Advanced Powder Technol., Vol. 18, No. 6, pp.

813824 (2007)
VSP and Society of Powder Technology, Japan 2007.
Also available online - www.brill.nl/apt
Invited paper
Forced convective heat transfer of nanouids
YULONG DING
1,
, HAISHENG CHEN
1,2
, YURONG HE
1
,
ALEXEI LAPKIN
3
, MAHBOUBEH YEGANEH
4
,
LIDIJA ILLER
4
and YURIY V. BUTENKO
4
1
Institute of Particle Science and Engineering, University of Leeds, Leeds LS2 9JT, UK
2
Institute of Engineering Thermophysics, Chinese Academy of Sciences, Beijing, China
3
Department of Chemical Engineering, University of Bath, Bath, UK
4
School of Chemical Engineering and Advanced Materials, University of Newcastle,
Newcastle upon Tyne, UK
Received 8 April 2007; accepted 14 June 2007
AbstractForced convective heat transfer is experimentally investigated using aqueous and ethylene
glycol-based spherical titania nanouids, and aqueous-based titanate nanotubes, carbon nanotubes
and nano-diamond nanouids. These nanouids are formulated from dry nanoparticles and pure
base liquids to eliminate complications due to unknown solution chemistry. All the formulated
nanouids show a higher effective thermal conductivity than that predicted by the conventional
theories. Except for the ethylene glycol-based titania nanouids, all other nanouids are found
to be non-Newtonian. For aqueous-based titania and carbon and titanate nanotube nanouids, the
convective heat transfer coefcient enhancement exceeds, by a large margin, the extent of the thermal
conduction enhancement. However, deterioration of the convective heat transfer is observed for
ethylene glycol-based titania nanouids at low Reynolds numbers and aqueous-based nano-diamond
nanouids. Possible mechanisms for the observed controversy are discussed from both microscopic
and macroscopic viewpoints. The competing effects of particle migration on the thermal boundary
layer thickness and that on the effective thermal conductivity are suggested to be responsible for the
experimental observations.
Keywords: Nanouids; convective heat transfer; thermal conductivity; rheology; mechanisms; heat
transfer enhancement.
1. INTRODUCTION
This work is concerned with forced convective heat transfer of nanouidsheat
transfer between a forced owing nanouid through a conned region and the
conning walls. Forced convective heat transfer plays a signicant role in almost
all industrial sectors. Examples include cooling of microelectronics, process

To whom correspondence should be addressed. E-mail: y.ding@leeds.ac.uk

814 Y. Ding et al.
intensication in the chemical industry, heat exchange/waste heat recovery in power
plants and cooling of car engines, to name but a few.
Despite the industrial importance, only a small number of studies have been
devoted to convective heat transfer, possibly due to the system being less well-
dened. Most of the reported studies show enhancement of convective heat transfer
by using nanouids [19]. A few studies show inconsistencies, i.e. enhancement
under certain conditions but little enhancement under other conditions [1012].
There are also studies that show little or even a decrease in the convective heat
transfer coefcient when nanoparticles are added to the base liquids [13]. This
work aims to understand and interpret the controversies through both experimental
work and simple analyses. Five types of nanouids were formulated, characterized
for their thermal and rheological properties, and measured for their convective
heat transfer coefcient. It will be shown that nanouids can be Newtonian and
non-Newtonian depending on the properties of the base liquid and nanoparticles,
particle concentration, and shear rate. It will also be shown that enhancement of
thermal conduction does not necessarily mean an enhancement in the convective
heat transfer.
2. MATERIALS AND EXPERIMENTAL TECHNIQUES
Four types of nanomaterials, i.e. titania, titanate nanotubes, carbon nanotubes
and nano-diamond particles, were used for nanouid preparation. Titania nanou-
ids were formulated by using dry nanoparticles manufactured (using the aerosol
process) by Degussa (Germany). X-ray diffraction analysis of the nanoparticles
showed they contained predominantly anatase with a small amount of rutile phase.
The primary titania nanoparticles were approximately spherical with an average
diameter of about 20 nm. However, the as-received titania particles were in the
form of large agglomerates. Sonication, high shear homogenization and high shear
medium milling were therefore used in series to break the agglomerates. The carbon
nanotubes were supplied by Professor F. Wei of Tsinghua University (China) and the
details of carbon nanotube nanouid preparation can be found elsewhere [7]. The ti-
tanate nanotubes were synthesized in our labs. The primary titanate nanotubes were
around 10 nm (diameter) 100 nm (length) and their synthesis was based on the
alkali hydrothermal transformation [14]. Nano-diamonds were provided by the Fed-
eral Research and Production Center Altai (Biysk, Russian Federation) and were
additionally boiled in concentrated nitric acid for 60 min to remove metal impurities
and non-diamond forms of carbon [15]. The primary nano-diamond particles were
around 250 nm in diameter and were produced by the so-called detonation method.
Nano-diamond particles and titanate nanotubes were found to be in the form of ag-
glomerates so de-agglomeration was performed using the high shear homogenizer.
Distilled water was used as the base liquid for formulating most of the nanouids,
whereas a few titania nanouids were made with ethylene glycol. No stabilizer
was used for titania, and titanate and carbon nanotubes nanouids. Stabilization
Forced convective heat transfer of nanouids 815
of aqueous nanouids was achieved by adjusting pH. Great difculties were
experienced in stabilizing nano-diamond nanouids by using pH control, so a
small amount of SDBS surfactant was employed (10 wt% with respect to particle
concentration). The formulated titania, and titanate and carbon nanotube nanouids
were found to be stable for a fairly long period of time before any signicant
sedimentation was visually observed. Despite the use of a small amount of SDBS,
signicant sedimentation was observed in the nano-diamond nanouids after a few
hours. The period of stability was sufcient for thermal conductivity and rheological
measurements, and for convective heat transfer experiments.
The formulated nanouids were rst characterized for their physical, thermal and
rheological properties. A Malvern nanosizer (Malvern Instrument, UK) was used to
measure the particle size distribution of nanouids except for carbon nanotubes,
for which scanning and transmission electron microscopy were used [7]. The
results showed that the average particle (agglomerate) size was around 120 nm
almost independent of particle concentration, indicating that the method used above
was not able to break the agglomerates into primary nanoparticles. The thermal
conductivity of the prepared nanouids was measured by using a KD2 thermal
property meter (Labcell, UK), which provided an uncertainty within around 3%.
The viscosity of nanouids was measured by using a Bohlin CVO rheometer with a
Mooney cell (Malvern Instruments).
The experimental system for measuring the convective heat transfer coefcient is
shown schematically in Fig. 1. The details have been reported elsewhere [9]. In
brief, it consisted of a ow loop, a heating unit, a cooling unit, and a measuring and
control unit. The ow loop included a pump with a built-in owmeter, a nanouid
tank, a collection tank, a test section and various valves. The test section was a
vertically oriented straight copper tube (1834 mm length, 3.97 mm inner diameter
and 6.35 mm outer diameter). The tube was heated by exible silicon rubber heaters
(Watlow, UK) linked to a DC power supply (TTi Ex752m; RS, UK). The power
supply was adjustable and had a maximum power supply rating of 300 W. There
was a thick thermal isolating layer surrounding the heaters to obtain a constant heat
ux condition along the test section. Eight T-type thermocouples were mounted
on the test section at the normalized axial positions with respect to the tube inner
diameter of around 50.4 (T1), 151.2 (T2), 201.6 (T3), 252.0 (T4), 302.4 (T5), 352.8
(T6), 403.2 (T7) and 453.6 (T8) from the inlet of the test section to measure the
wall temperature distribution. Two further T-type thermocouples were inserted into
the ow at the inlet and exit of the test section to measure the bulk temperatures
of nanouids. In the heat transfer experiments, the pump rotational rate, voltage
and current of the DC power supply were recorded, and the temperature readings
from the 10 thermocouples were registered by a data requisition system (National
Instrument, UK). The experimental system gave an uncertainty of nanouids heat
transfer measurements of about 6.5%.
816 Y. Ding et al.
Figure 1. Experimental system for convective heat transfer experiments.
3. EXPERIMENTAL RESULTS AND DISCUSSION
3.1. Thermal conductivity of nanouids
Thermal conductivity measurements were carried out for all nanouids formulated.
The following observations are obtained. (i) For a given type of nanouid, the effec-
tive thermal conductivity increases with increasing nanoparticle concentration and
the increase is generally a non-linear function of concentration. (ii) The thermal
conductivity increases with increasing temperature and the enhancement is a non-
linear function of temperature. (iii) Given particle concentration, the measured ther-
mal conductivities in the descending order are watercarbon nanotube nanouids,
waterdiamond nanouids, watertitanate nanouids, watertitania nanouids and
ethylene glycoltitania nanouids. For example for 0.1 wt% nanouids at 30

C,
the enhancements of these nanouids are 18%, 8%, 4%, 3 and 2%, respectively.
This indicates strong effects of particle shape and material properties, although
this comparison is rather crude (as solution chemistry and particle size, etc., are
not taken into account). Note that the last two gures (3 and 2%) are also within
the uncertainty of the measurements, although each data point is an average over
at least ve measurements. (iv) The conventional HamiltonCrosser model with
shape factor correction does not provide an adequate prediction of the experiments
in two aspects, i.e. the predicted thermal conductivity is lower than the measured
values, and prediction shows linear concentration and temperature dependence. It
is important to note that current method of comparing the effective thermal con-
ductivity of different nanouids in terms of particle concentration and/or tempera-
Forced convective heat transfer of nanouids 817
ture can be misleading because the effective thermal conductivity of nanouids is
also likely to be a function of primary particle size, particle shape and aggregate
size (often controlled by the solution chemistry and nanouid formulation process),
apart from temperature and concentration. In this sense, collaborations between
colloid chemists and thermophysicists would be a good way to attack the prob-
lem.
3.2. Rheological behavior of nanouids
Rheological measurements were performed on all nanouids. The results reveal the
following. (i) Nanouids can exhibit either or both Newtonian and non-Newtonian
behavior depending on particle size, particle shape, base liquid properties, solution
chemistry, particle concentration, shear rate, etc. (ii) Aqueous-based nanouids of
carbon nanotubes, titania, titanate and nano-diamond are non-Newtonian, whereas
the ethylene glycol based titania nanouids are Newtonian. (iii) Aqueous-based
nanouids of carbon nanotubes, titania and titanate show the shear thinning behav-
ior, whereas the aqueous-based nano-diamond nanouids exhibit shear thinning at
lowshear rates, Newtonian or weak shear thickening behavior at medium shear rates
and shear thickening at high shear rates (Fig. 2). As will be seen later, such unusual
behavior has an implication for its convective heat transfer behavior although the
mechanism remains a subject of further investigation. (iv) Given the shear rate, the
shear viscosity decreases with increasing temperature, decreasing particle concen-
tration or decreasing particle size. (v) Given other conditions, the shear viscosity of
Figure 2. Rheological behavior of nano-diamond nanouids at six temperatures (0.1 wt%, 0.01%
SDBS surfactant). This gure is published in color on http://www.ingenta.com
818 Y. Ding et al.
nanouids containing non-spherical particles is higher than those containing spher-
ical nanoparticles.
As the viscosity of nanouids at low shear rates reects the structuring of
nanoparticles in the base liquid, it also affects the effective thermal conductivity.
It may be possible to establishing a relationship between the low shear viscosity
and the effective thermal conductivity. Work is underway to address this.
3.3. Convective heat transfer of nanouids
Experiments on convective heat transfer were carried out on all the nanouids
formulated under various ow conditions. Pure base liquids were tested rst as the
base for comparison before nanouids were tested. The results can be summarized
as follows.
(i) The convective heat transfer coefcient of nanouids has the highest value
at the entrance, but decreases with axial distance and reaches a constant value in
the fully developed region. The entrance length depends on the properties and
behavior of nanouids. For a given nanouid, the entrance length at low ow rates,
e.g. laminar ow for Newtonian uids, is longer than that at high ow rates, e.g.
turbulent ow for Newtonian uids.
(ii) Given particle concentration and ow conditions, aqueous-based carbon
nanotube nanouids give the highest enhancement of convective heat transfer
coefcient, followed by (in descending order) aqueous-based titanate nanouids and
aqueous-based titania nanouids. The ethylene glycol-based titania nanouids and
aqueous-based nano-diamond nanouids are found to give virtually no enhancement
(Figs 3 and 4).
(iii) For aqueous based titania, and titanate and carbon nanotube nanouids,
the convective heat transfer coefcient generally increases with increasing ow
rate or increasing particle concentration and the enhancement exceeds by a large
margin the extent of the thermal conduction enhancement, indicating that different
mechanisms are operating. However, if one takes into account the enhancement of
the thermal conductivity, deterioration of the convective heat transfer is apparent
for the ethylene glycol-based titania and aquesous-based nano-diamond nanouids.
The exact reasons for this are a subject of our current investigation. However, for
aqueous-based nano-diamond nanouids, the use of SDBS surfactant creates some
foam. The foam could migrate to the wall region due to its surface activity, thus
prevents effective heat transfer [16]. Another reason for the convective heat transfer
deterioration of nano-diamond nanouids is their shear rheological behavior as
mentioned above. Quantitative understanding of these is currently underway and
the results will be reported later. The deterioration of ethylene glycol-based titania
nanouids is very interesting. It is believed to be associated with the high viscosity
of the base liquid (see below for more discussion). Another possible reason is
that the enhancement is within the error bars of the measurement system as the
thermal conductivity enhancement is small and the relatively large uncertainty of
Forced convective heat transfer of nanouids 819
Figure 3. Convective heat transfer coefcient of nano-diamond-based nanouids (0.1 wt%).
Figure 4. Ethylene-based titania nanouids (Reynolds number = 135).
the convective heat transfer measurements. It is noted that the work on ethylene
glycol nanouids was only carried out at low Reynolds numbers. The results thus
obtained may not apply to other conditions.
(iv) The data for the aqueous-based titania and titanate nanouids seem to in-
dicate that particle shape plays an important role in the convective heat transfer
enhancement given other conditions, i.e. large aspect ratios give a higher enhance-
820 Y. Ding et al.
ment. This is also supported by comparing the results of this work on carbon nan-
otube nanouids with those by Yang et al. [13] on disk-like graphite nanouids.
(v) There seems to be a relationship between the rheological behavior and
convective heat transfer behavior. For example, for aqueous-based carbon nanotube
nanouids, a drastic increase in the convective heat transfer coefcient occurs at
a ow rate corresponding to a shear rate where shear viscosity is close to the
lowest [7].
4. MECHANISMS OF ENHANCEMENT OF CONVECTIVE HEAT TRANSFER
The mechanisms of the enhanced convective heat transfer can be looked at from
both macroscopic and microscopic aspects. Considering a ow with uniform
velocity and temperature distributions through a pipe, the ow has a different
temperature from the wall temperature (Fig. 5). Due to friction between the uid
and the pipe wall, a hydrodynamic boundary layer will form at the wall region
in which the ow velocity increases from zero at the wall to maximum in a
radial position depending on the axial position from the entrance. At a certain
axial position from the entrance, the thickness of the boundary layer approaches
a constant value and the ow is regarded as fully developed. Similarly, due
to the different temperature of the uid from the pipe wall, a thermal boundary
layer is developed, although its thickness and the entrance length can be different.
Macroscopically, the forced convective heat transfer coefcient, h, is given by
h = k/
t
, where
t
is the local thickness of the thermal boundary layer and k is the
local effective thermal conductivity of nanouids adjacent to the wall surface. This
simple expression indicates that either or both of an increase in k and a decrease in
t
could result in an increase in the convective heat transfer coefcient. This explains
why the entrance region gives a higher convective heat transfer coefcient. As
nanouids have a higher thermal conductivity in comparison with the base liquid,
the simple expression also partially explains the enhanced convective heat transfer
Figure 5. Boundary layer development in a pipe ow in the laminar ow regime; for turbulent ow,
the entrance region is much shorter and the boundary layer thickness is thinner.
Forced convective heat transfer of nanouids 821
coefcient. The expression, however, cannot provide an adequate explanation
to the experimental observations that, in some cases the convective heat transfer
coefcient enhancement is much higher than the thermal conduction enhancement,
while in other cases, there is no convective heat transfer enhancement despite
considerable thermal conduction enhancement. Before a detailed discussion on
the apparent controversy, a point is made below on the view of nanouids being
homogeneous. There are a number of publications stating that nanouids are
homogenous and can be considered as single-phase uid; as a result, a number
of people even model nanouids based on this statement (e.g. Ref. [17]). Let
us rst accept the statement, then the convective heat transfer coefcient for a
fully developed pipe ow under constant wall heat ux conditions should take the
following form:
h = 4.26k/D, (1)
where D is the pipe diameter. Given D, (1) suggests that h is only a function
of k. This is in disagreement with experimental observations; see Section 2 and
Refs [3, 5, 13]. Let us look more closely at the entrance region. If nanouids
were homogeneous, the entrance region length should follow the expression for
the ow of single-phase ows. This is again in contradiction to the experimental
observations [5, 7, 9, 12]. For homogenous uids owing through a pipe with a
constant wall heat ux, the heat transfer coefcient for fully developed turbulent
ows is give by:
h = 0.023

0.8
U
0.8
C
0.33
p
D
0.2

k
0.67

0.47

, (2)
where U is the average ow velocity, C
p
is the heat capacity, is the uid density
and is the uid viscosity. Due to low particle concentrations of nanouids, the
heat capacity and density of nanouids are expected to be similar to those of the base
liquids. If nanouids were homogenous, then the convective heat transfer coefcient
would be proportional to (k
0.67
/
0.47
). This implies that the enhancement under the
turbulent ow conditions is much lower than that under the laminar ow conditions.
This again disagrees with the experimental observations [4, 9]. These arguments
suggest that nanouids are likely to be inhomogeneous during ow at least in some
cases. In the following, possible reasons for the inhomogeneity and the implications
for convective heat transfer are discussed.
Microscopically, there are at least two possible reasons for the inhomogeneity.
One is the presence of agglomerates in nanouids, which can be associated with
either sintering during nanoparticle manufacturing or solution chemistry during
nanouid formulation. The former is often seen in processes involving elevated
temperatures, e.g. aerosol reactors. The resulting agglomerates are very strong, and
are difcult to break down to primary nanoparticles even with prolonged high shear
processing and ultrasonication. The latter is due to attraction between nanoparticles,
e.g. van der Waals attractive force, and depletion phenomena. The agglomerates
822 Y. Ding et al.
(aggregates) can be controlled by adjusting solution chemistry and applying shear.
At this point, a revised denition of nanouids is proposed here as dilute liquid
suspensions of particles with at least one critical dimension smaller than around
100 nm. This denition includes suspensions containing nanoparticle agglomerates
which have been shown both theoretically and experimentally to be responsible
for the observed thermal conduction enhancement [18, 19]. The second reason is
particle migration due to viscosity and velocity gradients. Experimental evidence
of particle migration is the longer entrance length of nanouids as discussed in the
Section 2 and in a recent experimental study by Merhi et al. [20]. There are also
plenty of theoretical studies on particle migration (e.g. Refs [2123]). If particles
are very small, Brownian motion is dominant and the effect of the above-mentioned
particle migration is negligible. If particles are large, e.g. aggregates of hundreds
of nanometers, the contribution of the Brownian motion is small and a particle
depletion region may exist at the wall, which gives non-uniform distributions of
particle concentration, viscosity and thermal conductivity. The direct results of
particle migration are lower particle concentration at the wall region and a thinner
boundary thickness due to disturbance by the moving particles. This, according to
h = k/
t
, can lead to three possible results: (i) h is enhanced if the decrease in
t
exceeds the decrease in k, (ii) h does not change if the decrease in
t
is equal to the
decrease in k and (iii) h is reduced if the decrease in
t
is lower than the decrease
in k. This qualitatively explains the experimental results. However, quantitative
explanation requires understanding of how nanoparticles behave under shear, and
how they interact with each other and with uid in the boundary layer.
5. CONCLUDING REMARKS
Nanouids are dened as dilute suspensions of particles with at least one critical
dimension smaller than around 100 nm. A considerable amount of effort has been
put in to understanding the enhancement of thermal conductivity of nanouids
over the past decade, which has led to a conclusion that nanoparticle clustering
(structuring) is likely to be the dominant mechanism [19]. However, less effort has
been put in to the other aspects of nanouids such as natural and forced convective
heat transfer and boiling heat transfer, although the number of publications on these
aspects is on the increase.
This work is concerned with forced convective heat transfer, which is much
more complicated than thermal conduction in microscopically static conditions
due to the involvement of uid hydrodynamics, macroscopic motion of particles
and nanouidwall interactions. The complication is demonstrated experimentally
in this work; nanouids with an enhanced thermal conductivity do not guarantee
an enhancement in the convective heat transfer. The exact reason for this is not
fully clear, but particle migration could be a major factor responsible for the
experimental observations. Such a hypothesis requires validation, which can be
Forced convective heat transfer of nanouids 823
done experimentally, theoretically or even through mathematical modeling. Work
is underway to address this aspect.
Acknowledgments
The work is supported nancially by UK EPSRC under grants EP/D000645/1 and
EP/EP/E00041X/1. H. C. wishes to thank the Chinese Academy of Sciences for
a visiting fellowship. Y. V. B. is grateful to the European Communitys Sixth
Framework Programme for a Marie Curie Incoming International Fellowship under
grant MIF1-CT-2005-021528.
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