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Article history: In this study, a new analytical model for the effective thermal conductivity of liquids containing dis-
Received 3 August 2015 persed spherical and non-spherical nanometer particles was developed. In addition to heat conduction
Received in revised form 26 February 2016 in the base fluid and the nanoparticles, we also consider convective heat transfer caused by the
Accepted 30 March 2016
Brownian motion of the particles. For nanoparticle suspensions, the latter mechanism has significant
influence on the effective thermal conductivity, which is reduced compared to a system in which only
conduction is considered. The simple model developed allows for the prediction of the effective thermal
Keywords:
conductivity of nanofluids as a function of volume fraction, diameter, and shape of the nanoparticles as
Effective thermal conductivity
Modeling
well as temperature. Due to the inconsistency of experimental data in the literature, the model has been
Nanofluids compared with the established Hamilton–Crosser model and other empirical models for the systems alu-
Nanoparticles minum oxide (Al2O3) and titanium dioxide (TiO2) suspended in water and ethylene glycol. The theoretical
estimates show no anomalous enhancement of the effective thermal conductivity and agree very well
with the Hamilton–Crosser model within relative deviations of less than 8% for volume fractions of spher-
ical particles up to 0.25. In accordance with the Hamilton–Crosser model for non-spherical particles, our
model reveals that a more distinct increase in the enhancement of the effective thermal conductivity can
be achieved using non-spherical nanoparticles having a larger volume-specific surface area.
Ó 2016 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.ijheatmasstransfer.2016.03.129
0017-9310/Ó 2016 Elsevier Ltd. All rights reserved.
K.N. Shukla et al. / International Journal of Heat and Mass Transfer 99 (2016) 532–540 533
Nomenclature
a empirical parameter in model of Lin and Lu [13] Rp,conv thermal resistance of nanoparticle due to convection
abf thermal diffusivity of base fluid (m2 s1) (K W1)
A surface area of particle (m2) Re Reynolds number
b empirical parameter in model of Lin and Lu [13] T temperature (K)
dp diameter of spherical nanoparticle (m) up velocity of nanoparticle (m s1)
dp,eq volume-equivalent diameter of non-spherical nanopar- V volume (m3)
ticle (m)
h convective heat transfer coefficient (W m2 K1) Greek symbols
k thermal conductivity (W m1 K1) mbf kinematic viscosity of base fluid (m2 s1)
kb Boltzmann constant (1.3806488 1023 J K1) u volume fraction of nanoparticles
L edge length of the cube (m) qp density of nanoparticle (kg m3)
m mass of nanoparticle (kg) w sphericity of nanoparticle
n empirical shape factor of particle
N number of nanoparticles Subscripts
Nu Nußelt number
bf base fluid
Pe Peclet number cond pure conduction
Pr Prandtl number conv convection
Rbf thermal resistance of bulk fluid due to heat conduction
eff effective
(K W1) non-sph non-spherical
Reff effective thermal resistance of nanofluid (K W1) p particle
Rp total thermal resistance of nanoparticle (K W1) sph spherical
Rp,cond thermal resistance of nanoparticle due to heat conduc-
tion (K W1)
formulations of the two transport phenomena. Their model is also Eq. (5) presents a simple linear relation for the effective thermal
applicable for systems of liquids containing solid particles with dif- conductivity of diluted suspensions. Based on the continuum
ferent shapes and predicts their effective thermal conductivity keff model of Hamilton and Crosser [12], there have been some modi-
by fications considering additional effects. For example, Lu and Lin
[13] considered near- and far-field pair interactions applicable to
keff kp þ ðn 1Þkbf ðn 1Þuðkbf kp Þ
¼ : ð1Þ spherical and non-spherical inclusions and modified Eq. (5) to a
kbf kp þ ðn 1Þkbf þ uðkbf kp Þ
second-order polynomial,
The terms kbf and kp denote the thermal conductivities of the
base fluid (bf), that is the continuous phase, and the solid particle keff
¼ 1 þ au þ bu2 : ð6Þ
(p), that is the dispersed phase. u is the volume fraction of the dis- kbf
persed particles, while n is an empirical shape factor. The latter is
For spherical isotropic inclusions, the constants a and b are
connected with the sphericity w via
given as a = 2.25 and b = 2.27 for kp/kbf = 10 as well as a = 3.00
3 and b = 4.51 for kp/kbf ? 1. For non-spherical inclusions, anisotro-
n¼ : ð2Þ
w pic effects have to be considered which results in the formulation
of an effective thermal conductivity tensor for an anisotropic med-
The sphericity of a particle is defined as the ratio of the surface
ium. Besides the models described above, there are numerous
area of a sphere, Ap,sph, having the same volume as the particle, Vp,
other predictive methods – most of them empirical or complex –
to the surface area of the particle, Ap, according to
for the effective thermal conductivity that cannot all be mentioned
p1=3 ð6V p Þ2=3 here. A review about theoretical studies on the effective
w¼ : ð3Þ thermal conductivity of nanofluids is given by Kleinstreuer and
Ap
Feng [14].
Particles with strong deviations from spherical shape show Recently, Tertsinidou et al. [2] evaluated extensive data on the
smaller w and thus larger n values. For spherical particles with effective thermal conductivity of nanoparticle suspensions con-
w = 1 and n = 3, Eq. (1) can be simplified to the original Maxwell- taining aluminum oxide (Al2O3), copper (Cu), copper oxide (CuO),
like equation and titanium dioxide (TiO2) suspended in water (H2O) and ethy-
lene glycol (EG). When results for the same thermodynamic system
keff kp þ 2kbf 2uðkbf kp Þ
¼ ð4Þ are obtained using proven experimental techniques, they con-
kbf kp þ 2kbf þ uðkbf kp Þ cluded that the effective thermal conductivity of nanofluids exhi-
for predicting the enhancement of the effective thermal conductiv- bits no inconsistency with the continuum model of Hamilton and
ity of nanofluids containing spherical solid particles. Crosser [12]. The broad span of values for the enhancement of
The effective model of Hamilton and Crosser [12] can be applied effective thermal conductivity in the literature, with relative devi-
to low particle volume fractions and shows no dependence on the ations of several tens of percents for a given system, is rather
particle diameter and a very weak dependence on the temperature. attributed to poor characterization of the thermodynamic system
For kp kbf and small u, Eq. (1) reduces to and/or the application of experimental techniques of unproven
validity [2]. A systematic benchmark study [15] on the thermal
keff
¼ 1 þ nu: ð5Þ conductivity of nanofluids, performed over 30 laboratories world-
kbf wide and using a variety of experimental techniques, has also
534 K.N. Shukla et al. / International Journal of Heat and Mass Transfer 99 (2016) 532–540
pd3p
u¼ : ð8Þ
6L3
Thus, the particle diameter can be related to the side length of
the elementary cube by
1=3
6u
dp ¼ L: ð9Þ
p
Based on Eq. (9), the model is restricted to dp/L < 1. This imposes
a condition on the applicable particle volume fraction of
u < p/6 0.52, i.e., the maximum packing of spherical particles in
a nanofluid. However, such a dense packing is not realistic for a
nanofluid in terms of its synthesis and the suspension stability.
Thus, only reasonable values of u < 0.25 are considered within this
study.
Regarding non-spherical particles such as cylinders or plates of
volume Vnon-sph, they can be regarded as theoretical spherical par-
ticles having the same volumes as the non-spherical particles. The
volume-equivalent particle diameter of the non-spherical particles,
dp,eq, is
Fig. 1. Conceptual three-dimensional sketch of a cube with length L containing a 1
6V non-sph 3
spherical nanoparticle of diameter dp and bulk fluid molecules. dp;eq ¼ : ð10Þ
p
shown good agreement between the experimental data and the This approach allows for the same formulation of the volume
corresponding data predicted by the Hamilton–Crosser model [12]. fraction of non-spherical particles in the bulk fluid as given in Eq.
Nevertheless, the continuum model does not explicitly account (8). Furthermore, it can be used to model the heat transfer in such
for effects that are induced by nanoparticles with respect to the systems analogously to that described in the following for systems
effective thermal conductivity of nanofluids. Nanoparticles may with spherical particles.
cause additional energy transport due to Brownian motion because The basic idea of the present modeling approach is to treat the
of their small size, large specific surface area, and morphology. The heat transfer problem in connection with nanofluids by the analy-
motion of nanoparticles and base fluid molecules is affected by the sis of the corresponding thermal resistances present in such sys-
combined effect of hydrodynamic and Brownian forces that pro- tems. Fig. 2 illustrates the corresponding circuit diagram for the
duce micro-convection in the nanofluids. The aim of the present total thermal resistance of the nanofluid Reff based on the cube
work was to develop a new model for the effective thermal con- shown in Fig. 1.
ductivity of macroscopically static nanofluids taking into account The thermal resistance of the base fluid, Rbf, is considered to be
the heat transfer mechanisms caused by convection as well as parallel to the thermal resistance of the nanoparticle, Rp. Thus, Reff
thermal conduction of the particles and the base fluid. A compar- can be expressed by
ison of the model with the established model of Hamilton and
Crosser [12] and the predictions of Lu and Lin [13] is drawn for 1 1u u
¼ þ : ð11Þ
selected nanofluid systems as a function of the parameters volume Reff Rbf Rp
fraction, particle diameter, particle shape, and temperature.
Arranging the resistances of the bulk fluid and the particles in
parallel is reasonable because a heat flux can be either conducted
2. Description of the model through the base fluid or through the particle along a one-
dimensional temperature gradient. The key for a realistic descrip-
To develop an analytical model for the thermal conductivity of tion of the thermal resistance of the nanofluid is that the base fluid
liquids with suspended nanoparticles, the thermal resistances of as a continuum fluid phase is analogously treated as a continuum
the base fluid and the nanoparticles as well as of convection resistance. To account for the volumes in which the resistances of
induced in the fluid due to Brownian motion of the nanoparticles the two phases are present, the inverse values of the thermal resis-
are determined. Other possible heat transfer effects in form of ther- tances Rbf and Rp are weighted in Eq. (11) by the corresponding vol-
mal radiation or thermal diffusion of the nanoparticles due to a ume fractions (1u) and u. Here, the circumstance that the volume
temperature gradient were found to be negligible. fractions in the elementary cube are the same as those in the total
In the following, the model is derived on basis of a nanofluid nanofluid system can be employed.
system containing spherical particles. Furthermore, analogies or
differences in connection with the modeling of nanofluids contain-
ing non-spherical particles such as cylinders, cubes, or plates are
given. It is assumed that N nanoparticles of spherical shape with
diameter dp are uniformly suspended in a volume V of the nano-
fluid. The volume fraction of the nanoparticles u is then defined by
Npdp
3
u¼ : ð7Þ
6V
The volume V is now divided into N equal parts such that each
nanoparticle is located in a cube with a side of length L. Fig. 1
depicts a three-dimensional sketch of such a nanoparticle-cube Fig. 2. Circuit diagram for the thermal resistances of the bulk fluid due to
system. From Eq. (7) it follows that conduction and of the nanoparticle due to conduction and Brownian convection.
K.N. Shukla et al. / International Journal of Heat and Mass Transfer 99 (2016) 532–540 535
Reff and Rbf are defined by the corresponding thermal conductiv- depends on the surface area of the particle Ap and the convective
ities keff and kbf and the geometries of the cube in the form of heat transfer coefficient h. Eq. (3) can be used to derive an expres-
sion for Ap for particles of arbitrary shape,
L 1
Reff ¼ ¼ ð12Þ
Ap;sph pdp
2
keff L2 keff L
Ap ¼ ¼ : ð17Þ
and w w
2 1=3 31
1=3 1 þ 0:5 6u
w
u4=3 6 7
keff 6 p k
¼ ð1 uÞ þ p
bf
4 þ 5 :
kbf p 2 kp Nu
ð24Þ
Three different contributions can be seen in Eq. (24). The first
term (1u) considers the influence of the bulk fluid in form of its
volume fraction while the second term is related to the nanoparti-
cles. In the latter term, the brackets include the contributions from
conduction through the particles (associated with kp) and from
convective heat transfer between the particles and the bulk fluid
(given by w/Nu).
The thermal resistance due to micro-convection in the bound- It is obvious that neglecting the thermal resistance contribution
ary layer at the nanoparticle for all systems is by at least one order from the convective heat transfer between particles and base fluid
of magnitude larger than that due to conduction through the results in much larger enhancement factors because the thermal
nanoparticle itself. Increasing particle volume fractions result in resistance of the nanoparticle is significantly reduced to only the
only a slight decrease in the thermal resistance ratio. The same resistance of conduction through the particle Rp,cond. (see Fig. 5).
trends are also found for varied particle size and temperature. This Consequently, the additionally considered thermal resistance
result can be related to the fact that Nu is close to 2 for all nanopar- between contacting particles and fluid molecules reduces the
ticle systems studied here. Thus, the convective resistance caused effective thermal conductivity of the nanofluid compared to a the-
by Brownian motion and being proportional to 1/Nu 1/2 is more oretical system featuring no convective resistance between parti-
significant in Eq. (24) than the conduction resistance term propor- cles and fluid. Of course, an enhancement of the convective heat
tional to kbf/kp. Depending on the liquid-nanoparticle combination, transfer with, e.g., increasing Re, Pe, and thus Nu numbers
kbf/kp values between about 1/20 for TiO2/H2O and 1/160 for Al2O3/ decreases the corresponding resistance, but this effect is rather
EG can be found. In consequence, it can be deduced that the con- small with respect to keff. This is caused by the almost stagnant
vective heat transfer resistance is the limiting factor for the flow behavior of nanoparticles in the fluid. These findings valid
enhancement of the effective thermal conductivity of nanofluids for nanofluids with spherical particles are in contradiction to the
and may not be neglected in corresponding models. widely spread opinion in the literature [8–10] that Brownian con-
For non-spherical particles, the value for Rp,conv/Rp,cond is smaller vection is mainly responsible for the enhancement of the effective
than for spherical particles at a given particle volume, particle vol- thermal conductivity of nanofluids.
ume fraction, and nanofluid system. While Rp,cond is considered to Fig. 5 shows that the effective thermal conductivity increases
be constant in our model, Rp,conv of non-spherical particles is smal- with increasing u, with increasing slope for increasing u values.
ler than that of spherical particles due to the larger surface area Mainly due to the about eight times larger kbf/kp ratio for Al2O3/
and thus lower sphericity w. From this, it can already be concluded EG compared to TiO2/H2O, enhancement in the effective thermal
here that the effective thermal conductivity of nanofluids with conductivity is stronger for Al2O3/EG for a given particle size. For
non-spherical particles should be larger than that of nanofluids u = 0.25 and dp = 5 nm, a difference in the enhancement of about
with spherical particles with equal particle volume. More details 11% is found for the two nanofluids. For all the systems studied,
will be given later on. keff/kbf decreases with increasing particle size. This can be attribu-
In Fig. 5, the percentage enhancement factor (keff/kbf1) calcu- ted to the decrease in the Re, Pe, and Nu numbers as shown in
lated according to Eq. (24) is shown as a function of the volume Fig. 3. Since Nu d1/2
p approximately holds, the effective thermal
fraction u of spherical particles for the two systems Al2O3/EG and conductivity of the nanofluids does not change significantly for
TiO2/H2O at a temperature of 300 K. As described above, these dp > 25 nm. The influence of temperature on the effective thermal
two systems differ most strongly regarding the ratio kbf/kp, which conductivity enhancement of nanofluids is even less pronounced
allows for a better visualization of the influence of the volume frac- for various u and dp values. The reason for this has been given in
tion, particle diameter, and convection contribution. Regarding the the discussion on the Pe and Nu numbers. For example, considering
influence of convection, the enhancement found on basis of our the system Al2O3/EG containing nanoparticles with dp = 5, 25, and
model (Eq. (24)), which includes the effect of Brownian convection, 50 nm at u = 0.25, the differences in the enhancement factors in
is compared with a ‘‘theoretical” enhancement which does not the temperature range between 283.15 K and 363.15 K are 1.3%,
account for this effect. The latter system would consist of static 0.43%, and 0.30%, respectively.
particles suspended in the liquid, neglecting any thermal resis- To test the reliability of the present model, a comparison with
tance in the boundary layer where heat is transferred from the liq- experimental results seems straightforward. However, the current
uid to the solid particle. In this case, Rp,conv = 0 in Eq. (14) which is situation of experimental data in the literature shows an obscure
equivalent to neglecting the term w/Nu = 1/Nu in Eq. (24). picture of thermal conductivity enhancement for nanofluids in
general [2]. For the system Al2O3/EG at 298 K, for instance, Oh
et al. [22] measured the effective thermal conductivity of nanoflu-
ids containing spherical nanoparticles with a diameter of 45 nm by
using a 3x method with an uncertainty of 2% and obtained an
enhancement of about 7.5% with respect to the thermal conductiv-
ity at u = 0.03. In contrast, the measurement results of Xie et al.
[23] from a transient short hot wire method specified with an
uncertainty of less than 0.5% show an enhancement of about 27%
for the same system and particle volume fraction, only using smal-
ler spherical particles with a diameter of 26 nm. The enhancement
of 9.0% predicted by the Hamilton–Crosser model [12] agrees with
the result of Oh et al. [22] within their given uncertainty. Given this
data discrepancy, we preferred to check our model by comparing
with other common models in the literature, where the effective
medium model of Hamilton and Crosser [12] is considered to be
one of the most reliable ones [2].
At first, nanofluids containing spherical particles are investi-
gated. In Fig. 6, the enhancement of the thermal conductivity
(keff/kbf 1) predicted from Eq. (24) is given as a function of the
volume fraction u for all four nanofluids at a particle diameter of
dp = 25 nm and a temperature of T = 300 K. In addition to our
calculations, we also applied the continuum model of Hamilton
Fig. 5. Percentage enhancement factor 100 (keff/kbf 1) on the basis of Eq. (24) as and Crosser [12] given by Eq. (4) and the empirical model of
a function of the volume fraction u for different diameters dp of spherical particles Lu and Lin [13] according to Eq. (6) with the reported values for
at T = 300 K for the nanofluids Al2O3/EG and TiO2/H2O. a and b for the cases kp/kbf = 10 as well as kp/kbf ? 1.
538 K.N. Shukla et al. / International Journal of Heat and Mass Transfer 99 (2016) 532–540
Fig. 6. Percentage enhancement factor 100 (keff/kbf 1) as a function of volume fraction u at a temperature of T = 300 K for the nanofluids (a) Al2O3/H2O, (b) Al2O3/EG, (c)
TiO2/H2O, and (d) TiO2/EG containing spherical nanoparticles calculated from the present model (Eq. (24), dp = 25 nm), the Hamilton-Crosser model [12] (Eq. (4)), and the
Lu-Lin model [13] (Eq. (6) for the ratios kp/kbf = 10 and kp/kbf ? 1).
For all the nanofluid systems tested, very good agreement Al2O3/EG system with kp/kbf = 159.1 and their model for
between our model and the continuum model of Hamilton and kp/kbf ? 1. In conclusion, the very good agreement of the
Crosser [12] for various particle volume fractions is found. Regard- established model of Hamilton and Crosser [12] as well as other
ing the enhancement factors, the relative deviations between the empirical models [13] with our model indicates that the convective
continuum model and ours are less than 8% for volume fractions heat transfer caused by the Brownian motion of the nanoparticles
between 0 and 0.25 for the studied conditions. Also for varied tem- needs to be considered for the heat transfer in nanofluids.
peratures and particle diameters, this deviation is not exceeded Further evidence for this can be given by the investigation of
due to the very weak influences of T and dp on keff/kbf in our model nanofluids with non-spherical particles. In Fig. 7, the enhancement
and the fact that the Hamilton–Crosser model [12] also shows only of the thermal conductivity (keff/kbf 1) modeled according to our
very weak temperature dependence and depends on the particle prediction from Eq. (24) is exemplarily shown as a function of the
diameter. While our model provides lower values than the contin- sphericity of the particle w for the nanofluid Al2O3/H2O containing
uum model for low volume fractions, there is crossover for particle particles with dp = dp,eq = 30 nm at a temperature of T = 300 K and
volume fractions that seems to depend on the kp/kbf value of the volume fractions u of 0.05, 0.10, 0.15, and 0.20. Spherical particles
nanofluid. The lower this thermal conductivity ratio, the lower is are compared with cubic particles as well as seven cylindrical par-
the u value at which our model exceeds the Hamilton–Crosser ticles with varying aspect ratios, i.e., the ratio of length to diameter,
model [12]. which are specified in Fig. 7. While prolate cylindrical particles
In this context, a comparison of our model with that of Lu and have aspect ratios larger than 1, they are smaller for oblate parti-
Lin [13] provides further information. Their correlations show that cles. A broad range of w values is covered ranging from about
an increasing kp/kbf value results in a larger enhancement of the 0.22 for prolate cylinders with an aspect ratio of 200:1 to 1 for
effective thermal conductivity due to the addition of particles with spheres. To check our modeled data, we use again the continuum
larger thermal conductivity. Our model shows the same trend model of Hamilton and Crosser [12] in its general form given by
when the four nanofluids with different kp/kbf ratios are compared, Eq. (1).
see Fig. 6. While for the TiO2/H2O system with kp/kbf = 19.3 our Also for systems with non-spherical nanoparticles, our modeled
model fits better with the Lu-Lin model [13] for kp/kbf = 10, data and those predicted by Hamilton and Crosser [12] agree well
there is better agreement between our model in the case of the for the various particle geometries. Both models show that
K.N. Shukla et al. / International Journal of Heat and Mass Transfer 99 (2016) 532–540 539
4. Conclusions
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