries, silica particle
filled epoxy composites have been used in flip–chip pack-
ages as underfill materials. Fig. 1 shows a schematic dia-
gram of flip–chip package. The underfill material is used
to fill the gap between the chip and substrate around the
solder interconnections for the purpose of reducing the
thermal stresses imposed on the solder joints and further
improving the long-term reliability of electronic device
[1,2]. According to Hsu et al. [3], the key requirements of
underfill materials are high glass transition temperature
(>125 C), good adhesion to the surface of contact materi-
*
Corresponding author. Tel.: +60 4 5995262; fax: +60 4 5941011.
E-mail address: mariatti@eng.usm.my (M. Jaafar).
als, high modulus, low stress, minimal filler setting and
moisture absorption, optimized CTE (20–30 ppm/C),
low viscosity (<20 kcps at 25 C), fast cure, and long work-
ing life (>16 h at 25 C). In order to fulfill the requirements,
factors such as silica filler loading, filler shape, particle size
distribution, viscosity and flowability need to be considered
as these will affect the properties of underfill [4].
In general, unfilled epoxy resin has a CTE of 50–
70 ppm/C [5]. In order to attain the target CTE, underfills
are filled with low CTE filler particle. Fused silica has been
widely used as filler in polymer composites [1] due to the
exceptionally low coefficient of thermal expansion (CTE)
of fused silica (CTE = 0.5 ppm/C), compability with sili-
con chip, excellent dielectric properties and high chemical
and thermal stability [6]. However, it is noted that the price
of fused silica is quite high compared to other types of silica
such as silica mineral, fumed silica, etc. For example, con-
sidering the purifying and grinding techniques involve in
the production of silica mineral particles, the price of silica

0266-3538/$ - see front matter  2007 Elsevier Ltd. All rights reserved.
doi:10.1016/j.compscitech.2007.07.015
 F.N. Ahmad et al. / Composites Science and Technology 68 (2008) 346–353
Fig. 1. Structure and cross section of flip–chip [1].
mineral which is obtained locally (in Malaysia) is approxi-
mately 500% lower than the imported fused silica.
Realizing the high cost of fused silica, attempts have
been made to find an alternative filler to be used in underfill
materials. In this study, silica mineral particles were uti-
lized and it was produced using fine grinding technique.
The characterizations of this high purity silica mineral have
been reported elsewhere [7,8]. Our previous study observed
that the properties of silica mineral filled epoxy composites
were comparable with those of fused silica filled epoxy
composites [9], which indirectly indicated the possibility
of using this mineral filler in the underfill application.
Many previous works have been focused on size, distribu-
tion of filler and volume fraction of filler [2,6], however
only a few investigation into the effect of particle shape
has been published [10]. Here, underfills with various
shapes of silica mineral (angular, elongated and cubical)
filled epoxy composites were prepared and the properties
were compared with those of fused silica filled epoxy
composites.
2. Experimental
2.1. Materials
The epoxy resin named EPONTM Resin 8281, supplied by
Hexion Specialty Chemicals, Inc. was used as a matrix in
this research. It is also chemically termed as Bisphenol-A-
(epichlorohydrin). The curing agent used in the study was
Polyetheramine D230 (PEA D230), supplied by BASF
Corporation with a density of 0.946 g/ml at 298 K. High
purity silica mineral used in this experiment was supplied
by Sibelco Asia in powder form. The silica mineral powders
(without any additional pre-processing) were fed to the
Alpine 100 AFG opposed jet mill equipped with a 50
ATP-forced vortex classifier for fine grinding purposes.
The feed rate and grinding pressure were fixed at 12 kg/h
and 6 bars, respectively. The variation in the particle shape
was influenced by the operational parameters of the jet mill
and its condition in the grinding chamber, which controlled
the breakage mechanism in the jet mill. The classifier rota-
tional speed (which were varied from 7000, 13 000 and
19 000 rpm) would determined the mean particle size, d50
of the ground particles, and indirectly the retention time
of the particles in the grinding chamber. The d50 or the
mean particle diameter was taken as the 50% cumulative
passing size, and it was measured by sieve analysis. At
347
higher classifier rotational speed, the classified particles
were smaller and the retention time was longer whilst at
lower classifier rotational speed, the retention time was
shorter and the particles were coarser. Longer retention
time of particles in the grinding chamber caused more col-
lisions and attrition breakage due to rubbing between the
particles in the grinding chamber, hence producing finer
particles. This subsequently would remove the sharp edges,
hence producing more spherical and cubical particles.
Lower classifier rotational speed resulted in shorter reten-
tion time of particles in the grinding chamber, subsequently
minimizing the rubbing of particles in the grinding cham-
ber resulting in production of elongated and concave par-
ticles. Typical grinding duration for the different particle
shape types was about 20–30 min.
The classifier speeds which were varied at three levels
such as 7000, 13 000 and 19 000 rpm produced elongated,
angular and cubical particle shape, respectively. Fused sil-
ica filler which was supplied by Goodfellow, USA was used
as filler in epoxy composites and the composites was used
as a control in this investigation.
2.2. Preparation of composites
In the first part of the study, the effects of different per-
centage of filler loadings (0, 15, 30 and 45 vol.%) and filler
shape (angular, cubical and elongated) on the properties of
epoxy composites were investigated. Formula (1) was uti-
lized in the preparation of the composites.
Wf
qf
V f ¼ Wf ð1Þ
qf
þ Wqmm
where Wf = weight of filler, Wm = weight of matrix, Vf =
filler volume faction, qm = density of matrix and qf = den-
sity of filler.
Based on the properties shown in the first part, the sec-
ond part determined the optimal filler loading at 45 vol.%
in order to compare the properties of silica mineral and
fused silica composites. The mixing of epoxy resin, hard-
ener and silica filler was carried out in a mould followed
by ultrasonic agitation method using ultrasonic bath
(Elma Transsonic Digitals). According to previous
researchers [11,12], ultrasonically agitation method was
more effective to disperse particles into viscous system
compared to other technique such as conventional stir-
ring. This acoustic power by the sonication technique
would break up the aggregate of the particle powder
and dispersed the particle powder more evenly in the
resin. The sonication technique was performed at room
temperature. The mould was then transferred in a vacuum
oven for initial curing process at the temperature of 35 C
for 1 h to evacuate the entrapped air. Based on the visual
observation and the homogenous color of the sample,
minimum sedimentation occurred in the sample. The mix-
ture was then placed into the oven for curing process fol-
lowed by cooling at room temperature.
348 F.N. Ahmad et al. / Composites Science and Technology 68 (2008) 346–353
2.3. Measurement
The morphology properties such as silica shapes, filler
size distribution, interface between matrix and reinforce-
ment and surface fracture of the specimens were investi-
gated using ZEISS SUPRA 35 VP scanning electron
microscopy (SEM). Sample for microstructure observation
under SEM was prepared from cross sectional of the frac-
tured surfaces of flexural specimens. Thermal properties of
an epoxy filled with silica such as the weight loss profile and
thermal stability were investigated using thermogravimetric
analysis (TGA). TGA measurement was conducted in an
air atmosphere by using Perkin–Elmer Pyris 6 TGA. The
temperature was varied from room temperature to 600 C
at a heating rate of 5 C/min. The coefficient of thermal
expansion (CTE) was determined using a Linseis Dilatom-
eter L75. Linear thermal expansion coefficients of cured
samples were heated from room temperature to 250 C
with a heating rate of 10 C/min. Composite samples with
a dimension of 5 cm · 2 cm · 5 cm were used in this
measurement.
Flexural testing was performed based on ASTM stan-
dard, D 790-98 and according to three points bending tests
which utilized center loading on a simple supported beam.
The testing was conducted by using Instron series 1X Auto-
mated Materials Testing System model 3366 with load cell
of 10 kN. The crosshead displacement rate was set at
Fig. 2. SEM micrographs of the best represented the different shape of silica fillers: (a) silica mineral, angular shape, (b) silica mineral, cubical, (c) silica
mineral, elongated and (d) fused silica, irregular shape (8000· magnifications).
5 mm/min and span length to sample’s thickness ratio
was maintained at 16:1. The specimens used for flexural
testing were bars of rectangular cross section (flatwise) with
a length of 60 mm and width of 14 mm.
3. Result and discussion
3.1. Characterization of silica particle
Scanning electron microscope (SEM) micrographs of
the various shapes of the silica particles are shown in
Fig. 2. The angular shape of silica mineral particle indicates
that the shape having one or more sharp angles on its sur-
face. Meanwhile, the cubical shape shows smooth angles
compared to the angular shape. Elongated silica mineral
particle is characterized by longer length than width of
the particle. Apparently, fused silica consists of various
shapes such as spherical, cubical and hexagonal which
are referred as irregular shape. Minimal agglomeration is
observed in the morphology of silica mineral due to the
autogeneous breakage mechanism which allows the particle
breakage along the weak planes and minimizes surface
energy [7]. Apparently, unlike silica mineral, the fused silica
morphology shows agglomeration.
According to Bouwman et al. [11], the particle shape can
be described based on the aspect ratio, Stokes’s shape fac-
tor, radial shape factor, etc. The description based on
 F.N. Ahmad et al. / Composites Science and Technology 68 (2008) 346–353
aspect ratio is commonly being used by many researches
when dealing with shape factor [12,13]. Aspect ratio is
defined by the particle length: thickness ratio. In this study,
the aspect ratio of silica particles was calculated based on
100 numbers of particles (using SEM micrographs). Table
1 provides information on aspect ratios and mean particle
size of these three mineral particle shapes and irregular
fused silica that was used in this study.
In this study, the elongated silica shows the highest
value of aspect ratio which is more than 1 while the angular
silica shows the lowest value of aspect ratio which is less
than 1. Pabst et al. [12] in their studies defined that the
aspect ratio for elongated particle is more than 1. The val-
ues shown for cubical and irregular shape were in accor-
dance with previous work by Katz and Milewski [13]
where the aspect ratio of cubical particle was around 1
while the aspect ratio for irregular particle was in the range
of 1.4–4. In general the aspect ratios of silica mineral
(shown in Table 1) are in parallel with those of previous
works [12,13].
According to Wypych [14], particles shape with low or
high aspect ratio may affect the properties of the compos-
ite. The shape of silica particle affects the settling, separa-
tion during flow, viscosity and particle packing. It is
known that anisometric particles with difference in length
versus width are more effective to be used as reinforcements
than particles which has similar dimension in length and
width (isometric particle). This is because high surface area
will provide more contact area and therefore have a higher
potential to reinforce the matrix. For example, particle in
cubic shapes provide good reinforcement while elongated
particles give superior reinforcement, reduce shrinkage
and thermal expansion of the material [14]. However,
instead of aspect ratio factor, other factors such as filler
particle size, distribution of filler particles in the poly-
mer–matrix and good adhesion at the interface surface
might also influence the properties of particulate filled com-
posite systems.
From the data given in Table 1, based on group of min-
eral fillers, cubical silica shows the smallest dimension of
particle size while angular has the largest dimension of par-
ticle size. Fused silica which is used as a controller has a
mean particle size of 2.18 lm. The particle size of filler is
very important since it has an effect on flow rate and CTE
of the composite and most underfill material contain silica
ranging from approximately 10–50 lm [15]. However,
according to Lau et al. [16], the filler size of underfill material
should be less than 10 lm. Fillers with particle size greater
Table 1
Aspect ratio and mean particle size of various shape of silica
Sample Aspect ratio Mean particle size/d50% (lm)
Angular (silica mineral) 0.824 10.31
Cubical (silica mineral) 1.122 4.10
Elongated (silica mineral) 2.954 7.20
Irregular (fused silica) 1.362 2.18
349
than 10 lm should be avoided because it can reduce the per-
formance of composite rather than extend or reinforce.
3.2. Flexural and tensile properties of epoxy composites
The results of flexural strength of the composite system
as a function of filler loadings are presented in Fig. 3. In
general, the graph shows an increasing trend as the filler
loading increases, however, slight decrease in flexural
strength is observed at 15 vol.% of silica. The highest
strength of the epoxy filled with silica filler was observed
at filler loading of 45 vol.%. In general, elongated silica
filled epoxy showed higher flexural strength at almost all
filler loadings compared to those of cubical and angular
shape. As mentioned in Section 3.1, elongated particle
show high aspect ratio. High aspect ratio provides high sur-
face area, hence results in more contact area between the
filler and the matrix. Therefore, by presumably good adhe-
sion and bonding exist between the filler and matrix, posi-
tive reinforcement effect occurs in elongated silica filled
epoxy which might increase the strength of the composite.
Fig. 4 shows the micrograph of (a) elongated and (b)
angular silica filled epoxy composites. Elongated filler
shape having higher particle surface results in more contact
area between the filler and the matrix. From the micro-
graph, the interphase of these composite is good judging
from the adhesion between the contact of matrix and silica.
Silva et al. [17] studied about the mechanical analysis on
polypropylene composites filled with talc and CaCO3. They
found that the effective bonding between inorganic fillers
and matrix components typically improved the mechanical
properties of polymer composites. Angular shape silica
mineral epoxy composites (refer to Fig. 4b) shows the low-
est mechanical properties presumably because of the sepa-
ration at the particle–matrix interface which are directly
associated with the stress concentration factors at the edges
of the particle [18]. Furthermore, filler size of angular par-
ticle which is more than 10 lm is reported to reduce the
performance of composite [16].
irregular angular cubical elongated
140
120
Flexural strength (MPa)
100
80
60
40
20
0
0 15 30 45
Filler loading (volume %)
Fig. 3. Effect of filler loading on flexural strength of different silica particle
shapes in epoxy composites.
350 F.N. Ahmad et al. / Composites Science and Technology 68 (2008) 346–353
Fig. 4. Scanning electron fractograph of epoxy filled with elongated silica and angular silica at filler content of 45% in volume (8000· magnification).
The comparison between flexural strength and morphol-
ogy of silica mineral and fused silica filled epoxy at
45 vol.% were made. The 45 vol.% was chosen since higher
properties were shown at this percentage of filler loading. It
is observed that the flexural strength of fused silica is lower
compared to those of silica mineral composites. Based on
morphology study (shown in Fig. 5), it is found that min-
eral filler exhibits homogenous distribution in epoxy com-
posites compared to that of fused silica. The separation
at the edge of the particle–matrix interface still can be
observed in angular shape silica mineral filled epoxy com-
posites. The agglomerations of fused silica results in inho-
mogeneous distribution and hence weaken the interaction
between the filler and the matrix. This subsequently
reduces the mechanical properties of the fused silica com-
posite system. Agglomeration will cause defect to the com-
posite because of the presence of void between the
particles. This mean that agglomerates resulting as a weak
point in the composite material can lead to an undesirable
material property. Other factors such as filler–matrix com-
patibility, bonding at interface, aspect ratio, etc might also
influence the flexural strength of the fused silica compos-
ites. It should be reiterated that the flexural strength is
not the essential properties in the underfill application.
As noted in the previous works [3,4], the flexural modulus
and thermal properties are the key requirements of under-
fill materials.
Results of flexural modulus versus filler loading have
been depicted in Fig. 6. In general, it is found that the mod-
ulus of the epoxy filled epoxy increases with increasing of
filler loading. As shown in Fig. 6, elongated particle rein-
forced composite exhibits the highest modulus compared
to angular and cubical shape. Theoretically, higher aspect
ratio will increase the modulus of the particulate filler filled
polymer composite. The results are in accordance with the
previous work by Orefice et al. [19] on the effect of reinforc-
ing agents on the properties and behavior of polymer com-
posites with different aspect ratios. In their study, they
observed that the highest flexural modulus was obtained
by the short fiber reinforced composite (high aspect ratio)
while the composite reinforced with spherical particles
(low aspect ratio) showed the lowest flexural modulus. This
indirectly indicates that the aspect ratios, i.e., large surface
areas per volume, can lead to higher levels of stress trans-
ferability since this phenomenon is governed by shear
mechanisms between matrix and fiber/filler at the inter-
phase, hence increasing the flexural modulus of the com-
posite system.
The comparison of flexural modulus at 45 vol.% of min-
eral and fused silica filled epoxy composites is shown in
Fig. 6. As can be seen from the figure (based from error
bar), the fused silica shows a comparable flexural modulus
with angular silica mineral composites however slightly
lower flexural modulus observed in comparison with those
of cubical and elongated silica mineral. The agglomerations
of the fused silica make the dispersion of the filler into the
epoxy resin become inhomogeneous and this might weaken
the modulus of fused silica composites. Luyt et al. [20] have
reported that the size and distribution of filler particles in
polymer–matrix greatly influence the modulus of the com-
posites. In addition, the modulus for epoxy filled with var-
ious shape of silica mineral at 45 vol.% has fulfilled the
modulus requirement to be used as underfill materials.
The ideal modulus for underfill should be within 2–
12 GPa. The results are comparable with the modulus
shown by the existing material of fused silica filled epoxy.
The results of tensile strength, tensile modulus and elon-
gation at break of the composite system at 15% and 45% of
filler loadings are presented in Table 2. Similar trend as
found in flexural properties is observed here where the ten-
sile strength and modulus of the composite increase with
increasing filler content. The elongated silica mineral com-
 F.N. Ahmad et al. / Composites Science and Technology 68 (2008) 346–353 351

Fig. 5. SEM micrographs showing the fracture surface morphology of: (a) epoxy resin, and distribution of silica in epoxy at 45 vol.% of (b) angular silica;
(b) cubical silica; (c) elongated silica and (d) fused silica (500· magnification).

Table 2
irregular angular cubical elongated
Tensile properties of epoxy filled with mineral at 15 and 45 vol.%
10000 Samples Strength Modulus Elongation at break
(MPa) (MPa) (%)
Flexural modulus (MPa)

8000 Epoxy 43.3 ± 3.7 1995.3 ± 173.1 3.21 ± 0.59

EHA 41.9 ± 4.7 2345.3 ± 173.2 2.47 ± 0.34
15 vol.%
6000
EHC 46.5 ± 2.9 2412.6 ± 76.3 2.58 ± 0.46
15 vol.%
4000 EHE 47.5 ± 2.0 2482.0 ± 54.4 2.59 ± 0.30
15 vol.%
2000 EHA 53.3 ± 11.9 4910.0 ± 359.5 1.32 ± 0.65
45 vol.%
EHC 54.9 ± 5.7 4987.6 ± 443.1 1.47 ± 0.25
0 45 vol.%
0 15 30 45
EHE 61.2 ± 3.2 5204.1 ± 372.3 1.59 ± 0.25
Filler Loading (volume %) 45 vol.%
Fig. 6. Effect of filler loading on flexural modulus of epoxy filled with EHA, EHC and EHE refer to angular silica mineral, cubical silica mineral
various shape of silica. and elongated silica mineral, respectively.
352 F.N. Ahmad et al. / Composites Science and Technology 68 (2008) 346–353
posites show the highest strength and modulus while the
lowest trend is shown by angular silica mineral composites.
As discussed in flexural properties, the tensile test results
can be correlated with the aspect ratio factor. However,
instead of aspect ratio factor, the tensile properties of par-
ticulate filler filled system might be influenced by many fac-
tors such as filler particle size, distribution of filler particles
in the matrix polymer and good adhesion at the interface
surface [21]. As expected, from the table, the elongation
at break of these composite systems decreases with increas-
ing filler loading. The insignificant effect of mineral particle
shapes on the elongation at break of the composite was
observed.
According to Wypych [14], the elongation is usually
inversely proportional to tensile strength which means that
increasing the tensile strength of filled material usually con-
tributes to a decrease in elongation. The presence of filler
reduces the amount of a tough material available in this
system and therefore reduces the elongation at break of
the composites. However, the elongation properties are
rather reduced with the addition of fillers and are attrib-
uted to changes in motion, stress concentration and crack
initiation and propagation.
3.3. Thermal properties of epoxy composites
3.3.1. Coefficient of thermal expansion (CTE)
Table 3 shows the CTE and Tg values of the epoxy com-
posites. By comparing the CTE value of unfilled epoxy and
epoxy filled with silica mineral and fused silica at 45 vol.%,
it can be concluded that the CTE and Tg values decrease
and increase, respectively with the increase in the filler con-
tent. However, as expected (based on the CTE value of
fused and silica mineral), the CTE value of fused silica
composites is lower compared to those of silica mineral
composites. By adding the filler in composite material (pro-
viding good filler–matrix interaction in the system), the fil-
ler binds the matrix and prevents it from expanding as
much as it would on its own. Subsequently, this would
affect the thermal expansion of the composite system.
The result generally agreed with the trend observed by
He [22] who investigated on the effect of filler content on
Table 3
Dilatometer and TGA analysis of epoxy filled with mineral and fused
silica at 45 vol.%
Sample CTE Tg Onset Total weight loss
(ppm/ (C) temperature at 600 C (%)
C) (C)
Epoxy 63.6 48.8 331.28 90.85
EHA 45 vol.% 31.83 98 363.82 31.92
EHC 45 vol.% 36.11 90 363.28 32.04
EHE 45 vol.% 32.91 95 362.98 32.23
EFS 45 vol.% 29.72 83 363.82 32.72
EHA, EHC, EHE and EHS refer to angular silica mineral, cubical silica
mineral, elongated silica mineral and fused silica, respectively (note: CTE
of fused silica is 0.5 ppm/C and CTE of silica mineral is 2.65 ppm/C) [9].
the thermal expansion of the overmolded underfill materi-
als. The studies have shown that material with higher filler
content leads to a lower CTE and a higher modulus at tem-
perature below Tg. As expected, epoxy filled with 45 vol.%
of angular, cubical and elongated shows similar CTE
values.
3.3.2. Thermogravimetry (TGA analysis)
Thermal stability is very important for epoxy filled with
silica to be used in the underfill application since it might
affect the performance of the underfill. The thermal stabil-
ity can be described based on the onset temperature. The
onset temperature or also known as degradation tempera-
ture is calculated based on the line tangent to the inflection
point. The onset temperature (the temperature at which
degradation begins), and total weight loss of the specimen
of epoxy filled with various shapes of silica at filler loading
of 45 vol.% were determined by using TGA, and the results
are shown in Table 3. From the table, apparently epoxy
composites with incorporation of fillers show higher ther-
mal stability than those of unfilled epoxy. In general, as
shown in Table 3, the thermal stability of 45 vol.% of silica
mineral and fused silica filled epoxy is comparable to each
other. Upon heating to 600 C, the solid content which is
essentially indicating the silica fillers content can be
determined.
4. Conclusions
Based on the above test results and analysis, the follow-
ing conclusions can be made:
1. The elongated shape of silica mineral shows the highest
mechanical properties and comparable thermal proper-
ties compared to other shape of silica mineral and fused
silica. The optimum properties of this system are due to
the particle shape that has been described by the aspect
ratio where the elongated filler shows the highest aspect
ratio hence improving the bonding between resin and
filler.
2. Particle shapes types affect the mechanical properties of
silica mineral composites such as flexural strength, flex-
ural modulus, tensile strength and tensile modulus.
Higher mechanical properties were observed for higher
percentage of filler loading.
3. In general, the mechanical properties of epoxy filled with
silica mineral are higher compared to epoxy filled with
fused silica composites. This is due to the agglomera-
tion, filler–matrix compatibility, bonding at interface
and aspect ratio of the fused silica in the epoxy system.
4. In conclusion, epoxy filled with elongated silica mineral
exhibits high elastic modulus (9.453 GPa) and compara-
ble CTE (32.91 ppm/C) in comparison with fused silica
composites (control system). This polymer composite
fulfills some of the required properties for underfill appli-
cations and it could be considered as a candidate for
underfill material in electronic packaging applications.
 F.N. Ahmad et al. / Composites Science and Technology 68 (2008) 346–353
Acknowledgement
The authors gratefully acknowledge Universiti Sains
Malaysia for granting the research fund under USM short
term grant.
References
[1] Wang J, Ren W, Zou D, Qian Z, Liu S. Processing mechanics for flip–
chip assemblies. Comput Struct 1998;71:457–68.
[2] Sun Y, Zhang Z, Wong CP. Study on mono-dispersed nano-size silica
by surface modification of underfill applications. J Colloid Interf Sci
2005;292:436–44.
[3] Hsu DT, Kim HK, Shi FG, Tong HY, Chungpaiboonpatana S,
Davidson C, et al. Curing kinetics and optimal cure schedules for
underfill materials. Microelectron J 2001;31:271–5.
[4] Ahmad FN. Studies on various shapes of silica mineral fillers on the
properties of epoxy for underfill application. USM MSc Thesis.
Penang: Universiti Sains Malaysia; 2006.
[5] Adamson SJ, Adams T. Board design for flip chips and chip-scale
package underfill. Electron Bull Hong Kong 2003;6:32–8.
[6] Lee W Sun, Yu J. Comparative study of thermally conductive fillers
in underfill for electronic components. Diam Relat Mater
2005;14:1647–53.
[7] Samayamutthirian Palaniandy, Khairun Azizi Mohd Azizli, Mariatti
Mustapha, Farrah Mohd Noor, Hashim Hussin, Syed Fuad Saiyid
Hashim. lSIL as alternative filler in epoxy used in electronic
packaging. In: Asian symposium on material processing. Bangkok,
Thailand; 2006.
[8] Samayamutthirian Palaniandy, Khairun Azizi Mohd Azizli, Ee Xun
Hong, Syed Fuad Saiyid Hashim, Hashim Hussin. Custom made
micronized silica for paint industry via fine grinding process. Adv
Technol Mater Mater Process J 2006;8(1):109–16.
[9] Teh PL, Jaafar M, Akil HM, Seetharamu KN, Wagiman ANR, Beh
KS. Thermal properties of fused silica and glass powder filled epoxy
353
resin. In: Proceedings of 6th electronic materials and packaging,
Penang, Malaysia; 2004.
[10] Turssi CP, Ferracane JL, Vogel K. Filler features and their effects on
wear and degree of conversion of particulate dental resin composites.
Biomaterials 2005;26(24):4932–7.
[11] Bouwman AM, Bosma JC, Vonk P, Wesselingh JA, Frijlink HW.
Which shape factor(s) best describe granules? Powder Technol
2004;146:66–72.
[12] Pabst W, Berthold C, Gregorova E. Size and shape characterization
of polydisperse short-fiber systems. J Eur Ceram Soc 2005;26:149–60.
[13] Katz HS, Milewski V. Handbook of fillers for plastic. NY: Van
Nostrand Reinhold; 1987. p. 3–14.
[14] Wypych G. Handbook of Fillers, 2nd ed., vol. 131. Toronto, New
York; Ont.: Chem Tec; 2000. p. 241–75, 347–58.
[15] Quinones H, Babiarz A, Lewis A. Flip chip encapsulation reliability,
1998. <http://www.nordson.com/pdf/electronics/csp18.pdf:1-13>.
[16] Lau JH, Lee R, Chang C, Ouyang C. Effects of underfill material
properties on the reliability of solder bumped flip chip on board with
imperfect underfill encapsulants. Electron Compon Technol Conf
1999:578.
[17] Silva ALN, Rocha MCG, Moraes MAR, Valente CAR, Coutinho
FMB. Mechanical and rheological properties of composites based on
polyolefin and mineral additives. Polym Test 2002;21(1):57–60.
[18] Huang M, Li Z. Influences of particle size and interface energy on the
stress concentration induced by the oblate spheroidal particle and the
void nucleation mechanism. Int J Solids Struct 2005:1.
[19] Orefice RL, Hench LL, Brennan AB. Effect of particle morphology
on the mechanical and thermo-mechanical behavior of polymer
composites. J Braz Soc Mech Sci 2001;23(1):1–10.
[20] Luyt AS, Molefi JA, Krump H. Thermal, mechanical and electrical
properties of copper powder filled low density and linear low-
density polyethylene composites. Polym Degrad Stabil 2005;91(7):
1629–39.
[21] Bose S, Mahanwar PA. Effect of particle size of filler on properties of
nylon-6. J Min Mater Character Eng 2004;3(1):23–31.
[22] He Y. Thermal characterization of overmolded underfill materials for
stacked chip scale packages. Thermochim Acta 2005;433:98–104.