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ELSEVIER
THERMAL
S. Elomari,a
aSpacecraft Engineering,
M. D. Skibo,b A. Sundarrajan
Department
of Materials
& H. Richards
Incorporated,
Saint-Hubert,
J3 Y 8Y9, Canada
Abstract
nature, volume fraction and morphology of the reinforcement in the composite, many applications of aluminummatrix composites require controlled thermal-expansion
characteristics in order to match those of other components. A low CTE and high thermal conductivity are
desirable for applications such as electronic heat sinks
and space structures. Furthermore, a low density is
desirable for aerospace applications, particularly electrical structural applications. Conventional metals for
electronic packaging applications include copper, aluminum, Ni-Fe alloys, and Cu-W and Cu-MO blends;
however, these materials do not meet the requirements
in advanced electronic packaging applications for low
CTE, high thermal conductivity, low density and low
cost.
With these considerations in mind, Sic-particle-reinforced aluminum-matrix composites are receiving the
most attention as potential candidates for a variety of
uses in advanced electronic packaging. As shown in
Table 1, the Sic particles, which are available in different structures from inexpensive raw material sources,
exhibit low density, low CTE, high Youngs modulus,
and are commercially available in a particle size range
from 1 to 80 pm. The thermal conductivity, K, of Sic is
in the range 80 to 200 W m-l K-, depending on purity
and processing conditions.
Aluminum alloys reinforced with Sic particles offer
many distinct advantages over conventional materials
used for electronic packaging because of the following
considerations:
Aluminum-matrix
composites containing thermally oxidized Sic particles of controlled diameter ranging from 3
to 40pm have been produced successfully by vacuumassisted high-pressure infiltration. Their thermal-expansion coefficients (CTEs) were measured between 25 and
500 C with a high-precision thermal mechanical analyser
(TMA),
and compared with the predictions of various
theoretical models. The thermal-expansion
behavior of
the three-phase Al/SiC/SiOz
composite shows no signtficant deviation from the predictions of elastic analysis,
since the measured CTEs lie within the elastic bounds
derived by Schaperys analysis. The effect of particle size
is quite evident in the pressure-infiltrated
composites: the
larger the particles, the greater the thermal expansion of
the composite. The observed behavior of these composites
is discussed in terms of particle size, silica layer formed
during oxidation, and thermal stresses developed as a
result of the CTE mismatch between the reinforcement
and the matrix. 0 1998 Published by Elsevier Science
Ltd. All rights reserved
Keywords:
A. metal-matrix composites, B. thermal
properties, E. casting, SIC particles, oxidation
1 INTRODUCTION
Metal-matrix composites (MM&) has been identified as
attractive materials for a wide range of applications in
structural design, mechanical systems and electronic
packaging. Aluminum alloys reinforced with various
ceramics such as Sic and A1203 are a unique class of
advanced composite materials developed for use in
aerospace and commercial applications. Compared with
unreinforced
metals,
MMCs
exhibit
significant
improvements in strength and elastic modulus,-3 wear
resistance,4 fatigue resistance5 and damping capacity,6
in addition to high-temperature mechanical properties7
and low thermal expansion.*
Since the coefficients of thermal expansion (CTEs) of
metal-matrix composites can be tailored by varying the
S. Elomari
370
SIC
Al
Density
&cm-?
Elastic
moc$l;ls
a
3.2
2.1
450
70
CTE
(XlO~6C)
~.
4.1
23
Thermal
conductivity
(W m-i K-)
8&200
180-230
2 EXPERIMENTAL
et al.
2.2 Metal-matrix composites production by bighpressure infiltration
The high-pressure
vacuum-assisted
infiltration
technique is a method for fabricating
metal-matrix
composites, where the application
of a high pressure forces
molten metal into a porous preform made of a particulate reinforcement.
The thickness of the preform used in
this study was 30mm. The procedure of preform fabrication can be outlined as follows. First, SIC particles
were packed by hand into a boat made of Fiberfraxa
board. Stirring by an impeller was performed to establish a uniform particle distribution.
Finally, oxidation of
the particles in air under programmed
heating and isothermal conditions
was carried out at 1300C. The
temperature
in the hot zone was kept constant to within
* 1C. As the preforms used in this study were fabricated with different particle sizes, the oxidation
time
ranged from 120 to 240 min.
The matrix was 99.9% initial purity aluminum
from
ALCOA@ (Trademark,
Aluminum
Company of America, Pittsburgh,
Pennsylvania).
The composites
were
fabricated by vacuum infiltration
of a liquid metal into
a porous preform under high pressure. Preforms were
infiltrated
with pure aluminum
by using the squeezecasting press shown in Fig. 1. The apparatus consists of
a steel die containing
a cylinder in which a steel piston
travels. The piston is centered above the cylinder with a
steel ring. The interior of the cylinder was lined with a
tube of graphite foil and Fiberfraxa
insulation. Pressure
is provided by an RC-1010 ENERPAC
hydraulic ram.
A vacuum line at the bottom of the die permits application of a vacuum during infiltration.
The preform and the aluminum
were heated separately to 800C. The procedure consisted of dropping the
PROCEDURES
Upper platen
King centring
Piston
Die
f-t-t
Fiberfrax
Preform
c
Tl
Vacuum
Pump
Fig. 2. Oxidation
behavior
@I
Time (min)
of particulate
SiC
371
(LVDT) attached to the probe. The furnace, surrounding the sample stage and probe, provides heating/cooling during the measurement. A thermocouple adjacent
to the sample monitors sample temperature so that the
dimensional change can be followed as a function of
temperature. The data were obtained in the form of
PLC (per cent linear change) versus temperature curves.
Standard TMA data analysis software was used to
evaluate the coefficient of thermal expansion of the
composites tested. The CTE is determined at intervals
of 50C on the basis of the calculated slope fit between
two selected temperatures on the PLC versus temperature curve.
3 RESULTS
3.1 Characterization of oxidized Sic particles
Oxidation data in air for the silicon carbide particles are
shown in Fig. 2(a), and (b) illustrates the variation in
thickness of the silica layer, as determined by SEM
analysis, with particle size. In each case the per cent
mass gain of 100mg samples at 1300C is plotted as a
function of time. The results indicate that the weight
gain curves for these materials obeyed parabolic kinetics, as expected for a process whose rate is controlled by
diffusion through a growing oxide layer.O However, the
oxidation proceeds at a very high rate for smaller particles (3-10 pm) after a short exposure to air at 1300C.
The SEM micrograph of the oxidized Sic particles
[Fig. 3(b)], as compared with that of unoxidized particles [Fig. 3(a)], shows that the Sic particles have been
cemented together by the viscous silica glass formed by
the oxidation reaction. The large reinforcements (2040 pm) exhibited less coalescence than the other materials. In contrast, some fusion of the smaller particles
(3 pm) was observed and SiOZ droplets could be identified on many of the particles surfaces after the oxidation at 1300C. The particulate silicon carbide showed
extensive coarsening following this oxidation exposure
and clear evidence of bonding of the particles by the
glassy silica phase. After oxidation at 1300C. even for
(b)
in air at 1300C: (a) mass gain versus time for various particle
SiOz layer as a function of particle size.
of
S. Elomari et al.
372
Fig. 3. Appearance of 40 pm SIC particles: (a) as-received condition, (b) after oxidation treatment
periods of 2 h, the small particles of 3 pm size were
found to have fused into a bonded network as a result
of the flow of the silica glass from particle to particle.
3.2 Composite characterization
Figure 4 shows SEM micrographs
of polished sections
of the Sic/Al composites.
Pressure infiltration
of the
oxidized preforms produced composites in which most
of the material appeared
to be free of porosity and
macroscopically
homogeneous;
thus these composites
are expected to have isotropic properties. There was no
sign of interfacial
reaction between the reinforcement
and the matrix. Differential scanning calorimetry (DSC)
combined with EDAX in the SEM revealed no second
phases either in the matrix or near the matrix/reinforcement interfaces. The volume fraction of silicon carbide in the composites
was determined
via image
analysis to be in the range 0.54 to 0.56. The experimental uncertainty
of these measurements
is estimated
to be about 2%, hence the volume fraction is essentially
constant within the experimental
error at 0.55.
3.3 Thermal expansion
The thermal
expansion
results,
as a function
of
temperature,
for the different composites
containing
Fig. 4. Microstructures
oxidized SIC particles are shown in Fig. 5, which represents the average of four tests. In general, the thermal
cycling experiments produced no conclusive evidence of
thermal ratcheting
in any of the materials during two
cycles. Upon subsequent
heat-up, in cycle 2, the SiCparticle-reinforced
aluminum
composite
shows very
similar behavior to that in cycle 1; the only difference is
a more gradual increase in CTE at high temperature.
This feature has its origin in the thermal
stresses
induced in the matrix because of the difference between
the CTEs of the matrix and reinforcing ceramic particles.
As shown in Fig. 5, the effect of particle size is quite evident in the case of the composite reinforced with oxidized reinforcement.
The larger the particles, the greater
is the thermal expansion at a particular temperature.
Figure 6 shows the coefficient of thermal expansion
values as a function
of temperature
for each of the
composites tested. As expected from Fig. 5, the composite reinforced with larger oxidized particles shows consistently higher CTE than the composite
containing
smaller oxidized particles. It is evident that the CTE is
decreased by the oxidation process which is consistent
with the thermogravimetric
analysis shown in Fig. 2; the
smaller the particle size, the greater the degree of oxidation of the ceramic particles.
of infiltrated Sic/Al metal-matrix composites: (a) oxidized 40 pm SIC particles, (b) oxidized 3 Frn SIC particles.
0.7 -.
!i
,articlelrize : 3 um
j.................
0.6 _...............
.......
100
(a)
"0
100
Id
Fig. 5. Per
200
300
Temperature
200
300
Temperature
0.8
:
.._ ._....)
......_
400
(C)
400
CC)
0.7 _
d.cd_.
,3........
f!F$!!!;
j
.;.._............ 0.6 _.._......-...............
300
500
600
100
600
;
..____.____
+
i ............__..
___.._.._..
406
500
600
Temperature (C)
500
200
373
0
(d)
100
200
300
400
500
600
Temperature CC)
cent linear change (PLC) versus temperature for composites reinforced with oxidized SIC particles of various sizes: (a)
3 urn, (b) 10 urn, (c) 20 urn, (d) 40 urn.
4 DISCUSSION
4.1 Theoretical models
The CTE of a metal-matrix
composite is relatively difficult to predict precisely because it is influenced by several factors including matrix plasticity and the internal
structure of the composite,
which typically consists of
particles or fibers embedded
in a continuous
metallic
matrix.
RI3 pmEil0
pmm20 pm040
pm
The composites
used in this work are random and
isotropic. Despite the presence of a two-layer structure
for the oxidized particles, SiOZ and Sic, we assume that
both the matrix and the reinforcement
phases are linearly elastic over a small range of volumetric strains and
can be treated individually
as homogeneous
phases. In
the theoretical models to be described, it is assumed that
the interfacial shear strength at the interface is adequate
to avoid interface failure.
Several theoretical
analyses have been presented
in
the literature giving expressions for the CTE of metalmatrix composites; these are reviewed inm3. Of these,
the simplest and most often used are those of Kerner,
Schapery and Turner.
4.1.1 Kerners model
The Kerner model assumes that the reinforcement
is
spherical and wetted by a uniform layer of matrix; thus
the CTE of the composite is stated to be identical to
that of a volume element composed of a spherical reinforcement particle surrounded
by a shell of matrix, both
phases having the volume fractions present in the composite. This model gives the composite CTE as:
Temperature
Fig. 6.
(C)
(1)
374
S. Elomari et al.
Ly, = (Yp +
(a, - up)
(l/Kc) - (l/K,)
(l/Km) - (l/K,)
(3)
tic-=K,,,+
--!-+
K,-K,
VP
vm
(4)
K,,,+:G,n
(5)
(6)
315
T (Cl
50
100
200
300
400
500
450
450
450
450
450
450
192
192
192
192
192
192
227
227
227
227
227
227
SiOz
4.5
4.5
4.5
4.5
4.5
4.5
70.5
71.3
72.3
13.4
74.2
75.2
30.7
31.1
31.6
32.1
32.5
33.5
6'
0
100
(a)
Pa~icleste:3um
400
200
300
Tempersture ("C)
Pure aluminum
33.4
33.5
33.6
34.2
34.4
34.6
0.41
0.47
0.55
0.58
0.61
0.62
72.03
70.66
65.90
63.73
49.16
36.91
27.2
26.6
24.7
24.1
18.1
13.2
68.28
68.55
66.21
59.79
60.96
60.48
500
,
600
6'
0
"
"
100
@)
"
200
300
400
Temperature ("C)
500
1
600
500
600
18
~16
,6
h 14
P
14
El,
12
c
0 10
10
"0
loo
(c)
Fig. 7. Comparison
200
300
400
Temperature CC)
500
21.8
22.4
23.9
25.9
27.8
29.5
800
"0
(d)
loo
300
400
200
Tempenlture ("C)
of the measured CTEs of infiltrated SIC/Al composites with the theoretical predictions.
376
S. Elomari et al
the CTE of the composites will vary with the reinforcement size. It is not surprising that very small particles,
with their larger surface area, have a greater effect than
large particles-as
our own observations
demonstrate.
The measured
CTE shows, for each composite
type,
similar variations
with temperature,
but with a slight
decrease in the CTE value by about lop6 C as the
Sic particle size decreases from 40 to 3 urn. This effect
of particle size is, as shown in Fig. 5, relatively well
predicted
by mechanical
models using a three-phase
composite system.
Recently, Ma et af.18 examined the effect of reinforcement size on the CTE of Sic/Al metal-matrix
composites in which the SIC particle sizes were 3.5, 10 and
20 urn. They reported no significant effect of particle size
on the thermal behavior of the composites
produced
with SIC particles
having
undergone
no oxidation
treatment prior to the infiltration
process. These earlier
observations
and our own results demonstrate
that the
silica layer produced
by the oxidation
treatment
is
responsible
for the variation
in measured
CTE with
particle size.
The agreement of the high-temperature
CTE with the
prediction of the Kerner model is not in agreement with
published
CTE values for highly loaded SiC-particlereinforced
aluminum
composites,
which have been
found to agree with the Turner model above 40~01%
SiC.19 However, for 53~01% Sic/Al composites
produced by pressure infiltration,
Balch et a1.15 reported
that the measured low-temperature
CTE agreed fairly
well with that predicted by the Turner model, while the
CTE in the high-temperature
(175-325C) region was in
good agreement with Kerners prediction.
The authors
interpreted
these observations
as being an effect of residual stresses and void volume change in the thermally
cycled composites.
5 CONCLUSIONS
Several
work:
important
conclusions
can be drawn
from this
Vacuum-assisted
high-pressure
infiltration
produced composites
in which most of the material
appeared to be free of porosity and of high quality.
The thermal-expansion
coefficients
of pressureinfiltrated metal-matrix
composites
he within the
elastic bounds derived by Schaperys analysis.
Oxidized SIC particles in the amount of 56~01%
decreased
the
CTE
of
aluminum
from
25.2x 10-6C~
to 12x 10~6C-.
The experimental CTEs agree well with the values predicted
by the Schapery model at low temperatures
(5&
lYYC), while the CTEs in the temperature
range
from 400 to 500C are far from Kerners predictions.
ACKNOWLEDGEMENTS
The authors are grateful to Professors
Mortensen
(MIT) for the squeeze-casting
in this work.
Also,
Director
Spacecraft
of
Space Agency,
we would
like to thank
Engineering
for assistance
at
and stimulating
Flemings
facilities
and
used
Dr Vukovich,
the
Canadian
suggestions.
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