JournalofMetallurgicalEngineering(ME)Volume5,2016 www.mejournal.

org
doi:10.14355/me.2016.05.001

EffectsofBimodalandMonomodalSiC
ParticleontheThermalPropertiesof
SiCParticleDispersedAlMatrixComposite
FabricatedbySPS
KiyoshiMIZUUCHI1,**,KanryuINOUE2,YasuyukiAGARI1,MotohiroTANAKA1,TakashiTAKEUCHI1,
JunichiTANI1,MasakazuKAWAHARA3,YukioMAKINO4andMikioITO5
OsakaMunicipalTechnicalResearchInstitute,1650,Morinomiya,Jotoku,Osaka,5368553Japan

MaterialsScience&Engineering,UniversityofWashington,302RobertsHall,Box352120,Seattle,WA981952120,
USA.
2

KawaharaSPSTechnicalOffice,2425,Ohyabe,Yokosuka,2380024,Japan

ForumMACKIY,NorthBldg.,S04,KyotoUniversityKatsuraVenturePlaza,KatsuraInnovationPark,136,
GoryouOhara,Nishikyouku,Kyoto6128245,Japan.
4

CenterforAtomicandMolecularTechnologies,GraduateSchoolofEngineering,OsakaUniversity,21,
Yamadaoka,Suita,5650871,Japan
5

**Correspondingauthor.Tel:+81669638153;fax:+81669638145.
Emailaddress:mizuuchi@omtri.or.jp(K.Mizuuchi)

Abstract
Siliconcarbide(SiC)particledispersedaluminum(Al)matrixcompositeswerefabricatedincontinuoussolidliquidcoexistent
statebysparkplasmasintering(SPS)processfromthemixtureofSiCpowders,AlpowdersandAl5mass%Sialloypowders.As
theSiCpowders,twokindsofpowders,monomodalSiCpowdersof109.8mindiameterandabimodalSiCpowdermixture
of 109.8m and 14.3m in diameter, were used. The microstructures and thermal conductivities of the composites fabricated
were examined. These composites were all well consolidated by heating at a temperature range between 798K and 876K for
1.56ksduringSPSprocess.NoreactionattheinterfacebetweentheSiCparticleandtheAlmatrixwasobservedbyscanning
electron microscopy for the composites fabricated under the sintering conditions employed in the present study. The relative
packingdensityofthemonomodalcompositedecreasedfrom99.8%to95.1%withincreasingSiCvolumefractioninarangeof
55%and65%,whereasthatofthebimodalcompositewas97%orhigherthanthatinaSiCvolumefractionrangeupto70%.The
thermal conductivity of the bimodal composite was higher than that of the monomodal composite in a SiC volume fraction
range higher than 55%. The coefficient of thermal expansion of the composites falls in the upper line of Kerners model,
indicatingstrongbondingbetweentheSiCparticleandtheAlmatrixinthecomposite.
Keywords
MetalMatrixComposites;ParticleReinforcement;ThermalProperties;Sintering;SiliconCarbide

Introduction
Highperformancethermalmanagementmaterialsshouldhavehighthermalconductivities1,2)andlowcoefficients
ofthermalexpansion(CTEs)formaximizingheatdissipation3)andminimizingthermalstressanddistortion,which
arecriticalissuesinpackagingofmicroprocessors,powersemiconductors,highpowerlaserdiodes,lightemitting
diodes(LEDs),andmicroelectromechanicalsystems(MEMS)39).TraditionalpackagingbasematerialsareCuW10),
AlN11), BeO12) and Al/SiC1315). Among these materials, particularly, Almatrix composites containing dispersed
silicon carbide (SiC) particles have received the most attention as potential candidates for a variety of uses in
advancedelectronicpackaging.TheyarecurrentlycompetingwithestablishedmaterialssuchasCuWorCuMo
intheelectronicpackagingindustry16).

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High thermal conductive composites consisting of Al matrix and SiC particles have been reported by Chu et. al,
who fabricated a SiCparticledispersed Almatrix composite by a metal infiltration technique and obtained a
thermal conductivity of 163~186 W/mK for Al composites containing 50~65 vol.% SiC13,14). Almatrix composites
containing SiC particles are to date mainly fabricated by liquid metal infiltration into SiC preforms13, 14). This
process often uses Al alloys with Si and/or Mg additions to avoid the formation of interfacial products such as
Al4C3, leading to a detrimental effect on the thermomechanical properties of the composites. When Si and Mg
dissolve into the Al matrix, on the other hand, the thermal conductivity of the matrix decreases and lowers the
thermalconductivityofthecomposites.Inaddition,itisdifficulttomakeSiCparticlesdispersedhomogeneously
in the Al composite when it is fabricated by a metal infiltration technique. This is especially true when the
composite contains a lower volume fraction of SiC, say less than 50 vol. %, because of the difference in packing
densitybetweenSiCandAl.
Sparkplasmasintering(SPS)1725)appliedasanewmethodforpreparinghighperformanceofAlmatrixcomposites
containing SiC has been presented recently15). The main advantage of the SPS process is to fabricate various
materialsforrelativelyshortsinteringtimesatlowtemperatures,leadingtothepreventionofAl4C3attheinterface
between Al and SiC. Chu et. al fabricated SiCparticledispersed Almatrix composites by SPS and obtained a
thermal conductivity of 224 W/mK for an Al55 vol.% SiC composite15). However, pores always appear in their
study as an unavoidable structure in the Almatrix composites containing SiC fabricated in solid state by SPS,
whichleadstoinsufficientwettingbetweenAlandSiC.ThisresultsinweakAl/SiCinterfaces,especially,athigh
volume fractions ofSiC particles. Poresconsiderablymake the thermal conductivity of the Almatrix composites
decreaseduetoscatteringoftheheatflow26).
To fabricate highperformance thermal management materials with ultrahigh thermal conductivities and low
CTEs, we have recently initiated a series of investigations, where diamondparticledispersed metalmatrix
composites2731)werefabricatedbysparkplasmasintering(SPS)process1725,2734).
In our previous work, SiCparticledispersed Almatrix composites were fabricated in continuous solidliquid
coexistentstatebySPSprocess,andthecompositeswereshowntohavehighrelativepackingdensitiesandgood
bondingbetweentheAlmatrixandtheSiCparticles.Itwasshownthatthethermalconductivitywas252W/mKat
aSiCvolumefractionof50vol.%32,33).Itshouldbementionedthat,however,thethermalconductivityofAlmatrix
compositecontainingmonomodalSiCparticlesdecreaseswithincreasingvolumefractionofSiCparticleswhenit
ishigherthan50vol.%.Thisdecreaseofthermalconductivityismainlycausedbydrasticdeclinesoftherelative
packingdensityofthecompositeinaSiCfractionrangehigherthan50vol.%.
In order to make Almatrix composites having both high thermal conductivity and low CTEs in a SiC fraction
range higher than 50 vol.%, in the present work, composites containing bimodal SiC particles (hereafter called
bimodalcomposites)werefabricatedalongwiththosecompositescontainingmonomodalSiCparticles(hereafter
called monomodal composites). In the present fabrication, a continuous solidliquid coexistent state2933) was
created during SPS process. Process temperatures employed were lower than the melting point of Al and SPS
processparameterswereoptimized.Experimentalresultsofthermalpropertiesobtainedfromthemonomodaland
bimodal Almatrix composites are reported in the present study along with microstructures of the composites
fabricated under various process parameters. The packing density, the thermal conductivity and the CTEs of the
composites are measured, and the bimodal and monomodal SiC particle effect on the thermal property of the
compositesisevaluated.
Experimental Procedure
According to threedimensional Euclidean space, the maximum volume fraction of SiC particles in Almatrix
composite can ideally be 74 vol.% if SiC particles are spherical and of uniform size. Due to some experimental
constraints,Almatrixcompositesarecommonlyproducedwitharound50vol.%ofSiCwhenroughlymonosized
SiCparticlesareused.Inthepresentstudy,twosizesofSiCpowders(i.e.,GMF60FH2SiCswithameanparticle
diameter of 109.8m and GMF800H2 SiCs with a mean particle diameter of 14.3m, Pacific Rundum Co., Ltd.)
were employed as a filler material. As a matrix material, two kinds of metallic powders, Mitsuwa 99.9% purity
purealuminum(Al)powder(150mesh)andHikariMaterialAl5mass%Sialloypowder(70m),wereemployed.

JournalofMetallurgicalEngineering(ME)Volume5,2016 www.mejournal.org

Scanning electron micrographs of large SiC, small SiC, pureAl and Al5mass%Si powders used in the present
studyisshowninFig.1.Asseen,theshapesoflargeSiC,smallSiC,pureAlandAl5mass%Sipowderprovidedby
the abovementioned manufacturers are flat octahedronlike for SiC, teardroplike for pureAl and spherical for
Al5mass%Sipowder,respectively.
(a)

(b)

(c)

(d)

FIG.1SEMMICROGRAPHSOFASRECEIVED(A)SIC(109.8M),(B)SIC(14.3M),(C)PUREALAND(D)AL5MASS%SIPOWDERS,
SHOWINGTHEMORPHOLOGYOFTHEPOWDERSUSEDINTHESTUDY.

AlSialloypowderisimportanttouseinthepresentstudyforcreatingasolidliquidcoexistentstateduringSPS
processing. We have developed unique SPS fabrication techniques to make metalmatrix composites with or
without dispersed SiC particles. The uniqueness is that during SPS process at a low pressure, continuous
solidliquid coexistent state of the metal powder mixtures was created by thenature ofAlSi alloy. It should be
pointed out that because of a low thermal conductivity (150 W/mK) of Al5mass%Si alloy powder16) and also
because of necessity of avoiding drastic decrease in the thermal conductivity of Al matrix, an Albased powder
mixturecomposedof90vol.%ofpureAlpowderand10vol.%ofAl5mass%Sialloypowderwaschoseninthe
presentstudyasthematrixmaterial.
ThemixingratiooflargeandsmallSiCparticlesisimportantinbimodalSiCparticlemixturetoachievethehigh
packingdensityofAlmatrixcompositescontainingSiCparticles.Inthepresentstudy,theoptimummixingratio
was determined as follows. When one puts a bimodal powder mixture into a container and tap the mixture, its
porositycanbeevaluatedusingFurnasmodel35),whichisdescribedhere.Assuming(a)largeparticlesaremuch
largerindiameterthansmallparticles,(b)themassdensityoflargeparticlesisequaltothatofsmallparticles,and
(c) small particles fill up the gaps between large particles, the porosityof the bimodal powder mixture can be
calculatedinthefollowingequation(1)

1 1
(1)
v1

where 1 is the porosity when large particles are tapped into a container and v1 the volume fraction of large

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particles in a bimodal powder mixture composedoflarge andsmall particles.Alsoassuming(d)larger particles

areintermingleswithsmallones,theporosityofthebimodalpowdermixturecanbecalculatedinthefollowing
equation(2)

1 2
(2)
1 v1 2

where2 istheporositywhensmallparticlesaretappedintoacontainer.
In Furnas model35) every v1 value is proposed to choose a larger value of porosity between ones calculated in
equation (1) and in equation (2). In the present study, experimentally obtained porosities 1 and 2 values were
43.29%and56.63%,respectively,afterahundredtimesoftappingofeachpowdermixture.Usingthese1and2
values, the porosity () of a bimodal SiC powder was calculated and the result obtained is shown in Fig. 2 as a
function of v1. As seen, when the volume fraction of largeSiC particles in the bimodalSiC powder is75.1%, the
porosity of the bimodal SiC powder becomes minimum and it is 24.5%. From this result, in the present study, a
bimodal SiCpowder mixture composed of 75.1 vol.% of large SiC particles and 24.9 vol.% of smallSiC particles
was used to try to obtain the high relative packing density of Almatrix composites containing SiC. Relative
packingdensityisdefinedtobetheratioofthedensityofamaterialmeasuredexperimentallytothedensityofthe
materialassumedtohavenoporosity.
60
56.6%
50
43.3%

Porosity, (%)

40

30
24.5%
20
75.1%
10

0
0

20

40

60

80

Volume fraction of large SiC particle. v1 (%)

100

FIG2CHANGEINTHEPOROSITYOFTHESICPOWDERMIXTURECOMPOSEDOFLARGEPARTICLES(109.8MINDIAMETER)AND
SMALLPARTICLES(14.3MINDIAMETER)ASAFUNCTIONOFTHEVOLUMEFRACTIONOFLARGESICPARTICLESINTHESIC
POWDERMIXTURE.

Powder mixtures composed of four kinds of powders (large SiC, small SiC, Al and Al5mass%Si alloy powders)
were prepared as starting materials, and these powder mixtures with various volume fractions of SiC were
processedtofabricateAlmatrixcompositesusinganSPSequipment,FujiElectricIndustrialDr.Sinter1020.The
equipment consists of an electric power source and a pressure system, and the fabrication of composites was
carried out after powder mixtures were placed in a dieset made of Co/WC composite. A side view of our
custommadecylindricalCo/WcompositediesetusedinthepresentstudyisdepictedschematicallyinFig.3.
Formakingonediskshapedcompositespecimenwithgaugedimensionsof2mmthickand10mmindiameter,
about0.5gofthepowdermixtureofSiC,AlandAlSialloywaspreparedandsuchapowermixturewasplaced
carefullyintheabovedescribedcustommadedieset,andconsolidationwascarriedout.Thegaugedimensionsof
theCo/WCcompositedieusedinthepresentstudyare35mminoutsidediameter,10mmininsidediameterand
40mmhigh.DuringSPSprocessing,thedietemperaturewasmeasuredbyathermocouplethatwasplacedina
position5mmdistantfromtheinsideofthediewhereathermocoupleholewascreatedontheoutsidesurfaceof

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thedie.Theholewas2mmindiameterand7.5mmdeep.
Pressure
WC/Co punch

Pulsed current

WC/Codie

WC/Codie

Large
SiC SiC
-Si
particle
Al alloy
particle

K-Type

Al particle
Small SiC
particle

thermocouple

WC/Co punch
Pressure

-SiC
SiC particle
dispersed
Al matrix
composite

K-Type
thermo couple

FIG.3PROCESSINGOFSICPARTICLEDISPERSEDALMATRIXCOMPOSITEBYSPARKPLASMASINTERING.
PARTICLE,

:SMALLSICPARTICLE,

:ALPARTICLE,

:LARGESIC

:ALALLOYPARTICLE.

TheSPSprocessemployedisdescribedindetailasfollows.First,thelowerpunchwasinsertedintothediefromits
oneend,followedbypouringof0.5gofthepowdermixturecontainingSiCparticles.Then,theupperpunchwas
placedontothepowdermixture.Thepowdermixturewaspressedatapressureof80MPathroughtheupperand
lowerpunches,andthensparkplasmasinteringwasperformedafterevacuationtoavacuumof2Pa.Sinteringwas
thencarriedoutataheatingrateof0.83K/sinatemperaturerangebetweenR.T.and798K.Afterreaching798K,
furthersinteringwascarriedoutatalowheatingrateof0.05K/sinatemperaturerangebetween798Kand876K.
Whenthetemperaturereached876K,pulsedcurrentwasshutoffandthepressurewasimmediatelyincreasedto
300MPa.Whenthepressurereached300MPa,themixedpowderwaskeptfor0.18ksat876Kandthenfurnace
cooled. To visualize changes in the relative packing density of the Al/SiC composite during the SPS process,
longitudinaldisplacementsbetweenthepunchesweremonitoredasafunctionoftimeanddietemperature.The
dischargedpulsedcurrentusedwasabout240Aandsparkingwasgeneratedataconstantseparationoftimeof
approximately2.78103s.
DiskshapedcompositesthusfabricatedwereexaminedbyscanningelectronmicroscopyusingaJEOLJSM6460
LA microscope. Almatrix composite disks containing SiC were goldcoated and their thermal diffusivities were
measured by a laser flash technique using a Netzsch LFA457 thermal constants analyzer. The achieved packing
densityofthediskswasmeasuredinArchimedesmethodforoptimizingprocessparametersandforcalculationof
thermal conductivities. Coefficients of the thermal expansion (CTEs) of the composite were investigated on

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columnshapedspecimens,5mmindiameterand15mmlong,fabricatedfromthepowdermixtureofSiC,Aland
Al5mass%Si alloy by SPS under a similar processing condition mentioned above. The thermal expansion of the
compositewasmeasuredwithaRigakuTMA8310dilatometerinaN2flowingatmospherewithaheatingratioof3
K/mininatemperaturerangebetween243and483K.TheCTEsatroomtemperatureweredeterminedfromthe
slopeofthethermalexpansionagainsttemperaturecurveinatemperaturerangebetween288and298K.
Results and Discussion
RelativePackingDensityofCompositesFabricatedbySPS
The relative packing density of the SiCparticledispersed Almatrix composites fabricated was measured by
Archimedes method. Figure 4 shows the measured values as a function of SiC volume fractions. The relative
packingdensityofthemonomodalcompositewashigherthan99%inarangeofSiCvolumefractionbetween40%
and 55%. However, in a range of SiC volume fraction higher than 55%, the relative packing density of the
compositedrasticallydecreaseswithincreasingvolumefractionofSiC.TherelativepackingdensityofAl60vol.%
andAl65%SiCcompositedecreasedto98.9%and95.1%,respectively.Ontheotherhand,thebimodalcomposite
maintainedtherelativepackingdensityhigherthan98%inarangeofSiCvolumefractionupto65%.Thepresent
result evidently indicates that the consolidation of the composite containing the bimodal SiC particles is very
effectiveinfillingupporespresentinmetalmatriccompositecontainingSiCparticles.Inaddition,itissuggested
thatthemixingratiooflargeSiCparticlestosmallonesestimatedbyFurnasmodelisappropriateforthedecrease
oftheporosityintheSiCpowdermixtureusedinthepresentstudy.

Relative packing debsity, Dr (%)

100

99

98

97
Monomodal

96

Bimodal

95
40

50

60

Volume fraction of SiC, Vf (%)

70

FIG.4CHANGESINRELATIVEPACKINGDENSITYOFSICPARTICLEDISPERSEDALMATRIXCOMPOSITEFABRICATEDBYSPARK
PLASMASINTERINGASAFUNCTIONOFTHEVOLUMEFRACTIONOFSICINTHECOMPOSITE.

Microstructure
The mixtures of powders composed of pure Al, Al5 mass%Si alloy and SiC were compacted, consolidated and
sintered in order to fabricate SiCparticledispersed Almatrix composites by SPS process. The microstructure of
assintered monomodal and bimodal composites containing 65 vol.% SiC was investigated by scanning electron
microscopy.Figure5isscanningelectronmicrographstakenfromcrosssectionsofSiCAlcompositesconsolidated
insolidliquidcoexistentstatebySPS.AsseeninFig.5(a)and(c),therearesomecavitiesininterfacialboundaries
betweentheSiCparticleandtheAlmatrixinthemonomodalcomposite.Inaddition,somedirectcontactsbetween
largeSiCParticlesinthecompositeareobserved.Ontheotherhand,cavitiesontheinterfacialboundariesbetween
theSiCparticleandtheAlmatrixofthebimodalcompositeconsiderablydecreasesandthedirectcontactsbetween
largeSiCparticlesbecomenegligibleasshowninFig.5(b)and(d).Itshouldbeemphasizedthatthedecreaseof

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cavities and the SiC direct contacts in the latter composite is due probably to the effective filling up of gaps
betweenlargeSiCparticlesbysmallSiCparticles.
Monomodal

(a)

(b)

(c)

(d)

Bimodal

FIG5SEMMICROGRAPHSOFAL65VOL.%SICCOMPOSITESFABRICATEDBYSPARKPLASMASINTERING(SPS).(A)AND(C)FOR
MONOMODAL;AND(B)AND(D)FORBIMODAL.

The formation of Al4C3 phase was reported by Chu et al 13, 14) to occur on interfaces between SiC particle and
pureAlmatrixinAlSiCcompositeswhenfabricatedbymetalinfiltration.Inthepresentstudy,however,nosuch
aluminumcarbidesweredetectedbyscanningelectronmicroscopeobservation,asshowninFig.5(b)and(d).To
clarifywhetherornotAl4C3isformedonsuchinterfacesinthecompositefabricatedinthepresentstudy,further
detailed microstructural investigation is underway by scanning transmission electron microscopy (STEM) with
EDXanalysis.Theresultswillbesoonpresentedelsewhere.
ThermalConductivity
ThermalconductivitiesweremeasuredforSiCparticledispersedAlmatrixcompositesfabricatedbySPSprocess
andtheresultsobtainedwereplottedinFig.6asafunctionofthevolumefractionofSiCparticles. Asseen,at40,
45and50vol.%ofthevolumefractionofSiC,thethermalconductivityofthemonomodalcompositewas239,245
and252W/mK,respectively.Thethermalconductivityofthecompositeincreasedwithincreasingvolumefraction
ofSiCintheSiCfractionrangebetween40%and50%.Itshouldbeemphasizedthatthisresultindicatesthatthe
thermalconductancebetweenSiCparticlesandtheAlmatrixishighandalsoindicatesthatdamagesinthesurface
region of the SiC particles are small or negligible during consolidation under continuous solidliquid coexistent
stateinSPSprocessing.Similarresultsarealsofoundinourpreviousworks3234).Italsoshouldbepointedoutthat
thethermalconductivityofthemonomodalcompositedrasticallydecreasedwithincreasingvolumefractionofSiC
inafractionrangehigherthan50%andreached171W/mKinaSiCfractionof65%.Thedecreaseinthethermal
conductivity of this composite is considered to be caused by reduction in the relative packing density of the

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compositeinaSiCfractionrangehigherthan50vol.%.

Thermal conductivity, /(W/mK)

300

250

200

150

Monomodal
Bimodal;

100
40

50

60

Volume fraction of SiC, Vf (%)

70

FIG.6CHANGEINTHERMALCONDUCTIVITYOFSICPARTICLEDISPERSEDALMATRIXCOMPOSITEFABRICATEDBYSPARK
PLASMASINTERING(SPS)ASAFUNCTIONOFTHEVOLUMEFRACTIONOFSICPARTICLESINTHECOMPOSITE.

As seen in Fig. 6, at 55, 60, 65 and 70 vol.% of the volume fraction of SiC, on the other hand, the thermal
conductivityofthebimodalcompositeswas243,239,226and212W/mK,respectivelyanditisalsodecreasedwith
increasing volume fraction of SiC in a SiC fraction range between 55 and 70 vol.%. However, the thermal
conductivityofthebimodalcompositedecreasedgraduallyascomparedwiththatofthemonomodalcomposite,
and it should be mentioned that the thermal conductivity higher than 210W/mK was maintained even in a SiC
fractionrangeof70vol.%.
The thermalconductivityof theAlmatrix composite containing dispersedSiCparticlesfabricated in thepresent
study was compared with those of a similar composite fabricated by Chu et. al using SPS15). The Almatrix
SiCdispersedcompositefabricatedinthepresentstudyshowedhighervaluesofthermalconductivity.Thatis,the
thermalconductivityinthepresentstudyis239252W/mKinavolumefractionrangeofSiCbetween40and55%,
whereas it was 211224 W/mK in a volume fraction range between 50 and 60 % for the case of Chu et. al15). The
thermal conductivity difference between these two cases can be explained as follows. <1> Although similar SPS
process wasused in bothstudies, thestate of composite materials duringSPS processwasdifferent. That is,SiC
particledispersedAlmatrixcompositewasfabricatedincontinuoussolidliquidcoexistentstatebySPSprocessinthe
presentstudy,whereasthatwasfabricatedinsolidstateinthestudybyChuet.al15).ThebondingbetweentheSiC
particleandtheAlmatrixincontinuoussolidliquidcoexistentstatewouldbestrongerthanthatbetweentheSiC
particleandAlmatrixfabricatedinsolidstate.<2>Theformationof Al4C3oftenoccursbydirectcontactbetween
moltenAlandSiCparticlesduringconsolidation,resultinginadetrimentaleffectonthethermalconductivityof
Almatrix composites containing dispersed SiC particles 13, 14, 36). In the case of the continuous solidliquid
coexistentstateduringSPS,moltenareasintheAlmatrixchangetheirlocationseverymomentwithincreasingthe
die temperature at a slow heating stage, resulting in no formation of Al4C3 because of a short time of contact
between molten Al and SiC particles3234). <3> A twostage pressing scheme37) from 80 to 300 MPa was employed
during SPS consolidation in the present study. This pressing scheme would be effective not only in minimizing
pores or porosities but also in making strong bonding between the Al matrix and the SiC particles in Almatrix
compositecontainingdispersedSiCparticles37).
ThethermalconductivityoftheAl/SiCcompositefabricatedinthepresentstudywasalsocomparedwiththoseof
a similar composite fabricated by Chu et. al using metal infiltration technque13, 14). The Almatrix SiCdispersed
compositefabricatedinthepresentstudyshowedhighervaluesoftheralconductivity.Thethermalconductivityin
thepresentstudyis210252W/mKinavolumefractionrangeofSiCbetween40and70%,whereasitwas145186

JournalofMetallurgicalEngineering(ME)Volume5,2016 www.mejournal.org

W/mKinavolumefractionrangebetween45and65%forthecaseofChuet.al13,14).
ThelowerthermalconductivityforthecaseofChuet.al 13,14)canbeexplainedasfollows.Chuet.al13,14)fabricated
Al/SiC composites by liquid metal infiltration technique using not pure Al but Al alloys with Si and/or Mg
additions as a matrix material to avoid the formation of interfacial products such as Al4C3. When Si and Mg
dissolveintotheAlmatrix,thethermalconductivityofthematrixdecreasesandthelowthermalconductivityof
thematrixdecreasesthethermalconductivityofthecomposites.
Although high thermal conductivity was obtained for Al/SiC composite fabricated in the present study, gradual
decreaseinthethermalconductivityofAl/SiCcompositerewithincreasingvolumefractionofSiCinaSiCfraction
range between 55 and 70 vol.% as mentioned above. The gradual decrease in the thermal conductivities of the
bimodalcompositemaybecausedbythefollowingtworeasons:1thethermalconductivityofsmallSiCparticlesis
lowerthanthatoflargeSiCparticleduetothepurityofsmallSiCs,whichislowerthanthatoflargeones;and2
the thermal conductance between small SiC particles and the Al matrix is lower than that between large SiC
particles and the Al matrix, which may be caused by insufficient mixing of small SiC particles with Al matrix
particles. That is, higher thermal conductivity may be obtained for SiCparticledispersed Almatrix bimodal
compositebyusingsmallhighpuritySiCpowder,byoptimizationofthemixingofSiCandAlmatrixpowders,
andbyusingAlmatrixparticlesmuchsmallerthanSiCparticles.
CoefficientsofThermalExpansion
Two models by Turner38) and by Kerner39) have been proposed to calculate theoretical coefficients of thermal
expansion(CTEs)ofacompositematerial3741).Kernermodeltakessheareffectsintoaccountatboundariesbetween
particles and the matrix, whereas Turner model does not take such effects into account. Consequently, Kerner
modelhaswidelybeenusedfortheoreticalevaluationsoftheCTEsofcompositematerial.Hence,wealsoutilize
KernermodelinthepresentstudytoevaluateCTEsofthecompositesfabricated.Kernermodelcanbeexpressedin
equation(5),

c m .Vm d Vd Vd Vm ( d m )

Kd Km
(5)
Vm K m Vd K d (3K d K m / 4Gm )

where cis the coefficient of thermal expansion of the composite, d the coefficient of thermal expansion of the
dispersions (in this case, SiC, 4.5106/K), m the coefficient of thermal expansion of the matrix (in this case,
aluminum,24.0106/K),Vdthevolumefractionofthedispersionsinthecomposites,Vmthevolumefractionofthe
matrixinthecomposites,Kdthebulkmodulusofthedispersions(inthiscaseSiC,2.21011Pa),Kmthebulkmodulus
ofthematrix(inthiscase,aluminum,7.61010Pa)andGmtheshearmodulusofthematrix(inthiscase,aluminum,
2.61010Pa),
Figure 7 shows the comparison between theoretically predicted and experimentally obtained CTEs for the
SiCparticledispersedAlmatrixcomposites.KernersupperlineisobtainedbyconsideringAlasthematrixofthe
composite, whereas its lower line is obtained by considering the dispersed SiC as the matrix. For comparison, a
theoreticallyobtainedcurveusingTurnersmodelisalsoshown.Showninthisfigurearethetwolinesobtainedby
reversingtheroleofmatrixanddispersionsinKernermodel.ExperimentallyobtainedCTEsofthecompositesis
seentofallintheupperlineofKernermodel.TheCTEsoftheAlmatrixcompositescontainingmonomodalSiC
particlesobtainedinthepresentstudyare14.3106/Kat40vol.%SiCand12.5106/Kat50vol.%SiC.Inaddition,
theCTEsofAlmatrixcompositescontainingbimodalSiCparticlesare9.88106/Kat65vol.%SiCand9.39106/K
at 70 vol.% SiC. This result indicates that the SiC particles have bonded well to the Al matrix in the composite
fabricatedbySPS.
TheCTEsofAlmatrixcompositewithSiCobtainedinthepresentstudyare14.3and12.5106/Kat42.8and51.9
vol.% SiC, respectively. Considering into account 4~8106/K of the CTEs for some packaging base materials
currently in use, it should be appropriate to add more SiC particles to Almatrix composites to meet suitable
conditionsasheatspreaders.Inotherwords,AlmatrixcompositescontainingSiChigherthan75vol.%wouldbe
morepreferableinapplications.

www.mejournal.org JournalofMetallurgicalEngineering(ME)Volume5,2016

Coefficient of thermal expansion, (10-6)

25
Turner line
Kerner lower line
Kerner upper line

20

Expermental(Monomodal)
Experimental(Bimodal)

15

10

0
0

20

40

60

80

Volume fraction of SiC, Vf (%)

100

FIG.7COMPARISONOFCOEFFICIENTSOFTHETHERMALEXPANSIONPREDICTEDTHEORETICALLYUSINGKERNERMODELFOR
ALANDSICCOMPOSITEANDTHOSEOBTAINEDEXPERIMENTALLYFORALANDSICOMPOSITECONTAINING40,50,65AND70
VOL.%SICPARTICLES.

Summary
Two kinds of SiCparticledispersed aluminum (Al) matrix composites containing monomodal and bimodal SiC
particles were fabricated in a unique fabrication method, where the powder mixture of SiC, pure Al and
Al5mass%Sialloywasusedtoformcontinuoussolidliquidcoexistentstateduringsparkplasmasintering(SPS)
process.Microstructuresandthermalpropertiesofthecompositesfabricatedinsuchawaywereinvestigatedand
the bimodal and monomodal SiC particle effect on the thermal properties of the composites was evaluated. The
composites were well consolidated in the temperature range between 773 K and 878 K and scanning electron
microscopydetectednoreactionproductattheinterfacebetweentheSiCparticleandtheAlmatrix.Therelative
packing density of the composite containing monomodal SiC particles decreased from 98.9 to 95.1 % with
increasing SiC volume fraction in a volume fraction range between 50 and 60 %. However, the relative packing
densityofthecompositecontainingbimodalSiCparticlesbecamehigherthan98%inaSiCvolumefractionrange
up to 65%. The thermal conductivity of this composite was higher than that of the composite containing
monomodalSiCparticlesinaSiCvolumefractionrangehigherthan55%.Althoughthethermalconductivityofthe
bimodal composite decreased gradually in a SiC fraction range between 55 and 70%, the thermal conductivity
higher than 210W/mK was maintained for the bimodal composite even in a SiC fraction range of 70 vol.%. The
coefficientsofthethermalexpansion,CTEs,ofAlmatrixcompositescontainingSiCparticlesfellintheupperline
ofKernermodel,indicatinggoodbondingbetweentheSiCparticleandtheAlmatrixinthecomposite.
ACKNOWLEDGEMENT

This work was carried out with the support of JSPS KAKENHI Grant Number 26420751. The authors wish to
expresstheirappreciationforthissupport.
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