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Effective thermal conductivity of mixtures of uids and nanometer-size particles is measured by a steady-state
parallel-plate method. The tested uids contain two types of nanoparticles, Al2 O3 and CuO, dispersed in water,
vacuum pump uid, engine oil, and ethylene glycol. Experimental results show that the thermal conductivities of
nanoparticle– uid mixtures are higher than those of the base uids. Using theoretical models of effective thermal
conductivity of a mixture, we have demonstrated that the predicted thermal conductivities of nanoparticle– uid
mixtures are much lower than our measured data, indicating the de ciency in the existing models when used for
nanoparticle– uid mixtures. Possible mechanisms contributing to enhancement of the thermal conductivity of the
mixtures are discussed. A more comprehensive theory is needed to fully explain the behavior of nanoparticle– uid
mixtures.
474
WANG, XU, AND CHOI 475
II. Measurement of Thermal Conductivity heat conduction equation relating the power qP of heater 1, the tem-
of Nanoparticle– Fluid Mixtures perature difference 1T between the two copper plates, and the ge-
Two basic techniques are commonly used for measuring ther- ometry of the liquid cell as
mal conductivitiesof liquids, the transient hot-wire method and the
k D .qP ¢ L g /=.S ¢ 1T / (1)
steady-state method. In the present experiments, the one-dimen-
sional, steady-state parallel-plate method is used. This method pro- where L g (0.9652 mm) is the thickness of the glass spacer between
duces the thermal conductivity data from the measurement in a the two copper plates and S (9.552 cm2 ) is the cross-sectional area
straightforwardmanner, and it requires only a small amount of liquid of the top copper plate. The thermal conductivity of the uid can be
sample. calculated as
Figure 1 shows the experimental apparatus, which follows the
design by Challoner and Powell.12 The uid sample is placed in the k ¢ S ¡ k g ¢ Sg
ke D (2)
volume between two parallel round copper (99.9% purity) plates, S ¡ Sg
and the surface of the liquid is slightly higher than the lower surface
of the upper copper plate. The surface of the liquid can move freely where k g (1.4 W/m ¢ K) and Sg are the thermal conductivity and the
to accommodate the thermal expansion of the liquid. Any gas bub- total cross-sectionalarea of the glass spacers, respectively.
bles are carefullyavoided when the cell is lled with a liquid sample. Experimental error is estimated by comparing the measured ther-
The cross-sectionalarea of the top plate is 9.552 cm2 . The two cop- mal conductivityof DI water and ethylene glycol with the published
per plates are separatedby three small glass spacers with a thickness data.13 The absolute error for the thermal conductivitiesof both u-
of 0.9652 mm each and a total surface area of 13.76 mm2 . To control ids is less than §3%.
the temperature surroundingthe liquid cell, the liquid cell is housed The thermal conductivity of liquid changes with temperature.
in a larger cell made of aluminum. The top copper plate is centered When a small temperature differencebetween the two copper plates
and separated from the inside wall of the aluminum cell. Holes of is used, then the effect of the temperature variation is small. Us-
0.89-mm diameter are drilled into the copper plates and the ing the thermal conductivity data of water, it is estimated that the
aluminum cell. E-type thermocouples (nickel– chromium/copper– maximum measurement uncertaintyin this work caused by the tem-
nickel) are inserted into these holes to measure the temperatures. perature variation across the liquid cell is 0.5%.
The locations of the thermocouples in the top and lower copper
plates are very close to the lower surface of the upper plate and III. Experimental Results
to the upper surface of the lower plate. Because the thermal con- Nanometer-size Al2 O3 and CuO powders are obtained from
ductivity of copper is much higher than that of the liquid, these Nanophase Technology Company (Burr Ridge, Illinois). The aver-
thermocouples provide temperatures at the surfaces of the plates. A age diameter of the Al2 O3 powders (° phase) is 28 nm, and the
total of 14 thermocouples are used. average diameter of the CuO powders is 23 nm. The as-received
In this work, although the absolute value of thermal conductivity powders are sealed and are dry and loosely agglomerated.The pow-
is to be measured,there is no need to obtain the absolutetemperature. ders are dispersed into DI water, vacuum pump uid (TKO-W/7,
It is more important to measure accurately the temperature increase Kurt J. Lesker Company, Clairton, Pennsylvania), ethylene glycol,
of each thermocoupleand to minimize the difference in temperature and engine oil (Pennzoil 10W-30). The powders are blended in a
readings when the thermocouples are at the same temperature. It blender for one-half an hour and then are placed in an ultrasonic
was found that the accuracy in measuring the temperature increase bath for another half an hour for breaking agglomerates. A number
is better than 0.02± C. The differences in the thermocouple readings of other techniques are used to disperse the powders in water and
are recorded when the thermocouplesare at the same temperature in will be described later. The volume fraction of the powder in liquid
a water bath and are used as calibration values in later experiments. is calculated from the weight of the dry powder and the total vol-
During the experiment, heater 1 provides the heat ux from the ume of the mixture. Absorption of water vapor could occur when
upper copper plate to the lower copper plate. Heater 4 is used to the powders are exposed to air just before placing the powders into
maintain the uniformity of the temperaturein the lower copper plate. uids; however, the exposed surface of the powders is much smaller
Heaters 2 and 3 are used to raise the temperature of the aluminum than the total surface of the powders. The error caused by water
cell to that of the upper copperplate to eliminateconvectionand radi- absorption in determining the volume fraction is negligible.
ation losses from the upper copper plate. Therefore, input powers to Samples using water, pump uid, or engineoil as the base uid are
all of the heaters need to be carefully adjusted. During all measure- stable when the volume fraction is less than 10%. No agglomeration
ments, the temperature difference between the upper copper plate is observed for a number of weeks (at room temperature). When the
and the inside wall of the aluminum cell is less than 0.05± C, and volume fraction is greater than 10%, the uid becomes occulated
the temperature uniformity in the top and the bottom copper plates in the dispersion process. Samples using ethylene glycol as the base
is better than 0.02± C. The temperature difference between the two uid are stable up to a volume fraction of 16%. Unless otherwise
copper plates varies between 1 and 3± C. noted, samples are prepared without adjusting the pH value.
All of the heat supplied by heater 1 ows through the liquid be- Results of the thermal conductivity of Al2 O3 dispersions at the
tween the upper and the lower copper plates. Therefore, the overall room temperature(297 K) are shown in Fig. 2a. Figure 2b shows the
thermal conductivity across the two copper plates, including the ef- ratios of the thermal conductivity of the mixture ke to the thermal
fect of the glass spacers, can be calculatedfrom the one-dimensional conductivityof the correspondingbase uid k f . For all of the uids,
the thermal conductivity of the mixture increases with the volume
fraction of the powder. However, for a given volume fraction, the
thermal conductivityincreases are different for different uids. The
increases in ethylene glycol and engine oil are the highest, whereas
that in the pump uid is the lowest, about half of that in ethylene
glycol and engine oil. The effectivethermal conductivityof ethylene
glycol increases 26% when approximately 5 vol% of Al2 O3 pow-
ders are added, and it increases 40% when approximately8 vol% of
Al2 O3 powders are added. Figures 3a and 3b show thermal conduc-
tivities of CuO dispersionsin water and in ethylene glycol. For both
uids, thermal conductivityratio increases with the volume fraction
with the same linearity.
To examine the effect of different sample preparationtechniques,
Al2 O3 powders are dispersed in water using three different tech-
Fig. 1 Experimental apparatus. niques. Mechanical blending (method 1), coating particles with
476 WANG, XU, AND CHOI
Fig. 2a Thermal conductivityas a function of volumefraction of Al 2 O3 Fig. 4 Thermal conductivity of Al2 O3 – water mixtures prepared by
powders in different uids. three different methods.
IV. Discussion
In this section, thermal conductivitiesof nanoparticle– uid mix-
tures measured in this work are rst compared with experimental
data reported in the literature. Effective thermal conductivity theo-
ries in the literature are used to compute the thermal conductivityof
the mixtures. Results calculated from the effective thermal conduc-
tivity theories are compared with the measured data. Other possible
transport mechanisms and potential applications of nanoparticle–
Fig. 3a Thermal conductivity as a function of volume fraction of CuO
uid mixtures are discussed.
powders in ethylene glycol and water.
20,000 rpm). Lee et al.14 did not use such equipment and, therefore, tions. The difference between the measured data and the prediction
nanoparticles in their uids were agglomerated and larger than is less than a few percent when the volume fraction of the dis-
those used by Masuda et al.8 In the present experiments, the tech- persed phase is less than 20% (Ref. 20). The experimental data in
niques used to prepare the mixtures are different from those used by the comparison included those obtained by Turner21 on the electri-
Masuda et al.8 and Lee et al.14 This comparison, together with the cal conductivity of 0.15-mm or larger solid particles uidized by
data shown in Fig. 4, shows that the effectivethermal conductivityof aqueous sodium chloride solutions and those obtained by Meredith
nanoparticle– uid mixtures depends on the preparation technique, and Tobias22 on electrical conductivity of emulsions of oil in water
which might change the morphology of the nanoparticles. Also, in or water in oil with droplet sizes between 11 and 206 ¹m. There-
the work of Masuda et al.,8 acid (HCl) or base (NaOH) was added to fore, these effective thermal conductivities can accurately predict
the uids so that electrostatic repulsive forces among the particles the thermal conductivity of particle– uid mixtures when the parti-
kept the powders dispersed.Such additives,althoughlow in volume, cle size is larger than tens of micrometers.
may change the thermal conductivity of the mixture. In this work, The effective thermal conductivity equations shown in Table 1
acid or base are not used in most of the samples (except the one with are used to compute the thermal conductivity of the nanoparticle–
polymer coatings) because of concerns of corrosions by the acid or uid mixtures made in this work. The computed results of Al2 O3–
base. ethylene glycol are shown in Figs. 5a and 5b, together with the
measureddata. From Figs. 5a and 5b, it can be seen that the measured
B. Comparison of Measured Thermal Conductivity thermal conductivity is greater than the value calculated using the
of Nanoparticle– Fluid Mixtures with Theoretical Results effective thermal conductivity theories.
Thermal conductivitiesof composite materials have been studied
for more than a century. Various theories have been developed to
compute the thermal conductivity of two-phase materials based on
the thermal conductivityof the solid and the liquid and their relative
volume fractions. Here, the discussions are focused mainly on the
theories for statistically homogeneous, isotropic composite mate-
rials with randomly dispersed spherical particles having uniform
particle size. Table 1 summarizes some equations frequently used
in the literature.15¡20 Maxwell’s equation,15 shown in Table 1, was
the rst theoretical approach used to calculate the effective elec-
trical conductivity of a random suspension of spherical particles.
Because of the identical mathematical formulations, computations
of electrical conductivity of mixtures are the same as computations
of thermal conductivity, dielectric constant, and magnetic perme-
ability. Maxwell’s results are valid for dilute suspensions, that is, a)
the volume fraction Á ¿ 1, or, to the order 0.Á 1 /. A second-order
formulation extended from the Maxwell’s result was rst developed
by Jeffrey16 and later modi ed by several authors. No higher-order
formulations have been reported. Bonnecaze and Brady’s numer-
ical simulation19;20 considered far- and near- eld interactions be-
tween multiple particles. They showed that for random dispersions
of spheres, their simulation results agreed with Jeffrey’s equation16
up to a volume fraction of 20%, whereas Maxwell’s equation15 gave
results within 3% of their calculationfor a conductivityratio ® D 10
and within 13% when ® D 0:01, up to a volume fraction of 40%.
For high-volume fractions (Á > 60%), the theoretical equations are
generally not applicable because the near- eld interactions among
particles that produce a larger k e at high-volume fractions are not b)
considered. Fig. 5 Measured thermal conductivities of Al2 O3 – ethylene glycol
The equations in Table 1 have been successfully veri ed by ex- mixtures vs effective thermal conductivities calculated from theories:
perimental data for mixtures with large particles and low concentra- a) = 10 and b) = 1 .
ke 3.® ¡ 1/
Davis17 D1C [Á C f .®/Á 2 C 0.Á 3 /] 1) Accurate to order Á2 ; high-order terms represent
kf .® C 2/ ¡ .® ¡ 1/Á pair interactions of randomly dispersed spheres
2) f .®/ D 2:5 for ® D 10; f .®/ D 0:50 for ® D 1
ke
Lu and Lin18 D 1 C a ¢ Á C b ¢ Á2 1) Near- and far- eld pair interactions are considered,
kf applicable to nonspherical inclusions
2) For spherical particles, a D 2:25, b D 2:27
for ® D 10; a D 3:00, b D 4:51 for ® D 1
Bonnecaze N/A 1) Numerical simulation, expressions not given
and Brady19;20 2) Near- and far- eld interactions among two
or more particles are considered
a
Effective thermal conductivity of the mixture ke , thermal conductivity of the uid k f , ratio of thermal conductivity of particle to thermal conductivity of uid ®, and volume
fraction of particles in uid Á.
478 WANG, XU, AND CHOI
In the calculation, the thermal conductivity of Al2 O3 nanoparti- where Pe f D .r 2 °½c p f = k f /, r is the radius of particle, ° is the ve-
cles is taken as 2.5 W/m ¢ K (® D 10), lower than its bulk value of locity gradient calculated from the mean Brownian motion velocity
36 W/m ¢ K. No thermal conductivity data of the ° -Al2 O3 nanopar- and the average distance between particles, ½ is the base liquid
ticles are available. It is known that in the micro- and nanoscale density, and c p f is the speci c heat of base liquid. The thermal
regime the thermal conductivity is lower than that of the bulk ma- transport caused by the translational movement of particles was
terials. For example, it was found, through solving the Boltzmann given by Gupte et al.25 In their study, the base liquid and particles
transportequationof heat carrier in the host medium, that heat trans- were assumed to have identical thermal conductivity, density, and
fer surroundinga nanometer-sizeparticlewhose mean free path is on heat capacity.Their results are tted with a fourth-orderpolynomial
the order of its physical dimension is reduced and localized heating as
occurs.23 The mean free path in polycrystalline Al2 O3 is estimated
to be around 5 nm. Although the mean free path is smaller than 1ke;t D 0:0556Pet C 0:1649Pe2t ¡ 0:0391Pe3t C 0:0034Pe4t k f
the diameter of the particles, the ° -phase Al2 O3 particles used in
this work consist of highly distorted structures. Therefore, it is ex- (4)
pected that the mixture’s thermal conductivity is reduced. On the
other hand, from Fig. 5b, it can be seen that the measured thermal where the modi ed Peclet number is de ned as Pet D .U L½c p f =
conductivityof the mixture is greater than the value calculated using K f /Á 3=4 , U is the velocity of the particles relative to the base liquid,
the effective thermal conductivity theories even when the thermal and L D .r =Á 1=3 / ¢ .4¼ =3/1=3 . The total increase in thermal conduc-
conductivity of Al2 O3 is taken as in nity. Therefore, the theoretical tivity by the Brownian motion of particles consists of the increases
models, which compared well with the measurements of disper- due to both translational and rotational motions. However, it can be
sions with large size (micrometer or larger) particles, underpredict seen from Eqs. (3) and (4) that the increasein thermal conductivityis
the thermal conductivity increase in nanoparticle– uid mixtures. small because of the small (modi ed) Peclet number, meaning that
This suggests that all of the current models, which only account heat transferred by advection of the nanoparticles is less than that
for the differences between thermal conductivity of particles and transferred by diffusion. In other words, when the particles move
uids, are not suf cient to explain the energy transfer processes in in liquid, the temperature of the particles quickly equilibrate with
nanoparticle– uid mixtures. that of the surrounding uids due to the small size of the particles.
Calculations based on Eqs. (3) and (4) show that up to a volume
C. Mechanisms of Thermal Conductivity Increase fraction of 10%, the thermal conductivity increase by the Brownian
in Nanoparticle– Fluid Mixtures motion is less than 0.5% for the Al2 O3– liquid mixture. Therefore,
the Brownian motion does not contribute signi cantly to the energy
In nanoparticle– uid mixtures, other effects such as the micro- transport in nanoparticle– uid mixtures.
scopic motion of particles,particle structures,and surface properties It is dif cult to estimate the microscopic motions of particles
may cause additional heat transfer in the uids. These effects are caused by other microscopic forces and the effects of these forces
discussed as follows. on heat transfer. The surfaces of metal oxide particlesare terminated
by a monolayer of hydroxyl (OH) when the particles are exposed to
1. Microscopic Motion water or water vapor. This monolayer will induce an electric double
Because of the small size of the particles in the uids, additional layer,26 the thicknessof which varieswith the uids and the chemical
energy transport can arise from the motions induced by stochas- properties of the particle surface. For weak electrolytic solutions,
tic (Brownian) and interparticle forces. Motions of particles cause a typical double-layer thickness is between 10 and 100 nm (Ref.
microconvection that enhances heat transfer. In all of the effective 27). Therefore, when the particle size is in the tens of nanometers,
conductivity models discussed earlier, the particles are assumed to the thickness of the double layer is comparable to the size of the
be stationary when there is no bulk motion of the uids, which is particle. On the other hand, for the uids used in this work whose
true when the particle is large. In nanoparticle– uid mixtures, mi- particle volume fraction is a few percents, the average distance be-
croscopic forces can be signi cant. Forces acting on a nanometer- tween particles is about the same as the particle size, in the tens
size particle include the Van der Waals force, the electrostatic force of nanometers. For example, for 5 vol% Al2 O3 , the average dis-
resulting from the electric double layer at the particle surface, the tance between particles is about 33 nm. When the distance between
stochastic force that gives rise to the Brownian motion of particles, the particles is as small as tens of nanometers, the Van der Waals
and the hydrodynamic force. Motions of the particles and uids force is signi cant. The electric double layer and the Van der Waals
are induced and affected by the collective effect of these forces. force could have strong electrokinetic effects on the movement of
Notice that the stochastic force and the electrostatic force are sig- the nanoparticles and on the heat transport process.
ni cant only for small particles, whereas the Van der Waals force
is high when the distance between particles is small. Therefore, 2. Chain Structure
there exists a relation between the effective thermal conductivity
and the particle size, as observed by comparing the data obtained Studies of nanoparticles by transmission electron microscopy
(TEM) show that the Al2 O3 particles used in this work are spherical.
in this work with reported values. However, these forces have not
been calculated accurately because they are strongly in uenced However, some particlesin the liquids are not separatedcompletely.
by the chemical properties of the particle surface and the host- Using TEM, it is found that some particles adhere together to form
ing uid, the size distribution, and the con guration of the parti- a chain structure. According to Hamilton and Crosser,28 heat trans-
cle system. Little quantitative research has been done on the heat fer could be enhanced if the particles form chain structures because
transfer enhancement by the microscopic motion induced by these more heat is transportedalong those chains oriented along the direc-
forces. tion of the heat ux. The effect of the particle size is not considered
The heat transfer enhancement due to the Brownian motion can in their treatment. Assuming that an average chain consists of three
be estimated with the known temperature of the uid and the size particles, the thermal conductivity of particles is 10 times that of
of the particles. The increase of thermal conductivity due to the the base liquid, and there is 5 vol% particles in liquid, the thermal
rotational motion of a spherical particle can be estimated as24 conductivity will increase 3% according to Hamilton and Crosser’s
equation.28 If the thermal conductivity ratio is taken as in nity, the
increase of thermal conductivity is about 7%. Therefore, it is pos-
1:176.k p ¡ k f /2 sible that the chain structure contributes to a thermal conductivity
1k e;r D k f ¢ Á ¢
.k p C 2k f /2 increase in nanoparticle– uid mixtures. However, the actual particle
structures in liquids may not be preserved when the TEM measure-
kp ¡ k f 3 ments are taken. Therefore, the effects of particle structures are not
C 5 £ 0:6 ¡ 0:028 Pe 2f (3) accurately determined. Currently, there are no techniques available
k p C 2k f
for characterizing the structures of nanoparticles in liquid.
WANG, XU, AND CHOI 479
D. Viscosity of Nanoparticle– Fluid Mixtures and Applications with nanoparticles. With this assumption, the desirable heat trans-
of Nanoparticle– Fluid Mixtures for Heat Transfer Enhancement fer increase is offset by the undesirable increase in pressure drop.
Because of the increased thermal conductivity of nanoparticle– However, when uids with nanoparticles are owing in a channel,
uid mixtures over the base liquids, nanoparticle– uid mixtures motions of particles also enhance heat transfer due to the decreased
can be used for heat transfer enhancement. On the other hand, the thermal boundarythickness,enhancementof turbulence,and/or heat
viscosityof the mixtures should also be taken into accountbecause it conduction between nanoparticles and the wall as was found in the
is one of the parameters that determine the required pumping power studies of gas– particle ow. Therefore, more studies are needed on
of a heat transfer system. convection heat transfer in uids with nanoparticles to justify the
Figure 6 shows the relative viscosity of Al2 O3– water solutions use of them as a heat transfer enhancement medium.
dispersed by different techniques, that is, mechanical blending
(method 1), coating particles with polymers (method 2), and l-
V. Conclusions
tration (method 3). These viscosity data are obtained with a precali- The effectivethermal conductivitiesof uids with Al2 O3 and CuO
brated viscometer. It is seen that the solutions dispersed by methods nanoparticlesdispersedin water, vacuum pump uid, engine oil, and
2 and 3 have lower viscosity, indicating that the particles are better ethylene glycol are measured. The experimental results show that
dispersed. (It is a common practice to determine whether particles the thermal conductivities of nanoparticle– uid mixtures increase
are well dispersed based on whether or not the viscosity value is relative to those of the base uids.
minimized.29 ) The Al2 O3– water mixture shows a viscosity increase A comparison between the present experimental data and those
between 20 and 30% for 3 vol% Al2 O3 solutions compared to that of other investigatorsshows a possible relation between the thermal
of water alone. On the other hand, the viscosity of Al2 O3– water conductivity increase and the particle size: The thermal conduc-
used by Pak and Cho11 was three times higher than that of water. tivity of nanoparticle– uid mixtures increases with decreasing the
This large discrepancy could be due to differences in the dispersion particle size. The thermal conductivity increase also depends on the
techniques and differences in the size of the particles. dispersion technique.
The viscosity of the Al2 O3– ethylene glycol solution is shown Using existing models for computing the effective thermal con-
in Fig. 7. Compared with the Al2 O3– water solution, the Al 2 O3– ductivity of a mixture, it is found that thermal conductivities com-
ethylene glycol solution has a similar viscosity increase but a higher puted by theoretical models are much lower than the measured data,
thermal conductivity increase. indicating the de ciencies of the existing models in describing heat
For laminar ow in a circular tube, the convection heat transfer transfer at the nanometer scale in uids. It appears that the thermal
coef cient is proportional to the thermal conductivity of the uid, conductivity of nanoparticle uid mixtures is dependent on the mi-
whereas the pressure drop is proportional to viscosity. For turbu- croscopicmotion and the particle structure.Any new models of ther-
lence ow in a circular tube, the pressure drop is proportional to mal conductivityof liquids suspendedwith nanometer-sizeparticles
¹1=5 , whereas the convectionheat transfer coef cient is proportional should include the microscopic motion and structure-dependent be-
to .k 2f =3 =¹0:467 / according to the Colburn’s equation (see Ref. 13). havior that are closely related to the size and surface properties of
Using the measured thermal conductivity and viscosity data, the the particles. To use nanoparticle– uid mixtures as a heat transfer
increase in pressure drop is found to be about the same as the in- enhancementmedium, more studies on heat transfer in the uid ow
crease in heat transfer for all of the uid– particle mixtures stud- are needed.
ied in this work. This estimation is based on the assumption that
there are no other heat transfer mechanisms in the ow of the uids
Acknowledgments
Support of this work by the National Science Foundation (CTS-
9624890) and the U.S. Department of Energy, Of ce of Science,
Laboratory Technology Research Program, under Contract W-31-
109-Eng-38, is acknowledged.
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