Composites Science and Technology 53 (1995) 301-315

@ 1995 Elsevier Science Limited

Printed in Northern Ireland. All rights reserved
ELSEVIER 0266-3538(95)00001-l 0266.3538/95/$09.50

EFFECT OF SOLIDIFICATION RATE AND METAL

FEEDABILITY ON POROSITY AND SiC/A1203 PARTICLE
DISTRIBUTION IN AN Al-Si-Mg (359) ALLOY

A. M. Samuel, A. Gotmare & F. H. Samuel*

Dkpartement des Sciences Applique’es, Universite’du Qutbec ri Chicoutimi, Chicoutimi, Qutbec, Canada, G7H 2Bl

(Received 11 August 1994; accepted 25 November 1994)

Abstract particles takes place at smaller DASs, that changes to

In the production of particle-reinforced metal-matrix
composite castings, particle sedimentation during the
melting process and particle redistribution during
solidification can lead to particle segregation in the
as-cast structure, the effects of which, in addition to
those of porosity, can be highly detrimental to the
properties and quality of the casting. Solidification rate
and metal feedability are considered mainly respon-
sible for the two problems. The present work reports on
the inpuence of these factors on the particle distribution
and porosity in 359 alloy composites reinforced with
Sic and Al,O_, particles. The results show that the
microporosity observed in 359/SiC,, composites is a
consequence of pore nLccleation at the Sic particle sites
and hindered liquid metal flow due to particle
clustering; the former is responsible for the skewed
porosity distribution projiles typically observed in these
composites, similar to the type I distributions observed
in A356 alloy. In the 359/Al,O,,,,, composite, limited
feedability and the wider range or larger particle sizes
o,f the alumina particles result in the bell-shaped
porosity profile observed, as well as the larger
maximum pore size range (IOO-180p,m2 against
O-40 pm2 for the Sic,, composites}. The interparticle
distance distributions for the Sic,,, composites show
that ,finer dendrite arm spacings (DASs) produce a
more uniform distribution of the Sic particles, while
higher spacings lead to particle clustering, usually at
separations of about 5 pm, the probability increasing
with increase in Sic,,, content. In the 359/Al, O.?,,,,
composite, the distribution profile changes from a
normal, random distribution to an exponential type as
the DAS is increased. Together with the microstructural
observations, the distributions indicate that particle
pushing is the dominant phenomenon in the Sic,,,,
composites during solidification, whereas in the
Al&1,, composite, mechanical trapping of the
* To whom correspondence should be addressed.
301
particle pushing at larger spacings.
Keywords: particulate metal-matrix composites, Sic,
A&OX, porosity distribution, interparticle distance dis-
tribution, solidification
INTRODUCTION
Discontinuously-reinforced aluminum (DRA) metal-
matrix composites (MMCs) have been the subject of
much attention in recent years’,2 on account of their
promising potential as key engineering materials
and their relatively low production costs compared
to continuous-fibre-reinforced MMCs. Among the
various techniques reported in the literature for
producing these MMCs, that of incorporating fine
particulate ceramic reinforcements into molten metal
alloy has been of particular interest, having been
exploited to reach commercial production levels, as
witnessed by the aluminum alloy composites rein-
forced with silicon carbide or alumina particles
available on the market today.“.4
While such materials can be remelted easily and
cast into near-net shapes, rolled or even forged,
sedimentation of the reinforcement particles during
melting, and their segregation during solidification can
be a serious disadvantage with respect to the resultant
casting. an uneven distribution of the rein.forcement
lowering the composite strength.’ Even if uniform
dispersion of particles can somehow be ensured in the
melt, they can still become segregated in inter-
dendritic regions during solidification, the dendrite
growth rate of the matrix being an influential factor in
this respect. As the properties of the composite are
known to be critically dependent upon the distribution
of the reinforcement, it becomes important, therefore,
to have an understanding of the particle movement
and distribution in order to maximize the commercial
applicability of these MMCs.’
302 A. M. Samuel, A. Gotmare, F. H. Samuel

Another point of concern with respect to casting
quality, be it that of a composite or an alloy, is that of
porosity. Particle-reinforced MMCs are invariably
associated with this problem, although the presence of
the reinforcement particles has been seen to be
beneficial in some respects.7 The properties of the
composite are adversely affected, nonetheless, de-
pending upon the porosity content in the composite
casting.x
The factors most likely to influence both problems
are essentially those of solidification rate and metal
feedability, the former affecting the particle segrega-
tion, and the latter, porosity formation, with other
factors like dendrite arm spacing (DAS) of the matrix,
reinforcement particle size, thermal properties of the
matrix and reinforcement, etc., being automatically
implicated within their context.
On the basis of our previous investigations on
Al-Si-Mg composites reinforced with SIC and, more
recently, A&O3 particles, covering divers aspects of
these composites, ‘-I3 it was thought appropriate also
to study the influence of solidification rate and metal
feedability on the particle distribution and porosity in
these composites. The results of our investigations on
359/SiC/lOp, 359/SiC/2Op and 359/A&OJlOp com-
posites are reported in this article. The data on
porosity have been compared with those obtained for
A356 alloy-an important alloy in automotive and
other applications, from the point of view of assessing
the feasibility of the present composite materials as
replacements for the popular primary casting alloy.
EXPERIMENTAL PROCEDURE
The chemical compositions (as obtained from
inductive couple plasma (ICP) analysis) of the A356
alloy and the three composites used in the present
study are shown in Table 1. The SiC(,, reinforced
composites (10s and 20s) were received in the form of
12.5 kg 359/SiC/lOp and 359/SiC/2Op ingots from
Duralcan Canada, Usine Dubuc, Chicoutimi, Quebec.
The AlZQ3,,, reinforced composite was received in the
form of 6061 /A1203/20p cylindrical ingot.
The 359/SiC,,, ingots were cut into small pieces and
melted in 2 kg capacity silicon carbide crucibles, using
an electrical resistance furnace. In order to convert
the 6061 alloy into 359 alloy (matrix of the three cast
composites) to produce the 359/A1203/10p composite,
commercially pure aluminum and metallic silicon were
added to the 6061/A1203/20p melt to achieve the final
composition shown in Table 1. In all cases, the melt
was stirred mechanically, using a specially designed
impeller (-80 rpm at 735°C). The melt hydrogen level
was determined using the Leco vacuum fusion
technique and found to lie in the range 0.13-
O-15 ml/100 g Al.
Casting was done in a metallic permanent mold of
low-carbon steel (heated at different temperatures).
The mold was designed to promote directional
solidification. Typical casting dimensions and shape
are shown in Fig. 1. The inner surface of the mold was
coated with a thin layer of graphite (-50 pm). Before
pouring, the mold was tilted at 35” (with respect to the
horizontal axis) and moved up slowly during filling to
avoid turbulence.
Samples for metallographic observation were
sectioned normal to the solidification direction, at the
positions marked l-4 in Fig. 1. The samples were
polished by a technique especially developed for
SiC/A1203 particulate MMCs. Observations were
made with an optical microscope (Olympus PMG3).
No etching was applied. Porosity measurements were
made by image analysis (Leco 2001 image analyser in
conjunction with the optical microscope, at a
magnification of 200 times) and an appropriate
number of fields depending on the surface area, so as
to cover .the entire specimen surface (for details see
Ref. 9). The pore count was then normalized for
comparison purposes, to represent pore number per
constant surface area.
For interparticle distance measurements, several
optical micrographs (taken at 200 times magnification)
were enlarged to obtain 19 cm X 24 cm photographic
prints. The interparticle distances were then measured
by the line intercept method,14 by means of intercept
lines drawn from edge to edge across the prints, at
least 10 lines per photograph. In doing so, more than
400 particles were considered in each case.

Table 1. Chemical compositions of the A356 alloy and the three composites used in the
present work”

Alloy/ Designation Element (wt %) Reinforcement

composite type (vol.%)
Si Mg Ti Fe Cu Sr

A356 A356 7.11 0.40 0.09 0.10 0.01 -

359/SiC/lOp 10s 9.45 0.58 o-11 0.14 o+O2 0.014 11.3
359/SiC/2Op 20s 940 0.59 0.10 0.14 0.01 0.009 21.0
359/Al,O,/lOp 1OAL 10.91 0.42 0.009 0.02 0.12 - 12.0

u Obtained from ICP analysis.

 Particle distribution and porosity in 359 alloy composites 303

types can occur simultaneously and can significantly

affect the quality of the casting.”
During the course of solidification, several types of
feeding are involved at different stages of the
solidification. These include liquid, mass, inter-
dendritic and solid feeding, that occur from the initial
through the final stages of solidification.‘h A schematic
representation has been given previously.” Porosity
defects are caused by the limitations of these feeding
mechanisms, and it is thought that the interdendritic
feeding stage is the most important stage for their
creation. It is worthwhile mentioning here that, while
it has long been well understood that careful control
of the hydrogen level in the molten alloy is required to
achieve relatively porosity-free castings, more atten-
tion is now being paid to the feedability of the alloy:
the feedability is affected by the hydrogen level
present in the melt and considerably affects the
shrinkage and/or microporosity observed in a
particular casting.
Micro- or interdendritic porosity is frequently
observed in aluminum-base alloys, and is generally
attributed to failure of interdendritic feeding and the
precipitation of dissolved hydrogen gas, and the
usually long freezing range of most aluminum casting
alloys.‘x A mathematical model has been developed’”
Fig. 1. Front and side views of the casting obtained from the to investigate the effects of casting parameters on the
step-like metallic mold used in the present study. formation of microporosity in a casting due to
Metallographic specimens were sectioned normal to the
solidification direction at the positions marked l-4. interdendritic fluid flow during alloy solidification.
This” shows that the development of microporosity in
a casting can be decreased if alloys with narrower
mushy zones are used (similar to the 359 base alloy
RESULTS AND DISCUSSION used as matrix for the present composites), as well as
by those casting parameters which can enhance the
Porosity distribution cooling rate.
The shrinkage that occurs on solidification is the
In the present work, porosity size was classified into
primary source of porosity formation in solidifying
two groups: (a) microporosity for pore sizes (as
castings. In most cast alloys, the volume shrinkage
measured by the pore surface area) below 1000 pm’;
varies typically from 5-8%. Shrinkage porosity also
and (b) macroporosity for pore sizes larger than
occurs on a ‘micro’ level as ‘microshrinkage’ or
1000 pm’. It should be noted that this type of
‘microporosity’ which is dispersed in the interstices of
classification is arbitrary, as has been discussed in our
dendritic solidification regions, typically found in
earlier work. In fact, what is termed as ‘microporosity’
alloys with long solidification ranges (e.g. the 65-75°C
can vary from O-500 000 pm2 for A356 alloy to
range observed for A356 alloy for
O-25 000 pm2 in the case of the 359/SiC(,,
solidification/cooling rates lying between O-8 and
composites.’
16”C/s’*). Limited or inadequate liquid metal feeding
in the dendritic solidification area is instrumental in
356 alloy
the formation of this type of porosity.
As mentioned earlier, this alloy was used as a
The other main source of porosity arises from gas
reference due to its high industrial applicability, and
evolution resulting from a decrease in solubility of the
to compare its performance uis a uis the present
gas in the alloy on solidification. The gas so rejected
composite materials. Figure 2(a) displays the porosity
can nucleate both in the liquid during solidification
distribution in the range O-25 000 pm2 (obtained by
and in the solid immediately afterwards, giving rise to
image analysis). Three observations could be made:
two very different kinds of porosity, termed
‘interdendritic (or primary) porosity’ and ‘secondary (i) no pores were observed in the range
porosity’, respectively. These effects are typically O-1000 wm*, regardless of the sample section
exhibited by hydrogen in aluminum. Both porosity position or the mold temperature;
304 A. M. Samuel, A. Gotmare, F. H. Samuel

(iii) increasing the mold temperature from 25 to

450°C significantly increased the pore density.

Figure 2(b) shows the porosity distribution for pore

sizes greater than 25 000 pm*. These pores are mainly
shrinkage cavities or a combination of gas and
shrinkage porosity, or may even represent the extent
to which the shrinkage cavity forms in the riser
(depending upon the position where the sample is
sectioned), as can be observed from the pore shapes in
Fig. 2(c).
From Fig. 2(a) and (b), one can reasonably estimate
21 I5 28
that even with the use of a simplified mold geometry
13 24 50

DAS WN
as that of Fig. 1, porosity in Al-Si alloys may be
minimized if (a) the mold temperature is high enough
(a) to allow the liquid metal to fill the mold before
20r solidification starts (i.e. 250°C for the present mold
configuration), and (b) the hydrogen content is low
(0.13 ml/100 g Al).
The observation that microporosity in A356
castings is mainly a combination of gas and shrinkage
stems from the fact that such a combination is
essential for pore formation on account of the critical
nature of the conditions required for pore nucleation
to take place in a solidifying casting. These are
embodied in the expression:
PC + P, 2 P,,, + PH + y( 1/r, + 1 /r,)

where PG + I’, (the internal gas and shrinkage

DAS (I-Lm) pressures) represents the internal pressure 8 of the
(b) pore, which must be sufficient to overcome all of the
external forces acting upon it, i.e. the atmospheric
pressure, P,,,, the metallostatic pressure head, PHI and
the forces due to surface tension, y, of the solid/liquid
alloy in contact with the pore (and expressed as y
(l/r, + l/r*), r, being the principal radii of curvature of
the pore).
In a parametric study of microporosity in Al-Si
foundry alloys,*” statistical analyses were used to
describe the size and amount of porosity (as measured
by image analysis) as a function of alloying and
process variables in A356 casting alloy. The pore size
distributions could be divided into three types: type I
containing only one population of pores, skewed
toward small pore sizes; type II containing a bimodal
population of pores, with one population centered at
low pore sizes and another concentrated at large pore
(cl sizes; type III, again containing only one population of
pores, this time skewed toward the large pore sizes.
Fig. 2. Porosity distributions in the range (a) O-2.5 000 pm’,
(b) 25 000-100 000 pm* for A356 alloy. (c) Microstructure
Taking into account the hydrogen content and local
showing porosity size and shape in A356 alloy solidified at solidification time, among other parameters, and the
lO”C/s (samDle
. . corresponding to position 4, mold number of pores obtained in each type, the three
tempirature I-2X).’ distribution types were then attributed, respectively,
to porosity resulting mainly from nucleation of pores
(ii) lower sections were found to be much sounder (type I), porosity formed by nucleation and growth of
than the upper sections for the three mold pores (type II), and porosity increasing mainly due to
temperatures studied; growth and coarsening of pores (type III). Of all the
 Particle distribution and porosity in 359 alloy composites 305

parameters studied, the hydrogen content was found dendritic shrinkage or gas evolution at lower cooling
to be the most important factor in determining the rates, as shown in Fig. 3(e) and (f). In both cases, the
size and amount of microporosity formed. The pores were observed to be ‘smeared’ or surrounded by
porosity distribution plots for A356 alloy shown in the SIC particles.
Fig. 2(a) and (b) show an overall agreement with Figure 4(a) and (b) illustrates the distribution of
these observations. microporosity in 10s and 20s composites, respectively.
The main observations to be noted are: (a) increasing
Sic reinforced composites the mold temperature improves the metal feedability
The relationships between the mold temperature, as seen by the decrease in pore count for samples
sample position and the resulting dendrite arm spacing taken from the lower sections, however, at the cost of
PAS) of the as-solidified microstructure for increasing the microporosity (mainly shrinkage type)
359/SiC,,, composites are summarized in Table 2. An in the upper sections; (b) increasing the volume
earlier study’ showed that the porosity shape and size concentration of SIC particles significantly increases
were affected by the presence of the Sic reinforce- the pore count. Figure 4(c) clearly shows that the
ment particles through the tendency these particles effect of increasing the Sic volume fraction from 0.1
display to block or restrict the growth of the pores. As to O-2 on porosity formation is almost twice that
a result, a more uniform distribution of porosity was obtained on raising the mold temperature from 25 to
obtained compared to the unreinforced matrix alloy, 450°C. The type and nature of the porosity
where the porosity was seen to occur in the distributions will be discussed in the next section,
interdendritic regions that easily spread across several when the three composites are compared together.
dendrites when adjacent pores merged into each Figure 5(a) and (b) shows the porosity distribution
other, leading to very large pore sizes. In this way, the for pore sizes greater than 1000 pm’. Increasing the
composite material could be regarded as having a mold temperature from 25 to 250°C for the 10s
beneficial effect on the growth of porosity. composite resulted in a noticeable improvement in the
Figure 3(a)-(f) demonstrates the different forms pore count for lower sections. This advantage,
and sizes of pores observed in 359/SiC/lOp composite however, was lost when the mold temperature was
(with a solidification temperature range of 25--30°C raised to 450°C. For the upper (thicker) secions, pores
for cooling rates of O-8--16”C/s). Microporosity was in the range 1000-5000 pm2 were replaced by coarser
observed to form in different ways: (a) through ones, of the order of 15 000-25000 Frn’. Similar
nucleation at the SiC@,/matrix interface, as shown in behaviour was exhibited by the 20s composite, where
Fig. 3(a) and delineated by the arrows in the enlarged increasing the mold temperature was seen to
section shown in Fig. 3(b); (b) due to improper contribute to finer porosity (1000-5000 pm’) in the
feeding, where the fluidity/flowability of liquid metal lower sections and coarser porosity in the upper ones,
was insufficient to fill the. gaps between adjacent Fig. 5(b).
particles, Fig. 3(c); and (c) in the interdendritic From the above findings, nucleation and growth of
regions, due to limitation in feeding, as shown in Fig. pores during solidification of 359/SiC,,, reinforced
3(d). Macroporosity mainly occurred due to inter- composites (over a narrow temperature range, about
25°C) may be explained schematically as shown in Fig.
6. When solidification starts (i.e. at temperature
T = T,), a network of a-aluminum dendrites is
Table 2. Average thermal parameters and DA!%
developed. As solidification progresses (i.e. T, < T <
measured from 359/SiC~,, composite castings
T,,J. the SIC particles (that already exist in the melt)
Mold Sample DAS Cooling Solidification are rejected in front of the advancing a-aluminum
temperature position (pm) rate” time’” dendrite network. At this stage, one may reasonably
(“C) (“C/s) (s) presume that there is an accumulation oE hydrogen gas
1 13 46
in the pockets of interdendritic liquid due to the
25 2.3
2 16 27. 4.7 decrease in solubility accompanying solidfication.
3 18 19 6.9 This, and the inability of the solidification shrinkage to
4 21 13 9.5 be fed through the almost frozen (‘mushy’) liquid are
250 1 15 28 4.5 conditions that favour the role of Sic particles as
2 19 15 8.2 preferential sites for heterogeneous pore nucleation.
3 23 9.5 12.7 When the temperature reaches the eutectic tempera-
4 28 5.0 23.4 ture (i.e. T = T&, the growth of the pores is limited
4.50 1 24 8 15.0 by their ability to expand in a viscous media, by their
2 30 3.5 37.8 edges being surrounded by the SIC particles, and by
3 42 1.5 73.4
53 0.8
the simultaneous precipitation of eutectic Si particles
4 10x,0
from the remaining melt, where these particles are
306 A. M. Samuel, A. Gotmare. F. H. Samuel

Fig. 3. Microstructure showing porosity size and shape in 359/SiC/lOp composite solidified at 0+X/s (sample corresp.onding to
position 4, mold temperature -450°C): (a) microporosity; (b) enlarged portion of porosity in (a); (c) and (d) porosity due to
improper feeding, caused by segregation of Sic particles at separation distances of -5 pm; (e) and (f) interdendritic shrinkage
porosity.
 Particle distribution and porosity in 359 alloy composites 307

10s sw.m
I O-40
q 40-80
q 80-120
80
i :g:;
;
n 200-240 :
” 60
z
2
40

0
13 21 15 28 24 50
0
13 21 15 28 24 50
DAS (pm)
DAS (km)
(a)
(a)

0
13 21 15 28 24 50

DAS km)
@I

Fig. 5. Porosity distribution in the range 1000-25 000 pm’

for: (a) lOS, (b) 20s composite.

800

;
the narrow gap between two adjacent particles
2 (attributed to a capillarity-type phenomenon), Fig.
0 600
e 7(a), or the cavity formed by several particles, Fig.
ct 7(b). The plot of porosity distribution, Fig. 7(c), shows
400
no presence of the fine porosity in the range O-40 pm*
which represents the majority of fine pore sizes
observed in the Sic,,, reinforced composites, Fig. 4(a)
and (b). In the Al,O,(,, composite, however, the
0 maximum porosities are in general observed to lie in
13 21 15 28 24 50

DAS (w) the 10G180~m2 range, giving a porosity profile that

(cl
Fig. 4. Microporosity in the range O-240pm* for: (a) 10s;
(b) 20s composite. (c) Comparison of porosity (<lo00 pm*)
in the two composites.
pushed towards the centre of the interdendritic
(i.e. opposite to the direction of expansion
pores) by the advancing a-dendrites.
A&O., reinforced composite
Microporosity in this composite type mainly arises
from the insufficient flow of liqiud metal to fill either
is bell-shaped, compared to the skewed type of profile
observed in the case of the SiC(,, composites (Fig.
4(a) and (b)).
Referring to the porosity distribution types
observed previously2” for A356 alloy, one finds that
region the Sic,,, composites exhibit porosity profiles that are
of the typical of the type I distribution. This is to be
expected, due to the presence of the SIC particles in
the matrix alloy, where there is a tendency for pores
to nucleate at their sites (Fig. 3(b)). We have also
observed the tendency of the SIC particles to restrict
pore growth (Fig. 3(c) and (d)). A combination of
308 A. M. Samuel. A. Gohnare, F. H. Samuel

(a)

Viscous
liauid aluminum

(b)

Solid aluminum

4(&m
-_.-__i
(b)
250
r ww

Cc)
z
a” loo RT- I RT-4 250- 1 250-4 450-I 450-4
Fig. 6. Schematic diagram showing the different stages t
leading to pore formation in SIC<,,reinforced composite: (a)
T = 7;; (b) T, < T < T,,,; (c) T = T,,,.
SO

these two factors accounts for the typical skewed

0
distributions observed for both Sic(,) composites. The 13 21 15 28 24 50

low hydrogen content of the composite melts and the
relatively shorter solidification times involved (com-
pared to the A356 alloy) would also support a type I
distribution.
As for the A&O,,,, composite, as observed earlier,
its porosity distribution has a bell-shaped profile, that
only partly fits in with a type II distribution,
corresponding to porosity formed by nucleation and
growth of pores. The microstructural observations
show, however, that it is not so much a nucleation and
growth process that is responsible for the porosity
distribution observed, but rather a feedability problem
DAS (v)
(c)
Fig. 7. Porosity observed in 359/Al,O,/lOp composite
samples, showing: (a) microporosity; (b) macroporosity:
(c) porosity distribution in the range O-240 pm*.
that produces an insufficient flow of liquid metal to
fill either the gaps between two adjacent alumina
particles or the cavities between several surrounding
particles (Fig. 7). The wide range of, and larger
particle sizes of the alumina reinforcement (4-60 pm,
 Particle distribution and porosity in 359 alloy composites
average particle size about 23 pm) compared to the
Sic particles (average particle sizes of 12 and about
15 km for TOS and 20s composites, respectively) also
aid in hindering the feedability. Thus it is not strictly a
‘growth process’ that is resulting in the shift to the
larger pore sizes observed in the porosity distribution
plot, hut also the effect of larger gaps and cavities that
form due to the nature of the Al$& particles
themselves. The Al& particle density was about
4.6 x l@/cm’ (S*Ox 10J/cmz for the 10s composite).
A model describing the mechanism of porosity
formation as depicted in Fig. 7 has been presented in
detail elsewhere.*’
Particle distribution
One of the main problems associated with the
production of particle-reinforced composites using
conventional melt technology is that of particle
sedimentation (i.e. particle settling in the melt). The
resulting inhomogeneous distribution of the particles
in the melt together with the effects of particle
density, shape, and size, and gravity give rise to the
particle segregation or agglomeration observed in the
as-cast structure of the composite. As a well dispersed
distribution of these particles in the matrix alloy of the
MMC is essential for optimum mechanical properties,
it becomes important to identify and control the
process parameters related to this problem. Mechani-
cal stirring being usually incorporated during melt
preparation/holding, the stirring conditions, melt
temperature, and the type, amount and nature of the
particulate reinforcement are some of the main factors
to consider when investigating this phenomenon, as
witnessed by previous studies.‘.22
In addition to the sedimentation and agglomeration
effects, particle redistribution can also take place
during solidification through the action of the moving
solidification front that either rejects or engulfs the
particles as it moves through the casting. It has been
reported” that the non-uniform distribution of Sic
particles in 3 pm SiC@,/Al castings is produced during
solidfication and not during mixing of the molten
melt_
Several theories have been proposed to explain the
mechanisms of particle redistribution and particle
pushing and trapping.” Generally, a critical velocity
V,, is predicted, which determines whether the
particles will be rejected or trapped by the advancing
solidification front. Among the various factors
influencing VCI- are the surface energy, particle
characteristics like radius, size, thermal conductivity
and amount or concentration, as well as the impurities
existing in the liquid melt that can affect the melting
point.
In the following sections, the particle behaviour in
the composites studied has been inferred from the
309
particle distribution in the microstructure after
solidification. This method gives a good correlation
when the dendrite arm spacing of the as-cast structure
is larger than the particle size,** as is the case
generally observed in the present work.
Sic reinforced composites
Figure 8(a) and (b) shows the particle distributions
observed in lower section samples obtained at a motd
temperature of 25°C (DAS -13 pm) of 10s (average
particle size -12 Frn, representing >45% of the total
number of particles) and 20s (average particle size
-15 pm) composites, respectively. As can be seen,
the SIC particles are, on the whole, uniformly
distributed throughout the matrix, and appear to be
the result of particles pushing into the interdendritic
regions by the advancing ol-aluminum dendritic front.
This phenomenon is made more. apparent if one
examines the microstructure of the thicker sections
obtained at 450°C (DAS -55 pm), Fig. 8(c) and (d),
for 10s and 20s composites, respectively. where
particle clustering in the interdendritic regions is
clearly visible.
Several expcrimentai studies have heen carried out
in order to determine the critical velocity V,, and to
study particle pushing in the solidification of MMCs.
The results show that the particle/matrix combina-
tions belong to one of three categories, where (i) the
particles are captured by the solid/liquid interface at
all growth conditions; {ii) where they are dependent
upon a critical velocity V,, that decides if they will be
pushed or trapped by the interface; and (iii) where
they are pushed at any growth condition.**
Analysis of segregation of Sic by settling and
particle pushing in cast W&,/Al alloy MMCs*’ shows
that the models for particle pushing based on thermal
properties agree with the experimental results of this
system, although no current model encompasses all
the experimentally observed features. However, these
models need to be refined to include additional
features such as pushing of clusters, particle chemistry
and, in particular, the shape of the growth front,
which is dendritic, rather than planar in such
composites.
Figure 9(a)-(c) represents the interparticle distance
distribution histograms for 10s composite for mold
temperatures of 2.5, 250 and 45O”C, respectively,
obtained from image analysis measurements of sample
cross-sections (edge-to-edge). As mentioned pre-
viously, sample sections were taken normal to the
solidification direction to represent the entire casting
at a given mold temperature. The main observations
to be made from the three histograms are:
(i) finer DASs (close to ur even greater than the
average Sic particle size) produce a more
 A. M. Samuel, A. Gotmare, F. H. Samuel

Fig. 8. Microstructures showing Sic, distribution in 10s and 20s composite samples obtained at different DASs: (a) lOS,
13 pm; (b) lOS, 53 pm; (c) 2OS, 11 pm; (d) 2OS, 50 pm.

uniform distribution of the SIC particles. An
initial tendency toward clustering at inter-
particle distances in the range O-8 pm can be
observed;
(ii) increasing the dendrite arm spacing contributes
to segregation/clustering at separation distances
of O-5 pm, followed by exponential distribution
thereafter. This segregation is what accounts for
the limited feedability and associated porosity
observed in the microstructure of Fig. 3(c).
It should be mentioned that in the 10s composite,
Sic-free areas (caused by an insufficient number of
particles to cover the entire matrix surface) extending
up to 150 pm were frequently observed in the
microstructure (Fig. 8(a)). This would explain the
larger Sic interparticle distances in the histograms of
Fig. 9. A comparison between Fig. 9(a) and (c) shows
a more significant tail in the latter, especially for the
upper section samples with corresponding larger
dendrite arm spacings. It has been observedz4 that a
long tail is present in the interparticle distance
histogram of a slowly solidified investment cast sample
of ALSi/SiC/2Op composite, that is not present in the
case of a die cast sample of the same composite. The
tail is a consequence of the SIC particles being
separated by the large solidification cell size of the
investment cast sample. It has also been pointed outz4
that inhomogeneity of the particle shape, size and
distribution render it inappropriate to propose
discrete expressions for interparticle spacing in terms
of the volume fraction and particle size of the
reinforcement. At the same time, quantitative
determination of this inhomogeneity is not an easy
task to attempt.’
Increasing the SIC particle number, i.e. on going
from 10s to 20s composite, was found to increase the
probability for SIC particle clustering at separation
distances of 5 pm or less (Fig. lo), to reach a
maximum at a dendrite arm spacing of -55 pm. The
increase in the SIC particle number also led to a
reduction in the larger Sic interparticle distances (see
Figs 9(a) and 10(a)).
In a study of the dendritic segregation in
 Particle distribution and porosity in 359 alloy composites 311

70

&j 1OS RT-4 a2OS RT-4

q 10s RT-3 60 a 20s RT-3
q lOS RT-2 a 20s RT-2
n lOS RT-I SO
l 20S RT-1

3
; 40
x
s 30

r;
20

II 22 33 44 55 66 71 88 99 110 ’ 0 II 22 33 44 55 66 77 88 99 110

SIC Interparticle distance (Km) Sic Interparticle distance (pm)

(a) (a)
70
70
a 10s 250-4 q2OS 250-4
60 q 10s 250-3 60 q20s 250-3
fg 10s 250-2 q20s 250-2
IlOS 250-l 50 n 2os 250- 1
50
s
40 ; 40
E
J
w 30
e
I&
20

10

O 0 11 22 33 44 55 66 77 88 99 110 O 0 11 22 33 44 55 66 77 88 99 II0
Sic Interparticle distance (km) Sic Interparticle distance (rm)

(b) @)

6J I OS 450-4 Q2OS 450-4

er 10s 450-3 e3 20s 450-3
q 1OS 450-2 @2OS 450-2
l 1os 450-l mzos 450-I

s- 40
6
0
g. 30
e
IL
20

10

O 0 II 22 33 44 55 66 77 88 99 110
SIC Interparticle distance (Km) SIC Interparticle distance (Frn)

(c) (c)

Fig. 9. SIC interparticle distance distribution histograms for Fig. 10. Sic interparticle distance distribution histograms
10s composite samples obtained at different mold for 20s composite samples obtained at different mold
temperatures: (a) 25°C; (b) 250°C; (c) 450°C. temperatures: (a) 25°C: (b) 250°C: (c) 450°C.

particle-reinforced cast aluminum composites,5 the an Al-3Mg matrix alloy variously reinforced with Sic,
effects of matrix DAS, particle size, thermal B& TiB2, A&O3 and ZrB2 particles, for particle sizes
conductivities of matrix against particles and the ranging between 3 and 25 pm, and DASs of 5-50 pm.
difference in contact angles between particle/liquid The results indicated wide variations in segregation
and particle/solid interfaces were investigated, using behaviour among the different particle types, with
312 A. M. Samuel. A. Gotrnare, F. H. Samuel

segregation being observed to be most severe for the

lowest particle size and highest DASs, respectively.
The present results for 10s and 20s composites are in
agreement with the latter observation (particle size
effects were not investigated, since the composite
materials were obtained ready-made).

Al@, reinforced composite

Figure 11(a) represents the microstructure obtained
from 1OAL composite with DAS -13 pm. The
volume fraction of A1201 particles is approximately
0.12 f 0.02. The particle size varied between 4 and
60 pm with about 65% lying in the range 20-30 pm,
giving an average particle size of -23 pm and average
aspect ratio -2.3. A higher magnification micrograph,
Fig. 11(b), clearly shows the phenomenon of
mechanical entrapment of the A&O3 particles by the
aluminum dendrites for particle sizes much greater
than the DAS (marked A on the micrograph). Smaller
particles are pushed into the interdendritic regions
(marked B). When the DAS is larger than the particle
size, i.e. at a mold temperature -450°C most of the
A&O, particles are found segregated in the inter-
dendritic areas or lying on the cell boundaries, Fig.
1l(c).
The interparticle distance distributions for the
composite samples are shown in the histograms of Fig.
12(a)-(c). A normal bell-type random distribution is
the main characteristic feature when the mold
20i.Lm
temperature is -25”C, Fig. 12(a), with a peak around -__l_ J
25 pm. At 250°C mold temperature, lower sections
show more or less flat distributions, whereas upper
sections display a wider distribution pattern. An
exponential distribution is obtained when the mold
temperature is raised to 45o”C, Fig. 12(c), with
clustering observed at separations close to 15 pm.
The observed differences in the three cases may be
explained as follows. In the period between casting
and solidification, the denser reinforcement particles
are liable to undergo some settling in their molten
matrix surroundings, due to the effect of gravity. This
is expressed by the well known Stokes equation for
the terminal (or Stokes) velocity, UT, to which the
particles will accelerate, at which point sedimentation
and viscous drag forces will balance each other:

u-i-= (Apgd’)llSq Fig. 11. Microstructures of 1OAL composite samples

where Ap = density difference between the matrix and
particle; g = acceleration due to gravity; d = particle
diameter; and 17= dynamic viscosity of the fluid
surrounding the particle.
It has been reported that settling is hindered for
larger volume fractions of particles as well as for a
range of particle sizes. 25 The wide range of particle
size of the alumina reinforcement (4-60 pm) in the
present composite would explain the much more
obtained at different mold temperatures: (a) 25”C, low
magnification (note the wide variation in the alumina
particle size); (b) 25”C, high magnification (note the
presence of fine debris (circled) in the interdendritic region);
(c) 450°C.
random distribution observed in the case of the faster
cooled (mold temperature 25°C) samples of Fig. 12(a),
where there would be a much lesser time for settling
to occur, than in the slower cooled samples obtained
at the higher mold temperatures, Fig. 12(b) and (c).
 Particle distribution and porosity in 359 alloy composites 313

70 centrifugal casting technique, in conjunction with a

numerical process model, for 13 pm diameter A1203
60 particles in a commercial purity Al melt. Varying the
magnitude of the body (centrifugal) force and the
50
solidification rate alters the critical pushing velocity
2, that determines the transition from sedimentation-
2‘ dominated to particle-pushing-dominated redistribu-
g
3 30
tion. In the absence of body forces (i.e. for the case of
r
WI
gravity casting), this critical velocity was determined
20 to lie in the range of approximately l-5 mm/s.
Strictly speaking, while the present results and
IO previous results’” may not be compared, it is
nevertheless interesting to take note of the fact that
0
0 25 50 75 100 depending upon the conditions of solidification, the
A1203 Interparticle distance (Km) particle redistribution can be influenced by either
(a) sedimentation or particle-pushing. In other words,
after optimizing the particle distribution in the melt
using the proper stirring and melt conditions, further
mAL250-4
60
a AL250-3 control can be exercised during the solidification stage
AL2SO-2 to obtain distributions as desired.
AL250- 1 Figure 13 compares the frequency of interparticle
separations at -5 pm versus the DASs for the three
composites studied. It is interesting to note that for
dendrite arm spacings of -50 pm, nearly 50% of the
Sic particles are almost touching each other in the 20s
composite compared to about 35% in the case of 10s.
The difficulty of filling such narrow gaps contributes to
microporosity formation and explains the greater
amount of microporosity usually observed in the
former. The fractograph of Fig. 14 shows an example
A1203 Interparticle distance (pm) of this behaviour. The 1OAL composite, on the other
(b)
hand, shows an almost steady frequency level for all
707 DASs studied, the nature of the alumina reinforce-
ment (larger and more varied particle sizes)
tgAL450-4
60
0 AL450-3 contributing in part to the same.
nAL450-2
n AL450-1
CONCLUSIONS
The influence of solidification rate and metal
feedability on the particle distribution and porosity in

A1203 Interparticle distance (Fm)

(9
Fig. 12. A1203 interparticle distance distribution histograms
for 1OAL composite samples obtained at different mold
temperatures: (a) 25°C; (b) 250°C; (c) 450°C.

The exponential form of the distribution in the latter

case clearly points to the particle segregation taking
place under the corresponding conditions. DASMn)
A study has been made2’ of particle pushing during Fig. 13. Plots of frequency of interparticle distance at 5 pm
solidification in the Al-Al,O, ‘. _I svstem.
, --m--j using
------D a
-- versus DAS for the three composites.
314 A. M. Samuel, A. Gotmare, F. H. Samuel

tions support particle pushing as being the dominant

phenomenon during solidification.
4. In the 359/A&O,,,, composite, the interparticle
distance distribution profile changes from a normal
random distribution at lower DAS values to an
exponential type at larger ones, indicating the particle
segregation taking place. The observed distributions
may be attributed as resulting from the larger/wider
range of sizes of the alumina particles, that more often
lead to mechanical trapping rather than particle
pushing, particularly at lower DAS values.

ACKNOWLEDGEMENTS
The authors wish to thank Duralcan Canada, Usine
Dubuc, Chicoutimi, for providing the composite
Fig. 14. SEM fractograph of a 359/SiC(,, composite sample materials. Financial support received from the Natural
obtained from a tensile tested bar (with DAS -25 pm),
showing particle clustering. Note the absence of any matrix Sciences and Engineering Research Council of
component between the particles. Canada is gratefully acknowledged.

REFERENCES
359/SiC,,, and 359/Al,O,,,, composites was studied. Geiger, A. L. & Walker, J. A., JOM, August (1991)
Based on an analysis of the microstructural observa- 8-1.5.
tions, and the porosity and interparticle distance Lloyd, D. J., ht. Mater. Rev., 39 (1994) l-23.
distributions obtained, the following may be Allison, J. E. & Cole, G. S., JOM, January (1993)
19-24.
concluded. Hoover, W., Proc. 12th Riso Int. Symp., ed. N. Hansen
et al. Riso National Lab., Roskilde, Denmark, 1991, pp.
1. Microporosity in 359/SiC(,, composites derives in
387-92.
the main from pore nucleation taking place at the Sic 5. McCoy, J. W. & Wawner, F. E., Proc. Int. Conf. on Cast
particle sites, as well as from the hindered liquid metal Reinforced Metal Composites, ed. S. G. Fishman & A.
flow that results from particle clustering. The skewed K. Dhingra. ASM International, Materials Park, OH,
porosity distribution profiles observed in these 1988, pp. 237-242.
composites are similar to the type I distributions 6. Rana, F., Dhindaw, B. K. & Stefanescu, D. M., AFS
Trans., 97 (1989) 255-64.
observed in A356 alloy, attributed to pore nucleation. 7. Samuel, A. M. & Samuel, F. H., Met&. Trans. A, 24A
Macroporosity occurs due to interdendritic (1993) 1857-68.
shrinkage/gas evolution. The presence of the Sic 8. Samuel, A. M., Liu, H. & Samuel, F. H., /. Mater. Sci.,
particles invariably surrounding the pores indicates 28 (1993) 6785-98.
the restricting effect of these particles on pore growth. 9. Samuel, A. M.. Liu, H. & Samuel, F. H., Comp. Sci.
Techno/., 49 (1993) 1-12.
2. In the 359/Al,O,,,, composite, limited feedability 10. Labib, A., Liu, H. & Samuel, F. H., AFS Trans., 100
and the wider range of and larger particle size of the (1992) 1033-41.
alumina are responsible for the observed micro- 11. Samuel, A. M. & Samuel, F. H., J. Mater. Sci., 29 (1994)
porosity and the shift to a larger maximum pore size 3591-600.
range (loo-180 pm*), compared to that observed for 12. Gowri, S. & Samuel, F. H., Metalf. Trans. A, 23A (1992)
3369-76.
the Sic,,, composites (O-40 pm’). Although the 13. Samuel, F. H. & Samuel, A. M., Comp. Sci. Technol.,
resulting bell-shaped porosity profile partly corres- 53 (1995) 85-98.
ponds to the type II distribution observed in A356 14. Oswalt, K. J. & Misra, M. M., AFS Trans., 88 (1980)
alloy attributed to pore nucleation and growth, the 845-62.
observed features do not correspond as much to ‘pore 15. Samuel, A. M. & Samuel, F. H., AFS Trans., 100 (1992)
657-66.
growth’ as to the effect of the larger gaps and cavities 16. Kubo, K. & Pehlke, R. D., Metall. Trans. B, 16B (19%)
that occur on account of the larger particle size. 359-66.
3. Interparticle distance distributions for the 17. Campbell, J., Castings, Butterworth-Heinemann, Ox-
359/SiC,,, composites show that while finer DASs ford, 1991.
produce a more uniform distribution of the SIC 18. Huang, H. & Berry, J. T., AFS Trans., 101 (1993)
669-75.
particles, larger spacings lead to particle clustering, 19. Chiou, L. J. & Tsai, H. L., AFS Trans., 98 (1990)
usually at separations of -5 pm, the probability for 823-30.
clustering increasing with increase in Sic,,, content. 20. Tynelius, K., Major, J. F. & Apelian, D., AFS Trans.,
These distributions and the microstructural observa- 101 (1993) 401-13.
 Particle distribution and porosity in 359 alloy composites 315

21. Mohanty, P. S., Samuel, F. H. & Gruzleski, J. E., Proc.
Conf Int. Symp. on Light Metals Processing and
Applications. Canadian Institute of Mining, Metallurgy
and Petroleum, Montreal, 1993, pp. 273-82.
22. Mortensen, A. & Jin, I., Int. Mater. Rev., 37 (1992)
101-28.
23. Rohatgi, P. K., Yarandi, F. M., Liu, Y. & Asthana, R.,
Mater. Sci. Eng., Al47 (1991) Ll-L6.
24. Lloyd, D. J., Proc. 12th Riso lnt. Symp., ed. N. Hansen
et al. Riso National Lab., Roskilde, Denmark, 1991, pp.
81-99.
25. Richardson, J. F. & Zaki, W. N., Chem. Eng. Sci., 3
(1954) 65.
26. Kennedy, A. R. & Clyne, T. W., Cast Metals, 4 (1991)
160-4.