Materials Science and Engineering A332 (2002) 362– 370

www.elsevier.com/locate/msea

Predictive modeling of elastic properties of particulate-reinforced

composites
Wei Wu a, Keya Sadeghipour a,*, Ken Boberick b, George Baran a
a
Department of Mechanical Engineering, College of Engineering, Temple Uni6ersity, 12th and Norris Streets (084 -53), Philadelphia,
PA19122, USA
b
School of Dentistry, Temple Uni6ersity, 12th and Norris Streets (084 -53), Philadelphia, PA19122, USA

Received 7 May 2001; received in revised form 24 September 2001

Abstract

The Young’s modulus and Poisson’s ratio of isotropic composites made of particulate glass fillers in a BISGMA/TEGDMA
resin matrix are determined using an axisymmetric spherical cell finite-element model developed by Guild and co-authors for
modeling the elastic properties of rubber particles/epoxy composites with volume fractions of less than 0.5. Here, we have used
this method to calculate the elastic properties of particulate-filled composites with a range of filler volume fractions, including
those with filler fractions above 0.5, which are of primary interest for dental clinical applications. We have also conducted
modeling studies on the influence of imperfect interfaces and thin interlayers on the elastic properties of composites with low and
high filler volume fractions. Finally, we have conducted experimental tensile tests in order to compare theoretical predictions with
experimental data. The predictions from the current model agree well with the test results for a range of volume fraction up to
0.53. © 2002 Elsevier Science B.V. All rights reserved.

Keywords: Hard spherical filler composites; Variation of volume fraction; Variation of interlayer properties; Finite element modeling; Elastic
constants of composites

1. Introduction (FEA) [6,7]. One-dimensional models are based on the

Resin-based composites reinforced by glass particles
are used in multiple applications, including dental
restorative materials. The mechanical properties of such
composites are affected by a number of parameters
including the size, volume fraction and distribution of
the reinforcing spherical filler, the properties of the
interface between the filler and matrix, and the proper-
ties of the matrix resin itself. A predictive model, which
allows the description of the properties of the com-
posite material from the properties of the constituent
materials, would be useful, and permit optimization of
composite properties. The literature describes a variety
of approaches, which have been developed for this
purpose. They may be roughly divided into two cate-
gories: one-dimensional [1 – 3] and three-dimensional
analytical models [4,5], or two- and three-dimensional
numerical models, which utilize finite element analyses
* Corresponding author.
mechanics of materials and their application is straight-
forward, though fitting parameters are often needed to
achieve proper accuracy. Moreover, these models as-
sume a perfect adhesive interface between the matrix
and filler, and they cannot incorporate a statistical
characterization of particle dispersion. A survey of
these one-dimensional models has been presented by
Ahmed and Jones [8].
The basic geometric unit for most rigorous three-di-
mensional analytical and numerical models of particu-
late-filled composites consists of a spherical particle
surrounded by an annulus or cylinder of matrix; the
composite is presumed to be constructed of geometri-
cally similar unit cells with the same overall filler vol-
ume fraction. This is a widely used simplification, which
neglects the potential influence of particle distribution
patterns. Both analytical and numerical three-dimen-
sional models are based on the elastic theory and are
expected to have similar degrees of accuracy. In many
three-dimensional analyses, homogeneous surface dis-

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PII: S 0 9 2 1 - 5 0 9 3 ( 0 1 ) 0 1 8 3 6 - 6
 W. Wu et al. / Materials Science and Engineering A332 (2002) 362–370
placements or traction boundary conditions are applied
to the unit cell body of volume, V, and bounding
surface, S, and the effective properties (moduli) of a
composite are obtained by equating the volumetric
average stresses or strains in the heterogeneous unit cell
to the homogenized composite stress or strain compo-
nents [9]. The calculated effective properties are rigor-
ously correct only if the applied homogeneous surface
displacement boundary conditions produce homoge-
neous surface tractions. Otherwise, a generalized self-
consistent scheme may be employed where the model
geometry consists of a spherical particle surrounded by
an annulus of the matrix subsequently surrounded by
an equivalent unbounded composite medium, and ho-
mogeneous surface displacement or traction boundary
conditions are applied [10]. The effective properties
(moduli) of a composite are obtained by equating the
strain energy of the equivalent composite with a hetero-
geneous unit cell inclusion to the strain energy of a fully
homogenized composite (calculated from assumed elas-
tic constants); iterative procedures are needed.
Compared to analytical models, a major advantage
of numerical models, such as finite element analysis
(FEA), is the versatility of the application in extended
analyses, e.g. when the filler-matrix interface is imper-
fect, and where the crack initiation site and growth
direction must be simulated. Numerical models can also
simulate particle packing or particle clustering that
might occur in composites with high particle volume
fractions.
In some recent studies, a spatial statistical technique
developed by Davy and Guild [10] was incorporated
into axisymmetric FEA models by Guild and Young
[11] to study the influence of particle distributions on
stress states near rubber and glass particles dispersed in
a resin matrix; the representative geometric unit con-
sisted of a spherical particle surrounded by a cylinder.
Because this geometry cannot represent the isotropy of
a spherical particulate-filled composite, a different
spherical cell model was later developed, consisting of a
collection of spherical cells of different sizes, each con-
taining a single particle sphere surrounded by an an-
nulus of resin [12]. The form of representative cells in
Fig. 1. The spherical cell finite-element model.
363
these material models is based on the realistic assump-
tion of a random filler distribution, rather than that of
a fixed, regular distribution, as used in early FEA
models. This spherical model is adopted and extended
in the present study to calculate the elastic properties of
hard particulate-filled composites with a range of filler
volume content slightly above 0.5.
It has been recognized for some time that composite
properties cannot simply be obtained by summing up
the properties of the reinforcing phase and the matrix
phase. The properties of the filler-matrix interface play
a critical role. The concept of an interphase has been
introduced, referring to a distinct interfacial layer of
certain thickness, indicating that there is rarely an
abrupt transition from the filler to the matrix. Filler
coatings with a controlled thickness can be seen as an
engineered interphase. Although many of the theories,
which explain the reinforcing action of fillers, assume
perfect interfacial adhesion between the filler and the
matrix, the case of imperfect adhesion in elastic media
was discussed theoretically by Sato and Furukawa [13].
They assumed that the non-bonded particles acted as
holes. Spanoudakis and Young experimentally investi-
gated glass-filled epoxy resin and found that the best
overall mechanical properties were obtained in com-
posites containing particles treated with a coupling
agent [14,15]. While modeling the thermoelastic proper-
ties of particulate composites containing interfaces with
different degrees of imperfection (or damage), Hashin
[16] and Benveniste [17] developed models that simu-
lated the effect of an interface/interphase with substan-
tially different properties than those of the filler and
matrix as a displacement jump. This analytical device,
which can be applied to various types of interfaces/in-
terphases without clarifying the exact nature of the
‘imperfection’, has been adapted in our FEA model to
investigate the influence of thin interlayers and imper-
fect interfaces on the elastic properties of composites
with low and high filler content.
2. Methods
2.1. The axisymmetric spherical cell finite-element
model
The spherical cell finite-element model was first de-
scribed by Kinloch and Guild [12]. The version used in
this study is shown in Fig. 1. This composite cell model
consists of a glass sphere surrounded by an annulus of
resin or of interlayer and resin, and reflects the overall
isotropy of the material. The FEA code used was
ABAQUS/Standard Version 5.8 [18]. The spherical cell
can be modeled by axisymmetric 8-noded fully inte-
grated elements (CAX8) except at the apex, where
axisymmetric 6-noded triangle elements (CAX6) are
364 W. Wu et al. / Materials Science and Engineering A332 (2002) 362–370
used. The model contains 2944 CAX8 elements and
32 CAX6 elements. Most CAX8 elements have a ra-
dial thickness of 0.1 units out of 10 units, the fixed
outer radius of all cells, so that various particle con-
tents (from 0 to 0.80) and various interlayer thick-
nesses can be readily modeled. The thinnest interlayer
modeled in our work is 0.1 units, compared to the
outer radius of the cell, 10 units.
There are two independent elastic constants for an
isotropic material, and they can be determined by sep-
arately applying hydrostatic and unidirectional pres-
sure. Under both of these loading conditions, sides
AB and CA (Fig. 1) remain stationary for the sake of
symmetry. These boundary conditions are fixed
through each FEA run. One FEA run with a hydro-
static pressure P applied to the cell side BC can easily
determine the bulk modulus K of the isotropic com-
posite sphere as P/3(l/R), where l is the maximum
displacement, and R is the outer radius of the cell.
The second independent elastic constant can be
found by applying a unidirectional load to the cell. In
that case, the overall shape of a deformed isotropic
spherical cell must be an ellipse because this con-
straint reflects the interactions of neighboring parti-
cles. In order to produce an elliptical deformation to
a sphere (Fig. 1) subjected to y-directional strain m,
i.e. the ratio of the displacement at the pole and the
radius of the sphere, the unidirectional loading must
be applied by prescribed x and y directional displace-
ments along each node of boundary BC as:
Dx = − wmx, (1)
Dy =my. (2)
Given an input value of Poisson’s ratio of the cell,
w, Eqs. (1) and (2) provide a set of boundary condi-
tions for a FEA run; the Young’s modulus E can be
found from the average stress | along side AB di-
vided by the y-directional strain m, and | can be ob-
tained from one of the FEA output variables, i.e. the
sum of the y-reactions-to-earth along side AB. Obvi-
ously, E varies with different input values of w, there-
fore an iterative procedure is needed to determine the
true E and w, which fulfill the relationship between
the bulk modulus K, Young’s modulus E and Pois-
son’s ratio w,
E geometrically similar cells of the same volume fraction
K= . (3)
3(1− 2w)
More specifically, varying values of w and repeated
FEA runs give rise to different values of E until the
combined E and w satisfy Eq. (3). The calculation
process of the iterative procedure can be accelerated
by checking the reduction of the x reactions-to-earth
to zero in the FEA data file after each run. This is
equivalent to satisfying Eq. (3).
2.2. The statistical concept behind the FE model
An important feature of the above-described
axisymmetric spherical cell is the incorporation of a
spatial statistical technique developed by Davy and
Guild [10], the form of a representative cell for FEA
is based on a random distribution of filler particles.
The material model is based on the concept that the
interactions of neighboring particles with the given
particle are not directional; the overall effect is an
average arising from all neighboring particles. Thus,
the overall material can be divided into composite
cells, each containing a single particle sphere with a
surrounding matrix. The boundary of a given cell is
the region of matrix closer to that particle than any
other. These cells are the Voronoi cells. For a random
distribution of particles, the distribution of cell sizes
can be calculated [10]. On average, the shape of the
Voronoi cell is spherical. Thus, the overall material
model is a collection of spherical cells of different
sizes, each containing a single particle. Strictly, any
overall property for the composite should be obtained
by summing the contributions from the different cell
sizes. This integration may be carried out practically
by application of a ‘dispersion factor’ to the property
value found for the cell describing the overall volume
fraction. Several procedures have been presented to
implement the above-described statistical results [10].
The simplest is that E and w for a composite are
calculated from only one FEA run for the cell de-
scribing the overall volume fraction. This amounts to
ignoring variations in cell size. However, such a sim-
ple procedure does not merely provide a crude esti-
mate of E and w, especially for composites of high or
low volume fractions (e.g. \0.5). For high volume
fractions, there is only small variability in cell size,
while for low volume fractions, the increase in vari-
ability of cell size is offset by a decrease in the vari-
ability of E and w when the cell size (or cell radius) is
large relative to the particle size (or particle radius).
This procedure is used to calculate the results in the
current paper. Note that the statistical background
behind this straightforward procedure should be em-
phasized; otherwise, this procedure can only be visual-
ized as a composite spheres assemblage (CSA) model
representative of the composite constructed entirely of
(overall volume fraction). However, such a CSA
model is not appropriate in the current application:
according to CSA theory, a composite cell has effec-
tive properties, E and w, which in the strict sense are
equal to the assemblage effective properties if it is
CSA admissible; a composite cell is CSA admissible if
applied homogeneous surface displacements produce
homogeneous surface tractions [9,16]. The homoge-
neous displacement boundary conditions are of form:
 W. Wu et al. / Materials Science and Engineering A332 (2002) 362–370
Ui (S)= m 0ij xj, (4)
and the homogeneous traction boundary conditions
are:
Ti (S)= | 0ij nj, (5)
where S is the boundary surface, and m 0ij and | 0ij are
constant strain and stress, respectively.
Under unidirectional loading in the current applica-
tion, the boundary conditions of Eqs. (1) and (2),
which are homogeneous surface displacements, cannot
produce homogeneous surface tractions as in Eq. (5),
and therefore, the spherical composite cell does not
produce effective E and w in the strict sense when
visualized as a CSA model.
2.3. The effect of high filler content
In the literature, most theoretical calculations for
the elastic properties of particulate filler composites
have been limited to those with an overall filler con-
tent of less than 0.5. Our investigations include com-
posites with higher filler content. In this case, a direct
FEA run for the cell describing the overall volume
fraction could provide accurate values of E and w, as
explained in the preceding section if particles are ran-
domly dispersed within the resin. This requirement
appears to be true for the experimental materials that
are the subject of this study. It has also been shown
that for composites with a low filler content (B 0.48),
particles can be safely assumed to be randomly dis-
persed within the resin; thus all the resin acts as the
continuous phase [10]. It is believed, however, that
with an increase in the filler content, the probability
of filler clustering increases, leading to local phase
inversions where the fraction of resin entrapped within
the aggregate increases [19]. For composites with an
overall filler content greater than 0.5, one may deduce
two possible composite microstructures in addition to
that where particles are randomly dispersed. In the
first case, the resin is completely entrapped within the
filler aggregates or clusters, with particles touching
each other. In this case, one may compute the proper-
ties of composites using the composite cell model with
phase inversions, i.e. the particle sphere is replaced by
a resin sphere, and the annulus of resin is replaced by
an annulus of filler. This is of course an approximate
model because the shape of the entrapped resin can-
not be spherical. However, the elastic properties, E
and w, are considered to be ‘average’ variables, so that
the error due to rounding-off the corners of the en-
trapped resin might be small. In the sections which
follow, theoretical predictions of elastic moduli for
two-phase composites with filler volume contents
greater than 0.5 include the case of phase inversions
also.
365
In the second type of microstructure, the composite
contains a mix of regions with randomly dispersed
particles and regions of resin entrapped within particle
clusters. In this case, one could compute composite
properties using a composite cell model both with and
without phase inversions; then, the composite proper-
ties are obtained as a weighted average of the results
from both regions. This approach could be extended
to composites with more than two regions with differ-
ent microstructures. In principal, such composites
would consist of regions with randomly dispersed par-
ticles, but with each region containing a different vol-
ume of filler.
2.4. Interlayers and imperfect interfaces
Interface or interphase modeling is quite complex.
In this study, the FEA model with 8-noded fully inte-
grated elements of thickness of 0.1 unit is such that
we can incorporate various interface properties by
modifying the elements between the filler and resin
matrix. In practice, interphases can be formed by vari-
ous chemical and engineering approaches, with thick-
nesses estimated to be in the range of 30– 240 nm [20].
The appropriate choice of interphase properties and
thickness is a means of realizing a simultaneous im-
provement in both fracture toughness and composite
strength.
An imperfect interface bond may be due to damage,
such as interfacial debonding, or it may be considered
to result from a very compliant, thin interphase. Both
lead to a poor stress transfer. In fact, when a very
thin interphase layer exists, it is difficult to locate the
exact damage site for the type I imperfect interface. In
other words, the damage (crack) could occur within
the entire region of the interphase layer rather than
precisely at the interphase/filler interface or at the in-
terphase/matrix interface.
Mathematically, both types of imperfect interfaces
cause interfacial displacement jumps between the fiber
(or filler) and matrix [16,17]. In the spherical coordi-
nate system, the stresses and the displacement jumps
at the imperfect interface of an axisymmetric particle
filled cell can be related:
|y = Dr [U m p
r − U r ], (6)
|rq = Dq [U m m
q − U q ]. (7)
Eqs. (6) and (7) describe the imperfect interface in
terms of interface displacement jumps, which are lin-
early related to associated interface stresses. Note that
the interfacial stresses, |rr and |rq, are continuous. In
both equations, Dr and Dq are interfacial parameters
characterizing the degree of imperfection in normal
and tangential directions and are apparently material
properties that could be approximated from experi-
366 W. Wu et al. / Materials Science and Engineering A332 (2002) 362–370
Fig. 2. Young’s modulus of a two-phase composite as a function of
filler content.
Fig. 3. Poisson’s ratio of a two-phase composite as a function of filler
content.
mental data. Infinite values of these parameters imply
a vanishing of the interface displacement jumps, and
therefore, a perfect interface, while zero values imply
vanishing of the interfacial stresses and therefore a
completely disconnected, broken interface. U is the
displacement and the superscripts, p and m, indicate
the particle and matrix. Note that the type II imper-
fect interface is due to a very compliant interphase;
hence, imperfection parameters, Dr and Dq must be
expressed in terms of two independent properties (e.g.
Ei, wi or Ki, Gi ) and thickness, t, of the thin inter-
phase. This is indeed the case; Hashin [16] has shown
that for a vanishingly thin interphase:
Dr =(Ki + 4Gi /3)/t,
Dr /Dq = 2(1− wi )/(1 − 2wi ).
In FEA, Eqs. (6) and (7) can be modeled using
spring elements in normal and tangential directions at
the interface between the filler and matrix. The stiff-
ness of the spring elements represents Dr and Dq, i.e.
the degrees of damage in normal and tangential direc-
tions. Conversely, we can model both type I and type
II imperfect interfaces by using a very thin interphase
layer with imperfection in the normal and tangential
directions expressed by different combinations of Ei
and wi. In our FEA models, this layer can simply be
modeled by very thin solid elements similar to those
used for the particle and matrix, and a successively
decreased modulus Ei models the increased degree of
interface imperfection according to Eqs. (8) and (9).
This approach is taken in this study as it is also used
to model the influence of the thickness and properties
of engineered interphases or coatings on the elastic
properties of composites. A limitation of this ap-
proach, when used in modeling the type I imperfect
interface, is that Dr \ Dq is implied by Eqs. (8) and
(9) because Poisson’s ratio is in the range of 0–0.5.
More complex interphase modeling, including an in-
homogeneous interphase, has also been suggested [21].
Essentially, the above-described interfacial parameters,
Dr and Dq, are replaced in this sort of model by an
adhesion parameter and the variation of interphase
properties along the radial direction is modeled by a
linear, parabolic, or logarithmic equation [21]. This
approach may not provide a particular advantage in
our case, because the interphase is thin along the ra-
dial direction.
It should be pointed out that modeling an imper-
fect interface-by-interface displacement discontinuities
is not necessarily the best choice. The principal ad-
vantage of the displacement approach is that imper-
fect interfaces formed by various mechanisms can be
modeled in a unified, readily implemented approach.
For instance, if a plane crack constituting debonding
is propagating precisely at the fiber/interphase or in-
terphase/matrix interface with a crack surface closed
due to Poisson or residual stress contraction, model-
ing with interfacial stresses satisfying Coulomb’s fric-
tion law (a stress criterion) appears to be physically
unequivocal. However, if the debonded surfaces are
rough and open, interfacial shear stresses may still
exist and Coulomb’s friction law fails.
2.5. Material properties and experiment
The composite whose properties are used in model-
ing calculations is a light-cured epoxy-like resin that
consists of a 60:40 blend of BISGMA/TEGDMA re-
inforced by dispersed spheres of borosilicate glass.
(8) The beads are coated with a silane agent to effect
bonding between the filler and matrix. The literature
(9)
[22] reports that the average Young’s modulus Em for
this resin matrix is 3.5 GPa determined from four-
point flexure tests. We use this value in the following
 W. Wu et al. / Materials Science and Engineering A332 (2002) 362–370
Fig. 4. Effective Young’s Modulus E/Em as a function of interlayer
(interphase) thickness in a three-phase composite of Vf = 0.65.
Fig. 5. Effective Young’s Modulus E/Em as a function of interlayer
(interphase) thickness in a three-phase composite of Vf = 0.4.
Fig. 6. Poisson’s Ratio w as a function of interlayer (interphase)
thickness in a three-phase composite of Vf = 0.65.
367
Fig. 7. Poisson’s Ratio w as a function of interlayer (interphase)
thickness in a three-phase composite of Vf =0.4.
Fig. 8. Effective Young’s Modulus E/Em as a function of interface
damage parameter Em /Ei in a two-phase composite with an imperfect
interface.
finite element parametric studies (Figs. 2–8). Al-
though tensile tests are rather difficult to perform for
the current material because of its brittleness, we have
performed these tests for the same resin and a series
of composites of volume fraction up to 0.53. Under
our test conditions, an average modulus of 3.2 GPa
for the pure resin was obtained. Therefore, for pur-
poses of comparison between theoretical and experi-
mental data, we shift to 3.2 GPa as input for FE
models. Ep for the glass filler particle is 75 GPa. Pois-
son’s ratio wm for the matrix is 0.35, and wp for the
filler is 0.24.
368 W. Wu et al. / Materials Science and Engineering A332 (2002) 362–370
3. Results
3.1. Effect of 6olume fraction of glass fillers on elastic
properties
Finite element cell models, representing a range of
filler (particle) volume fractions from 0 to 0.82, have
been analyzed, and the elastic properties of these mate-
rials are presented in Figs. 2 and 3 as a function of the
filler volume Vf. For filler volumes \0.5, two extreme
cases are considered: particles randomly dispersed
within the resin and resin fully entrapped within filler
particle aggregates or clusters, i.e. phase inversion.
3.2. Effect of the interphase and an imperfect interface
on elastic properties
Numerical studies on the influence of interphases
(filler coatings) with varying thickness (0.1– 0.6 units)
and stiffness (0.5 and 2 Em) on composite properties are
presented in Figs. 4– 7 for medium and high Vf (0.4 and
0.6467). The Poisson’s ratio for the interphases is as-
sumed to be equal to that of the matrix (0.35). Within
a rather wide range of 0.27– 0.42, the Poisson’s ratio’s
effect on the composite modulus is negligible. Note that
along the radial or thickness direction, there is only one
element modeling the thinnest interlayer (0.1 units). In
order to certify the degree of accuracy of complex
stresses around a thin interphase with properties differ-
ent from both the hard filler and resin, stresses around
interphases were transformed to polar coordinates and
plotted along the circumferential direction. All results,
including the following cases of imperfect interphases,
show that radial and shear stresses on either side of the
interface, in the filler and interphase or in the interphase
and matrix, are identical, as required for continuity. The
excellent agreement in radial and shear stresses on either
side of the interface is a stringent test for refinement of
Fig. 9. Theoretical and experimental Young’s modulus of a two-phase
composite as a function of filler content. The input for the matrix
modulus is 3.2 GPa.
the FEA mesh containing a thin interphase, and also
assures the accuracy of the predicted elastic constants, E
and w, as accurate stresses are likely to produce accurate
determinations of E and w.
Numerical results concerning the influence of imper-
fect interfaces with varying degrees of imperfection
(damage) on composite properties are presented in Fig.
8 for high Vf (0.6467). According to Eqs. (8) and (9), we
can model imperfect interfaces by using a very thin
interphase (0.1 units) with the imperfection in normal
and tangential directions implied by different combina-
tions of Ei and wi for this layer; increasing degrees of
imperfection are characterized by a successively de-
creased modulus Ei, as exemplified in Fig. 8 where a
fixed Poisson%s ratio, wi, equal to that of the matrix
(0.35) is assumed for the sake of simplicity. For a
specific composite material with an imperfect interface,
the appropriate Ei, wi could be determined from experi-
mental data, and that Ei should fall on the curve shown
in Fig. 8.
3.3. Experimental 6erification of theoretical models
Provided in Fig. 9 are the average tensile test results
for Vf = 0, 0.3, 0.10, 0.20, 0.355, 0.475 and 0.532 and the
corresponding FE calculated values. The input Young’s
modulus of matrix is 3.2 GPa and it equals the tensile
test result for Vf = 0. The interface quality is considered
to be perfect. The numerical results agree reasonably
well with those of the experimental data. The major
distinction is that numerical values are somewhat lower
than those of the experiments when Vf B 0.5. A possible
explanation for this finding is that the FE models are
based on only one cell describing the overall volume
fraction. Strictly speaking, the contributions from cells
of different sizes should be calculated and summed up.
Such a simple procedure is most crude for intermediate
Vf as explained in the Section 2.2. Generally speaking,
the power of the current model has been proven, and it
provides the confidence for the validity of the results of
the parametric studies (Figs. 2–8) presented here.
4. Discussion
It is found from Figs. 2 and 3, and where we assume
no phase inversion, that the Young’s modulus of the
composite increases from 3.5 to 13.72 GPa as the filler
content increases from 0 to 0.647 by volume. The rate
of increase, increases with Vf. The calculated Poisson’s
ratio increases up to a Vf of 0.1, and thereafter, de-
creases. Intuitively, it seems that this ratio should de-
crease monotonically with increasing filler content, and
we speculate that the initial increase can be attributed
to special deformation restraints due to the spherical
geometry.
 W. Wu et al. / Materials Science and Engineering A332 (2002) 362–370
For the curves describing the phase inversion struc-
ture (Vf \0.5), the Young’s modulus of the composite
increases from 38 to 61.21 GPa as the filler content
increases from 0.517 to 0.82. The modulus values for the
phase inversion structure are much higher than those for
the normal structure of particles enclosed by matrix.
This can be explained by the ‘stiff cage’ effect of the
annulus of glass. The increase is linear with Vf, i.e. a
constant rate of increase, because the stiffness of the
inner matrix is negligible. However, the experimental
value for Vf =0.562 seems to indicate that phase inver-
sion has not yet occurred for the experimental materials.
On the other hand, the calculated Poisson’s ratio with
presumed phase inversion is lower than that without
phase inversion, but increases with Vf, a finding that is
counterintuitive. This can also be attributed to deforma-
tion constraints due to the spherical geometry.
The primary numerical conclusion from Figs. 4 and 5
is that the Young%s modulus of composites varies nearly
linear with the change of the interphase thickness. This
conclusion is valid for two different Vf and interphase
stiffness values chosen arbitrarily, and is assumed to
hold for other values of Vf and interphase stiffness. It
also provides the engineer-designer with an expeditious
estimate of properties for filled composites with various
coating thicknesses. It is also interesting to note that for
a fixed Vf, the linear decrease and increase rates are
same for two interphases of the same Ei /Em (hard) and
Em /Ei (soft). The higher the Vf, the higher the rate of
increase or decrease, because an interphase of certain
stiffness and thickness plays a more prominent role in a
high Vf composite tantamount to a lesser proportion of
the matrix. The general tendency of changes in Poisson’s
ratio is again more difficult to comprehend. The numer-
ical values of w in Figs. 6 and 7 appear to initially vary
in a linear manner and subsequently remain more or less
constant; some slight increase or decrease in the second
segment of the curve is a numerical fluctuation due to
the iteration procedure). As in the modulus curves, the
initial rates of increase and decrease are nearly equal.
Unlike the case of the modulus, however, the variation
or deviation of w from that of the two-phase composite
(Ri − Rp =0 with Ri and Rp being the radii of the
interphase and particle, respectively) is negligible. As a
reasonable approximation, Poisson’s ratio for the two-
phase composite could be taken as that of a three-phase
composite with an interphase having a modulus approx-
imately twice that of the matrix.
The study of the effect of the interface strength in Fig.
8 shows that the growing imperfection or weakening of
the interface successively decreases the composite mod-
ulus until it asymptotically attains the value for a
debonded interface, giving rise to a voided matrix or
removal of the filler particle; therefore, with an increas-
ing degree of imperfection, the composite modulus is
lower than that of pure matrix.
369
A note in passing is that the current model assumes
a unique interface parameter Dr for tension and com-
pression. In fact, when the radial displacements around
the interphase with a high degree of imperfection mod-
eled by a low Ei are examined, the interpenetration of
the filler and matrix is implied, which is physically
impermissible. Indeed, Dr (Eq. (6)) could be different for
tension and compression in many scenarios; it is plausi-
ble to assume that in compression, Dr is infinitely large.
Modeling different Dr in tension and compression is not
necessary in the current study because the overwhelming
proportion of the interface is in tension, so the overall
material properties should be insensitive to some local
interpenetration.
5. Conclusions
A predictive finite element model was used to investi-
gate the elastic properties of a spherical glass bead-rein-
forced resin matrix composite with a range of filler
content. An important feature of the axisymmetric FE
cell model is the incorporation of a spatial statistical
technique developed by Davy and Guild [10], which
may provide a real description of a random distribution
of filler particles in the matrix. The power of this model
is confirmed by the uniaxial tensile test results for
composites with a range of volume fraction up to 0.53.
Subsequently, we illustrated how this model can be
modified to study the effect of imperfect interfaces on
the elastic properties of composites, and to become a
useful tool for designing an engineered interphase be-
tween filler and matrix. The Young’s moduli of com-
posites vary approximately linearly with a change in
interphase thickness for any filler content, and the rates
of modulus increase and decrease are similar for both
soft and hard interphases having equal Em /Ei and Ei /
Em.
Acknowledgements
This work was supported by United States Public
Health Service grant DE 09530.
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