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Applied Energy 135 (2014) 548559

Contents lists available at ScienceDirect

Applied Energy
journal homepage: www.elsevier.com/locate/apenergy

Heat transfer performance and transport properties of ZnOethylene


glycol and ZnOethylene glycolwater nanouid coolants
K.S. Suganthi, V. Leela Vinodhan, K.S. Rajan
Centre for Nanotechnology & Advanced Biomaterials (CeNTAB), School of Chemical & Biotechnology, SASTRA University, Thanjavur 613401, India

h i g h l i g h t s
 High thermal conductivity and low-viscous ZnOethylene glycol nanouids prepared.
 ZnOethylene glycolwater nanouids prepared by hierarchical method.
 Liquid layering and Brownian motion contribute to thermal conductivity enhancement.
 Improvement in nanouid cooling performance inline with thermal conductivity rise.

a r t i c l e

i n f o

Article history:
Received 20 May 2014
Received in revised form 14 August 2014
Accepted 5 September 2014
Available online 26 September 2014
Keywords:
ZnOethylene glycol
ZnOethylene glycolwater
Transient heat transfer
Nanouid
Liquid layering
Heat transfer rate ratio

a b s t r a c t
Experiments were carried out on preparation and characterization of ZnOethylene glycol (EG) and ZnO
ethylene glycolwater nanouids and analysis of their performance as coolants. Favorable interactions
between ZnO nanoparticles and ethylene glycol molecules ensured superior transport properties of
ZnOEG nanouids. These interactions were utilized during formulation of ZnOEGwater nanouids
with preservation of ethylene glycol molecules over ZnO nanoparticles surface rendering them with better transport properties. ZnOEG nanouids containing 4 vol.% nanoparticles showed thermal conductivity enhancement of 33.4% and viscosity reduction of 39.2% at 27 C. Similarly, 2 vol.% ZnOEGwater
nanouids showed thermal conductivity enhancement of 17.26% and viscosity reduction of 17.34% at
27 C. Disturbance of hydrogen bonding network of ethylene glycol by ZnO nanoparticles resulted in
reduced dispersion viscosity. Empirical models were developed to predict the thermal conductivity
enhancement and viscosity reduction of the nanouids apart from elucidating mechanisms for the same.
Transient heat transfer experiments showed that ZnOEG and ZnOEGwater nanouids had better heat
absorption characteristics compared to their respective base uids. The enhancements in heat transfer
were proportional to thermal conductivity enhancements, which showed that superior thermal conductivity of nanouids could be harnessed for cooling applications.
2014 Elsevier Ltd. All rights reserved.

1. Introduction
Thermal management and energy storage systems are thrust
areas of research in elds such as automobile/industrial cooling,
renewable energy utilization as evident from the recent literature
[111]. Maintenance of ideal working temperature by removing
the heat dissipated is essential for proper functioning of high speed
engines, microprocessors, etc. This has become a great challenge
due to increasing thermal loads driven by technological advancements. The strategies to improve efciency of heat transfer systems include active modes (increasing coolant velocity, use of
coolants with higher thermal conductivity) and passive modes

Corresponding author. Tel.: +91 9790377951; fax: +91 4362 264120.


E-mail address: ksrajan@chem.sastra.edu (K.S. Rajan).
http://dx.doi.org/10.1016/j.apenergy.2014.09.023
0306-2619/ 2014 Elsevier Ltd. All rights reserved.

(use of ns, channels with expansions and constrictions, higher


heat transfer area). Thermal conductivity of liquids (0.1 < kl
< 10 W/mK) lies between that of insulators and non-metallic solids. It is possible to tailor the thermophysical properties like thermal conductivity and viscosity through use of nanoparticle
dispersions. Nanouid, colloidal dispersion of solid nanoparticles
in liquid [12] belongs to a new class of coolants on which extensive
research has been carried out over the past two decades.
Research on nanouids has been extended towards exploring
the inuence of different kinds of nanomaterials like metal
[1317], metal oxide [1727], carbon nanotubes [2831], graphene
[32,33], etc. on the important transport properties: thermal conductivity and viscosity. The factors that greatly affect transport
properties of nanouids include morphology of nanomaterials
[18,29,3436], dispersion quality [3740] and the method of
preparation [4144].

K.S. Suganthi et al. / Applied Energy 135 (2014) 548559

549

Nomenclature
Symbol
a, b, c
cp
k
m
Q
T
t
Uf
Uxj
x
y

Meaning
coefcients in Eq. (14)
specic heat (J/kg K)
thermal conductivity (W/mK)
mass (kg)
amount of heat transferred (W)
temperature (C)
time (s)
uncertainty associated with the measurement of parameter f
uncertainty in the measurement of variable Xj
function of nanoparticle concentration
function of nanoparticle concentration and temperature

It is challenging to achieve higher thermal conductivity and


lower viscosity simultaneously in nanouids. Introduction of solid
nanoparticles in liquids will eventually increase thermal conductivity [4547] as well as viscosity and hence higher pumping power
[43,45]. However, we have recently demonstrated the preparation
of metal oxide (MOx)propylene glycol (PG) nanouids with lower
viscosity and higher thermal conductivity than pure propylene glycol [24,40,48]. Favorable interactions between metal oxide nanoparticles and propylene glycol molecules led to lower viscosity of
MOxPG nanouids. This makes the MOxPG nanouids as excellent prospects for cooling applications. These research ndings
motivated us to investigate transport properties of ethylene glycol
based nanouids, since ethylene glycol (EG) is chemically similar to
propylene glycol having hydrogen bonding networks.
The properties of ethylene glycol based nanouids have been
widely studied [39,4956] due to their use as coolants in automobiles. Sandethylene glycolwater dispersions prepared using stirred bead milling and ultrasonication showed thermal conductivity
enhancement of above 20% at a particle concentration of 1.8 vol.%
[50]. Single-walled CNT inclusions were dispersed in ethylene glycol using bile salt as dispersant and at 0.2 vol.% of nanotube loading, thermal conductivity increased up to 14.8% [53]. Thermal
conductivity of Al2O3ethylene glycol nanouids have been studied over a wide temperature range (298411 K) using a liquid
metal transient hot wire apparatus [49]. Viscosities of CuOEG
water mixture nanouids have been studied over a temperature
range of 35 to 50 C [52]. The dispersions showed Newtonian
ow behavior over the temperature range investigated [52].
ZnOethylene glycol nanouids containing 5 vol.% of nanoparticles, prepared by 3-h ultrasonication yielded thermal conductivity
enhancement of 26.5% [51]. These nanouids were non-Newtonian
(shear-thinning) at higher concentrations and Newtonian at lower
concentrations [51]. Kole and Dey [39] prepared ZnOEG nanouids by extended ultrasonication and the optimum ultrasonication
time was found to be 60 h. Approximately 40% enhancement in
thermal conductivity of ZnOEG nanouids was reported for particle volume concentration of 3.75 vol.% [39].
Understanding the mechanism of interaction between nanomaterials and base uid molecules could lead to nanouid formulation methods, which result in well dispersed nanouids. In our
earlier work [44], one such formulation method was reported
which resulted in nanouids with improved transport properties.
Surfactant-free ZnOpropylene glycol nanouids prepared using
ultrasonication had higher thermal conductivity [57] and lower
viscosity compared to those of propylene glycol [48]. Formation
of propylene glycol molecular layers over ZnO nanoparticles in
ZnOpropylene glycol nanouids was found to be responsible for
higher thermal conductivity, while the disturbance to hydrogen

A, B
N

functions of nanoparticle concentration


number of factors in Eq. (1)

Greek symbols
/
nanoparticle volume concentration
l
viscosity (mPa s)
q
density (kg/m3)
Subscripts
bf
base uid
nf
nanouid
r
relative/ratio

bonding network of propylene glycol contributed to lowering of


their viscosity in comparison to that of pure propylene glycol. Thus,
a coolant with higher thermal conductivity and lower viscosity was
prepared and the underlying mechanisms were understood
[48,57]. With these ndings, a new method of formulation of
ZnOPGwater nanouids was developed in which, water was
commixed with ZnOPG dispersion instead of dispersing ZnO
nanoparticles in PGwater mixture using the conventional
method. This method aided in preservation of propylene glycol
molecular layers over ZnO nanoparticles and foreclosed the interaction of ZnO nanoparticles and water molecules. The proposed
method allowed preparation of ZnOPGwater nanouids without
any surfactants and with better transport properties [44]. However, viscosity reduction of ethylene glycol based nanouids has
not been evidenced in literature thus far.
In this work, ZnOethylene glycol (EG) nanouids were
prepared using ultrasonication without using any surfactant.
ZnOEGwater nanouids were prepared using the method similar
to that proposed in our earlier work [44]. Transport properties of
ZnOEG and ZnOEGwater nanouids were studied as a function
of temperature and nanoparticle volume concentration. Models
have been developed to predict the viscosity and thermal conductivity of ZnOEG nanouids and ZnOEGwater nanouids. These
nanouids have been tested for their cooling performance under
transient conditions.
2. Materials and methods
2.1. Materials
Zinc nitrate hexahydrate, ammonium carbonate, ethylene
glycol were procured from Merck, India. All the chemicals were
used as procured without any purication.
2.2. Synthesis and characterization of ZnO nanoparticles
ZnO nanoparticles were synthesized using chemical precipitation method using Zinc nitrate hexahydrate as precursor at room
temperature [58,59]. Ammonium carbonate has been used as
reducing agent in the synthesis procedure described in our earlier
work [59]. Morphology and crystallographic patterns of the
synthesized ZnO nanoparticles were examined using scanning
electron microscopy (JSM 6701F, JEOL, Japan) and powder X-ray
diffractometry (D8 Focus, Bruker, Germany).
2.3. Formulation of nanouids
ZnOEG nanouid of concentration 4 vol.% was prepared by dispersing the synthesized ZnO nanoparticles in ethylene glycol by

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K.S. Suganthi et al. / Applied Energy 135 (2014) 548559

ultrasonication (Vibracell, Sonics, USA). Ultrasonication (130 W,


20 kHz) was carried out until ZnOEG dispersion attained maximum thermal conductivity and minimum viscosity. Viscosity and
thermal conductivity of ZnOEG dispersions were measured at regular intervals of time during ultrasonication. ZnOEG dispersions
of different volume fractions were prepared by diluting 4 vol.%
ZnOEG nanouids with required volume of ethylene glycol.
A hierarchical method demonstrated in our earlier work [44]
has been utilized for the preparation of 2 vol.% ZnOEGwater
nanouids by mixing water with 4 vol.% of ZnOEG in equal volumes. The prepared nanouids thus had a base uid composition
of 50 vol.% water and 50 vol.% ethylene glycol. Different concentrations of ZnOEGwater nanouids were prepared by further diluting 2 vol.% ZnOEGwater nanouids with 5050 vol.% ethylene
glycolwater mixture.
2.4. Characterization of nanouids
Transport properties like viscosity and thermal conductivity
were studied for the ZnOEG and ZnOEGwater nanouids as a
function of temperature and nanoparticle volume fraction. Thermal
conductivity of nanouids was measured using transient-hot wire
method (Decagon devices, USA). KS-1 probe has been used for measurements. Temperature of the sample was maintained using a circulating water bath (TC-502, Brookeld Engineering, USA).
Viscosities of nanouids were measured using a rotational viscometer (LVDV-II + Pro, Brookeld Engineering, USA). S18 and
S64 spindles were used for ZnOEG at higher (27140 C) and
lower temperatures (1020 C) respectively. S00 spindle was used
for ZnOEGwater nanouids over the entire temperature range
investigated. During the viscosity measurements, temperature of
the ZnOEG nanouids and ZnOEGwater nanouids were maintained using a temperature controller (Thermosel, Brookeld
Engineering, USA) and constant temperature bath (TC-502, Brookeld Engineering, USA). Hydrodynamic particle size distribution of
ZnOEG dispersions was measured using dynamic light scattering
technique (NanoZS, Malvern instruments, UK) as a function of
ultrasonication time.
Thermal conductivity, viscosity and hydrodynamic size distribution measurements were repeated at least three times to ascertain
the repeatability and reproducibility of measurements. Uncertainties in viscosity, thermal conductivity and average hydrodynamic
size have been shown in the graphs as standard deviations.
Coefcients of variation during thermal conductivity and viscosity
measurements for the standards provided by the respective manufacturer were 0.25% and 0.77% respectively. Maximum coefcient
of variation in thermal conductivity and viscosity measurement of
nanouids and base uids were 0.87% and 1.76% respectively.
Total uncertainty in the measurement of a parameter was
calculated taking into account of the random error only, as the systematic error was negligible compared to random error. Uncertainties in relative viscosity, thermal conductivity ratio and heat
transfer ratio were calculated using the following formula [60]
and have been expressed as standard deviation.

" 
2 #0:5
N
X
@f
Uf 
U xj
@xj
j1

2.5. Heat transfer experiments


In order to compare the performance of nanouids as coolants
in relation to their base uids, transient heat transfer experiments
were carried out using nanouids and base uids. The experimental setup (Fig. 1) comprised a stainless steel sample reservoir,
electrical heating coil connected to AC power supply and a

Fig. 1. Schematic representation of the experimental setup used for heat transfer
experiments.

temperature sensor connected to data logger. In order to maintain


constant heat ux boundary condition, test section was heated by
supplying constant AC power through the heating lament wound
over the test section, which was subsequently insulated. In a typical experiment, the test section was lled with a constant volume
of test uid. A constant voltage of 10 V was supplied. Temperature
increase of test uid was measured as a function of time for about
1020 min. The test uids studied were: 1.5 vol.% ZnOEG, 1 vol.%
ZnOEG, 0.25 vol.% ZnOEG, and EG and 2 vol.% ZnOEGwater,
1.5 vol.% ZnOEGwater, 0.5 vol.% ZnOEGwater and EGwater.
3. Results and discussion
ZnO nanoparticles used in this study had uniform spherical
morphology with a size range of 2540 nm (Fig. 2a). Highly crystalline nature of the ZnO nanoparticles synthesized through chemical
precipitation method was evident from the X-ray diffraction pattern (Fig. 2b), which are in accordance with those for hexagonal
wurtzite phase (JCPDS No. 89-1397).
As evident from the scanning electron micrograph, synthesized
ZnO nanoparticles prevail in slightly agglomerated state. Nanouids with high dispersion quality are known to have superior
transport properties [55,61,62]. The advantages of well dispersed
nanouids to be used as coolants are (i) higher surface area for heat
transfer, (ii) lower viscosity and lesser pumping power, and (iii)
good colloidal stability due to the smaller size of aggregates [46].
Ultrasonication plays a critical role in the formulation of nanouids by assisting in breakage of aggregates resulting in high quality dispersions. However, there exists an optimum ultrasonication
time in the preparation of nanouids [24,40,48,61,62]. In case of
extending ultrasonication beyond the optimum ultrasonication
time, re-aggregation may occur leading to formation of larger
aggregates resulting in instability of the nanouids [59]. Other
than the physical and chemical properties of the dispersed phase
of nanouids, dispersion characteristics have signicant inuence
on thermal conductivity, viscosity and stability of nanouids.
Hence, it is pertinent to determine optimum ultrasonication
energy (or) time required to prepare nanouids with superior dispersion characteristics, evidenced in terms of increased thermal
conductivity and reduced viscosity.
Fig. 3a shows the inuence of ultrasonication time on thermal
conductivity and viscosity of 4 vol.% ZnOEG nanouid. Thermal
conductivity of ZnOEG nanouid (4 vol.%) gradually increased
with increasing ultrasonication time and saturated at about 30 h.
Also, viscosity of the dispersion decreased with increasing

K.S. Suganthi et al. / Applied Energy 135 (2014) 548559

Fig. 2. (a) Scanning electron micrograph of synthesized ZnO nanoparticles and (b)
X-ray diffraction pattern of ZnO nanoparticles.

sonication time. Fig. 3b shows the inuence of ultrasonication time


on the average hydrodynamic diameter of the ZnOEG dispersion,
from which it is evident that the average hydrodynamic diameter
decreased with ultrasonication time.
As ultrasonication time increased, larger aggregates of ZnO
nanoparticles had been broken up into smaller aggregates
(Fig. 3b). Formation of smaller aggregates resulted in increase in
the fraction of heat conducting paths and decrease in the fraction
of continuous phase with relatively higher thermal resistance. In
other words, size reduction of aggregates or dispersion of nanoparticles resulted in increased surface area which resulted in increase
in thermal conductivity. As ZnOEG dispersion was ultrasonicated,
larger aggregates were broken up progressively and hence the persistent increase in thermal conductivity. At about 30 h, saturation
in thermal conductivity increase was observed showing that nanoparticles/clusters were well dispersed.
Aggregate sizes in solidliquid dispersions have profound inuence on their viscosity. Greater the ratio of aggregate size to primary particle size, higher is the resistance to uid ow [59,63]
and hence higher viscosity. As ultrasonic processing progressed,
viscosity decreased (Fig. 3a) probably due to the reduction in the
size of the aggregates.
3.1. Viscosity of dispersions
3.1.1. Inuence of nanoparticle concentration on viscosity
3.1.1.1. ZnOEG dispersions. Viscosities of ZnOEG nanouids were
independent of shear rate over a range of 66238 s1 (Fig. 4a) for
the concentration range investigated (0.254 vol.%). This reveals

551

Fig. 3. Inuence of ultrasonication time on (a) thermal conductivity and viscosity of


4 vol.% ZnOEG nanouids at 27 C and (b) average hydrodynamic diameter of ZnO
nanoparticles in ZnOEG nanouids.

that dispersion of ZnO nanoparticles did not alter the ow behavior


signicantly and nanouids remained to be Newtonian.
Relative viscosity (lr = lnf/lb)ZnO nanoparticle volume concentration relationship of ZnOEG nanouids (Fig. 4b) shows that
relative viscosity of ZnOEG dispersions (averaged over shear rates
in the range 66238 s1) decreased with increasing nanoparticle
loading. Viscosities and relative viscosities of ZnOEG nanouids
showed a contradictive behavior with those reported for other
nanouid systems as well as ZnOEG nanouids in literature. Gallego et al. [64] reported increasing viscosity of ZnOEG nanouids
with increasing nanoparticle concentration. However, those nanouids were prepared by ultrasonication for a time period of 16 min
only, which was much lower compared to the ultrasonication time
used in this study. Yu et al. [51] dispersed ZnO nanoparticles of size
1020 nm in ethylene glycol using ultrasonic processing for 3 h.
ZnOEG dispersions thus prepared had higher viscosities (100%
increase) than base uid and showed shear thinning characteristics
at particle concentrations P3 vol.%. Moosavi et al. [65] observed
26% enhancement in viscosity of ZnOEG nanouids for a very
low particle concentration of 0.6 vol.%, while using ammonium citrate as dispersant. From the nanouid viscosity-ZnO nanoparticle
concentration data of the above [51,64] and the shear-thinning
nature of nanouids in the work of Mossavi et al. [65], it appears
that those nanoparticles exhibited high degree of aggregation.
ZnOEG nanouids prepared by Kole and Dey [39] were ultrasonicated for an optimum ultrasonication time of 60 h and viscosities
of ZnOEG nanouids (63.5 vol.%) were very close to that of base
uid. This was attributed to the well-dispersed nature of ZnO
nanoparticles in ethylene glycol. Hence the disparity observed in

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K.S. Suganthi et al. / Applied Energy 135 (2014) 548559

3.1.1.2. ZnOEGwater nanouids. The inuence of nanoparticle


concentration on relative viscosity of ZnOEGwater nanouids
(Fig. 5) shows decreased viscosities at higher particle concentration. It may be recalled that the ZnOEGwater nanouids were
prepared by addition of water to ZnOethylene glycol dispersion,
which had lower viscosity than ethylene glycol due to disturbance
in hydrogen bonding network. By adding water to ZnOEG dispersion, viscosity reduction has been maintained by preserving ethylene glycol molecular layers over ZnO nanoparticles and thus
avoiding the direct contact of ZnO nanoparticles and water molecules. It is known that the direct contact of surfactant-free ZnO
nanoparticles with water molecules promote their aggregation
[44,59,68] and increase dispersion viscosity. Hence, through prevention of direct contact between surfactant-free ZnO nanoparticles and water and preservation of ZnO nanoparticlesethylene
glycol interactions, 17.34% reduction in viscosity has been obtained
for 2 vol.% ZnOEGwater nanouid. The percentage reduction in
viscosity of 2 vol.% ZnOEGwater nanouids (17%) is comparable
to that of 2 vol.% ZnOEG nanouid (20%).
3.1.2. Inuence of temperature on viscosity
3.1.2.1. ZnOEG nanouids. As coolants, nanouids will be subjected to temperature variations. Hence, it becomes pertinent to
investigate rheological behavior of nanouids under thermal loads.
Inuence of temperature on viscosity of ZnOEG nanouids has
been studied over a wide temperature range of 10140 C
(Fig. 6a and b). Viscosity of ZnOEG nanouids decreased in an
asymptotic manner with increasing temperature similar to that
of ethylene glycol, the base uid (Fig. 6a). Viscosity variation of
nanouids and the base uid with temperature could be tted into
power law as follows

l AT B
Fig. 4. (a) Inuence of shear rate on viscosity of ZnOEG nanouids of different
concentrations and ethylene glycol and (b) inuence of nanoparticle volume
concentration on relative viscosity of ZnOEG nanouids.

the viscosities of ZnOEG nanouids might be due to the differences in nanouid formulation method (ultrasonication time/use
of surfactant), morphological characteristics of ZnO nanopowder
used, etc. which ultimately resulted in different aggregate size
distributions.
Intermolecular as well as intramolecular hydrogen bonding persists in ethylene glycol. Metal oxide nanoparticles are known to
have hydroxyl groups on their surface when dispersed in polar liquids [66]. Hydroxyl groups engaged in intramolecular and intermolecular hydrogen bonding between ethylene glycol molecules are
likely to form hydrogen bonds with hydroxyl groups on nanoparticles surface. Hence, the hydrogen bonding network of ethylene
glycol is reorganized.
At higher nanoparticle concentration, the number of ZnO nanoparticles interacting with ethylene glycol molecules was higher
and hence, perturbations to the hydrogen bonding network of ethylene glycol were enhanced leading to decrease in viscosity with
increasing nanoparticle concentration.
In our recent studies of propylene glycol based nanouids
[24,40,48,67], rheological behavior similar to that of ZnOEG
nanouids of the current study was observed. CuOPG,
ZnOPG, Fe2O3PG, sandPG, Mn0.43Fe2.57O4PG nanouids had
viscosities lesser than propylene glycol and perturbations in
hydrogen bonding network was identied as the rationale
behind the unusual rheological behavior of propylene glycol
based nanouids.

Value of B signies the temperature dependency of viscosity of


the uids. B value decreased with increasing concentration with
pure ethylene glycol having the highest B value. This shows that
the addition of nanoparticles had reduced the temperature dependency of ZnOEG nanouids.
The decrease in viscosity of liquids with increasing temperatures is due to decrease in the magnitude of intermolecular attractive forces such as hydrogen bonds [69,70]. With reduction in
intermolecular forces of attraction at higher temperatures, their
inuence on viscosity is also reduced. Hence at higher temperatures, the perturbation of hydrogen bonds does not proportionately
lead to reduction in nanouid viscosity, while the contribution of

Fig. 5. Inuence of nanoparticle volume concentration on relative viscosity of ZnO


EGwater nanouids.

K.S. Suganthi et al. / Applied Energy 135 (2014) 548559

553

Fig. 7. Inuence of temperature on relative viscosity of ZnOEG nanouids at


different concentrations.

Fig. 6. Inuence of temperature on viscosity of ZnOEG nanouids and ethylene


glycol (a) 27140 C and (b) 1020 C.

nanoparticles to increased viscous dissipation is temperature-independent. Hence, viscosity of ZnOEG nanouid shows lower temperature dependence than pure ethylene glycol, with lowest
temperature dependence observed at the highest nanoparticle concentration (4 vol.%) investigated.
In order to further evaluate the effect of addition of nanoparticles on nanouid viscosity, the relative viscosity of nanouids was
calculated as follows:

lr lnanofluid lbase fluid

Anf T Bnf
Abf T Bbf

temperatures at which liquid viscosities depend on intermolecular


forces than that at higher temperatures at which inuence of intermolecular forces on liquid viscosity is negligible.
Another striking observation from viscosity measurements is
that relative viscosities of ZnOEG nanouids were lower than
unity up to temperature of 110 C. This shows that pumping power
required to circulate ZnOEG nanouids will be lower than that
required for pure ethylene glycol up to 110 C. As long as the temperature is below 110 C, relative viscosity of 4 vol.% nanouid is
lower than that of 2 vol.% whereas at 140 C, the relative viscosity
of 4 vol.% is higher than that of 2 vol.%.
To get better understanding, variation of relative viscosity with
nanoparticle concentration at different temperatures has been
plotted in Fig. 8. The slope of the curve gradually changes from
negative to positive as the temperature is increased from 10 to
140 C.

3.1.2.2. Viscosity model. The abundance of suspensions and dispersions in practical applications puts forward the demand for development of models to predict viscosity. Einstein [71] derived an
expression to determine viscosity of dispersions of spherical,
non-interacting particles in a dilute suspension. Mooney [72] proposed a model for prediction of relative viscosity of concentrated
suspensions (/ > 0.05) in which empirical constants were used. A

Fig. 7 shows the relationship between relative viscosity and


temperature at different nanoparticle concentrations. From Fig. 7,
it can be observed that relative viscosity increases with increasing
temperature, which implies that decrease in viscosity of nanouids
with temperature is lower than that of base uid. Highest reduction in viscosity of ZnOEG nanouids has been observed at the
lowest temperature investigated. For instance, reduction in viscosity of 4 and 2 vol.% ZnOEG nanouids at 10 C are 66% and 45%
respectively. At lower temperatures, movement of liquid molecules is dominated by intermolecular forces, which have higher
inuence over liquid viscosities at lower temperatures. At higher
temperatures, intermolecular forces between molecules begin to
diminish and the movement of liquid molecules is controlled by
their translational energy. Since the addition of ZnO nanoparticles
brings out reduction of dispersion viscosity by disturbing hydrogen
bonding network, viscosity reduction is more pronounced at lower

Fig. 8. Inuence of nanoparticle volume concentration on relative viscosities of


ZnOEG nanouids at different temperatures.

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K.S. Suganthi et al. / Applied Energy 135 (2014) 548559

semi-empirical equation for shear viscosity of suspensions was


proposed by Krieger and Dougherty [73] for a wide range of particle concentrations. Taking particle aggregation into account, Chen
et al. [74] proposed a modied form of KriegerDougherty equation that predicted viscosity enhancement of dispersions with
aggregation well. All these models were used to predict the
enhancement in viscosity of dispersions due to particle addition.
Since viscosity reduction has been observed for ZnOEG nanouids, these models cannot be directly used for viscosity prediction.
A new empirical model is developed to predict the viscosity of
ZnOEG nanouids over a concentration and temperature range
of 04 vol.% and 27140 C respectively. This model takes into
account increase in viscosity due to particle addition, decrease in
viscosity due to disturbance in intermolecular forces due to nanoparticle addition and the effect of temperature as follows:

lr x  y

where x is increase in relative viscosity due to particle addition and


y is decrease in relative viscosity due to disturbance in intermolecular forces. While x is a function of nanoparticle volume fraction,
y is a function of nanoparticle volume fraction and temperature.
To determine the expression for x that describes increase of
nanouid viscosity with nanoparticle concentration, relative viscosity of nanouid at 140 C was correlated with nanoparticle concentration, as the inuence of intermolecular forces of attraction
on viscosity at this temperature was minimal. Relative viscosity
(lr)-nanoparticle volume concentration (/) relationship at 140 C
was found to be lr = 1 + 5.9765/. This expression can be used to
predict the increase in viscosity due to particle addition.
Therefore, Eq. (4) becomes

lr 1 5:9765/  f T; /

Fig. 9. Comparison between experimental and predicted relative viscosities of


ZnOEG nanouids.

Taking into account of the fact that the relative viscosity-nanoparticle concentration relationship is linear at all temperatures
(Fig. 8), the y in Eq. (4) is expected to vary linearly with nanoparticle concentration and non-linearly with temperature.
Using the relative viscosity data over a temperature range of
27140 C, the following empirical correlation was obtained using
Minitab 16 with a regression coefcient of 0.9135.

lr 1 5:9765/  518:979/T 0:9014

The developed empirical model predicts the relative viscosity of


ZnOEG dispersions well, as evident from Fig. 9 that shows the
comparison between predicted and experimental relative
viscosities.
3.1.2.3. ZnOEGwater nanouids. Fig. 10(a) shows the inuence of
temperature on viscosity of ZnOEGwater nanouids and EG
water (base uid) over a temperature range of 1055 C. Viscosity
of ZnOEGwater nanouids decreased with increasing temperature exponentially and could be tted to power law as ZnOEG
nanouids (Eq. (2)).
B values (from Eq. (2)) of EGwater, 1 vol.% ZnOEGwater and
2 vol.% ZnOEGwater were found to be 0.7756, 0.7298 and 0.6937
respectively. Similar to ZnOEG nanouids, B values decreased
with increasing nanoparticle concentration. Value of B in Eq. (2)
is an indication of dependency of viscosity of the uids on temperature. Viscosity of ethylene glycolwater mixture, the base uid
showed higher temperature dependency compared to nanouids,
which might be due to the higher magnitude of intermolecular
forces that existed in the base uid.
Relative viscosities of ZnOEGwater nanouids have been calculated using Eq. (3) and have been plotted against temperature
(Fig. 10b). Relative viscosities were less than one over the entire
temperature range investigated (1055 C). Relative viscosity of

Fig. 10. (a) Inuence of temperature on viscosity of ZnOEG nanouids and


ethylene glycol and (b) inuence of temperature on relative viscosity of ZnOEG
nanouids at different concentrations.

2 vol.% nanouid was lower than that of 1 vol.% nanouids at all


temperatures.
The relative viscosity may be related to temperature and
nanoparticle concentration using the form Eq. (5) with expression for f(T, /) specically derived for ZnOEGwater system
as follows:

f T; / 5T 0:1802 /0:5455

K.S. Suganthi et al. / Applied Energy 135 (2014) 548559

555

Eq. (5) for ZnOEGwater nanouid becomes

lr 1 5:9765/  5T 0:1802 /0:5455

The developed empirical model predicts the relative viscosity of


ZnOEGwater dispersions well, as evident from Fig. 11 that shows
the comparison between predicted and experimental relative
viscosities.
3.2. Thermal conductivity of dispersions
3.2.1. ZnOEG nanouids
Fig. 12(a) shows the variation of thermal conductivity of ZnO
EG nanouids with nanoparticle volume concentration at 27 C.
Linear variation of thermal conductivity with nanoparticle concentration depicts the well dispersed nature of nanoparticles or
nanoclusters in ZnOEG nanouids. About 33.4% increase in thermal conductivity has been observed for 4 vol.% ZnOEG nanouids.
Thermal conductivity ratios of ZnOEG nanouids prepared in this
study had relatively higher thermal conductivity ratios than that of
other researchers [51,64,65] except that of Kole and Dey [39]
(Fig. 12b). The differences in thermal conductivity of ZnOEG
nanouids can be attributed to the difference in morphology of
the nanomaterial used and ultrasonic processing. ZnOEG nanouids prepared by Kole and Dey [39] being sonicated for prolonged
time (>60 h) had smaller sizes of aggregates (<100 nm) resulting in
higher thermal conductivity than that of the present study (sonication time 30 h).
From the experimental thermal conductivity data, thermal conductivity ratio-nanoparticle volume concentration relationship (at
27 C) can be expressed as

kr 1 7:926/

HamiltonCrosser model of thermal conductivity of dispersions


for spherical particles is as follows:

kr 1 3/

10

Comparing Eqs. (9) and (10), it can be observed that slope of the
Eq. (9) is about 2.64 times greater than that of HamiltonCrosser
equation (Eq. (10)). Anomalous enhancement in thermal conductivity of nanouids is due to nanoscale phenomena occurring in
the colloidal solidliquid dispersions. Microconvection induced
by Brownian motion of nanoparticles, ordered arrangement of
liquid molecules over solid nanoparticles (liquid layering), particle
clustering and ballistic heat transport [75] have been identied as
the major mechanisms responsible for anomalous enhancement of

Fig. 12. (a) Inuence of nanoparticle volume concentration on thermal conductivity


of ZnOEG nanouids at 27 C and (b) inuence of nanoparticle volume concentration on thermal conductivity ratio of ZnOEG nanouids and comparison with
literature and (c) inuence of temperature on thermal conductivity of ZnOEG
nanouids.

Fig. 11. Comparison between experimental and predicted relative viscosities of


ZnOEGwater nanouids.

thermal conductivity. Contribution of each of these mechanisms to


thermal conductivity enhancement of nanouids depend on
hydrodynamic size distribution of solid particles, physical and
chemical nature of base uid, temperature, interaction between
dispersed and continuous phase, etc. Hence, contribution of each
of the nanoscale mechanisms to thermal conductivity enhancement of nanouids differs for each nanouid system.

556

K.S. Suganthi et al. / Applied Energy 135 (2014) 548559

Liquid layering of propylene glycol molecules over ZnO nanoparticles was found to inuence thermal conductivity enhancement in ZnOPG nanouids and its unique temperature
dependence [57]. As propylene glycol and ethylene glycol have
similarity in chemical nature, the course of thermal conductivity
change with change in temperature can be explained by the liquid
layering of ethylene glycol molecules on ZnO nanoparticles
surface.
Fig. 12(c) shows the inuence of temperature on thermal conductivity of ZnOEG nanouids and ethylene glycol, the base uid.
Highest thermal conductivity enhancement was achieved at the
lowest temperature investigated, 10 C (Fig. 12c). The trend of variation of thermal conductivity of ZnOEG nanouids with temperature could be divided into two sections, (i) a temperature range
(1030 C), within which nanouid thermal conductivity
decreased with temperature and (ii) a temperature range (30
60 C), within which nanouid thermal conductivity was temperature-independent.
Ordered arrangement of liquid molecules over solid surfaces
have higher thermal conductivity compared to bulk liquid, since
the ordered liquid molecular structure mimics the atomic arrangement in crystalline solids with high thermal conductivity. The
thickness of such ordered layers greatly inuences thermal conductivity enhancement of nanouids and have been shown to
increase with decreasing temperature [57]. The thickness of ethylene glycol molecular layer increased with decreasing temperature
and the maximum thermal conductivity enhancement was
observed at the lowest temperature (10 C). It can also be observed
from Fig. 12c that the magnitude of the slope of the curve (10
30 C) increases with increasing concentration. Thermal conductivity increase at 10 C for 4 vol.%, 2 vol.% and 1 vol.% are 55%, 36% and
14% respectively. The amount of liquid layers contributing to thermal conductivity enhancement will be higher at higher concentrations owing to the presence of larger number of nanoparticles.
In our earlier work [57], a simplied form of Yu and Chois
model given below, was used to predict thermal conductivity
enhancement of ZnOPG nanouids at lower temperatures.

kr

knf
1 3/1 b3
kbf

11

In the above equation, / is the volume fraction, b is the ratio of


thickness of liquid layer to the radius of nanoparticle and knf and kbf
are the thermal conductivity of nanouid and thermal conductivity
of base uid respectively. Since temperature dependency of thermal conductivity of ZnOEG nanouids followed the same trend
as ZnOPG nanouids, simplied Yu and Chois model [57] was
used to predict thermal conductivity enhancement of ZnOEG
nanouids.
By tting the experimental thermal conductivity data of ZnO
EG nanouids in Eq. (11), b values at 10, 20, 27, 30 C were calculated to be 0.6598, 0.6175, 0.407, and 0.33233 respectively.
Decreasing b values with increasing temperature showed that
the thickness of liquid layers surrounding nanoparticles decreased
with increasing temperature. A comparison of experimental and
calculated thermal conductivity ratios (using Eq. (11)) is made in
Fig. 13, from which it is evident that Eq. (11) with temperaturedependent b values predict the thermal conductivity ratio well
for the temperature range of 1030 C.
Other than liquid layering, Brownian motion of nanoparticles
and particle clustering are two important mechanisms responsible
for thermal conductivity enhancement in nanouids [75]. Increase
in thermal conductivity with increasing temperature is attributed
to the Brownian motion of particles due to their higher energy at
higher temperatures and micro-convection induced by Brownian
motion of particles [18,7678]. No signicant difference in thermal

Fig. 13. Comparison of experimental and predicted thermal conductivity ratios of


ZnOEG nanouids.

conductivity was observed over the temperature range of


3050 C. Since viscosity of the dispersion is relatively low in this
temperature range, an increase in thermal conductivity due to
Brownian motion of particles is expected. However, no such
increase in thermal conductivity was observed. Hence, we postulate that the increase in thermal conductivity due to Brownian
motion of particles might have been offset by the decrease in thermal conductivity due to decrease in thickness of liquid layers in
accordance with decreasing b at higher temperatures.

3.2.2. ZnOEGwater nanouids


Fig. 14(a) shows the inuence of nanoparticle concentration on
thermal conductivity ratio of ZnOEGwater nanouids. The thermal conductivity was found to increase with nanoparticle concentration in a linear fashion, which indicates absence of signicant
particleparticle interactions. The solvation layers of ethylene glycol on ZnO nanoparticles surface has been preserved in ZnOEG
water nanouids also, as evidenced by negligible particleparticle
interaction and colloidal stability. If water molecules are in contact
with surfactant-free ZnO nanoparticles, agglomeration of nanoparticles, instability of the dispersion and deterioration of transport
properties become inevitable. However, they have been eliminated
by the use of simple hierarchical method of preparation of ZnO
EGwater nanouids.
Thermal conductivity ratio-nanoparticle volume concentration
relationship of ZnOEGwater nanouids at 27 C is as follows:

kr 1 8:195/

12

From Eqs. (9) and (12), it is evident that the thermal conductivity enhancements of ZnOEG and ZnOEGwater nanouids are
comparable. This might be yet another testimony to the preservation of layers of ethylene glycol over ZnO nanoparticles.
The inuence of temperature on thermal conductivity of
ZnOEGwater nanouids (2 vol.%) is shown in Fig. 14b. Temperature-independent behavior of ZnOEGwater nanouids can be
attributed to the combined inuence of liquid layering and Brownian motion. As temperature increases, thickness of liquid layers
decreases and hence thermal conductivity decreases. This is offset
by Brownian motion due to lower dispersion viscosity. Hence,
these two phenomena counterbalanced each other resulting in
temperature-independent thermal conductivity of ZnOEGwater
nanouids.

557

K.S. Suganthi et al. / Applied Energy 135 (2014) 548559

T at 2 bt c

15

The coefcients a and b and the intercept c for each of the


test uids are shown in Table 1. Starting from a constant initial
temperature, amount of heat absorbed (Q) was calculated for a period of 10 min using Eqs. (13) and (15).
3.3.2. Heat transfer rate ratio (Qratio)
To compare the cooling capability of nanouids with respect to
that of base uids, the ratio of heat removed by nanouid (Qnf) to
the heat removed by base uid (Qbf) has been calculated as Qratio
as follows:

Q ratio

Q nf
Q bf

16

For both ZnOEG and ZnOEGwater nanouids, Qratio were


found to be greater than one at all concentrations (Fig. 15). The better thermal performance of both ZnOEG and ZnOEGwater
nanouids might be attributed to enhanced thermal conductivity
of the nanouids. The better performance of nanouids in comparison with base uid indicates that they function as better coolants
in comparison to the base uids at all nanoparticle concentrations
investigated. The Qratio was found to increase linearly with nanoparticle concentration for both the nanouids. It may be recalled
that the thermal conductivity of both these nanouids increase linearly with nanoparticle concentration as discussed in Section 3.2.
Hence, it is evident that there is a direct correlation between thermal conductivity enhancement of nanouids and enhancement in
heat transfer rate with nanouid coolants.
3.4. Stability of nanouids
ZnOEG and ZnOEGwater nanouids were colloidally stable
over a period of two months and no settling of particles was
Fig. 14. (a) Inuence of nanoparticle volume concentration on thermal conductivity
of ZnOEGwater nanouids at 27 C and (b) inuence of temperature on thermal
conductivity of 2 vol.% ZnOEGwater nanouids.

3.3. Transient heat transfer experiments


3.3.1. Data reduction
The heat transfer performance of nanouids was analyzed
through evaluation of amount of heat transferred (Q) over a xed
length of time as follows:

Q mcp

dT
dT
V qcp
dt
dt

13

In Eq. (13), V is the volume of the test uid. The product of density and specic heat (qCp) was calculated as follows [79,80]:

qcp nanofluid /qcp nanoparticle 1  /qcp base fluid

14

The test uid temperaturetime data were tted using a polynomial equation for the entire duration of the experiment as
follows:

Fig. 15. Inuence of nanoparticle volume concentration on Qratio of ZnOEG and


ZnOEGwater nanouids.

Table 1
Coefcients a and b and the intercept c for each of the test uid.
Nanoparticle volume concentration (%)

0
0.25
0.5
1
1.5
2

ZnOEG

ZnOEGwater

8.383E06
8.594E06

9.829E06
9.361E06

0.0292
0.0302

0.0332
0.0339

30.981
30.411

29.489
31.096

6.78E06

7.53E06

6.84E06
1.23E05

0.0286

0.0313

0.0321
0.0354

31.803

30.373

28.981
32.685

558

K.S. Suganthi et al. / Applied Energy 135 (2014) 548559

observed during characterization of transport properties and heat


transfer experiments. Taking the average hydrodynamic size as
the particle diameter, particle settling velocity and Brownian
velocity can be used to assess the stability of ZnOEG and ZnO
EGwater nanouids [50]. Brownian velocities of particles in
ZnOEG and ZnOEGwater were 1.64  105 m/s and
7.109  105 m/s respectively. Particle settling velocities of ZnO
EG
and
ZnOEGwater
were
1.607  109 m/s
and
9
7.048  10 m/s respectively. Brownian velocities of the particles
are higher than that of particle settling velocities which implies
that settling of particles is less probable ensuring the colloidal
stability.
4. Conclusions
Spherical ZnO nanoparticles with a size range of 2540 nm
were synthesized by room temperature chemical precipitation
and dispersed in ethylene glycol by probe ultrasonication without
any surfactant. ZnOEGwater nanouids were prepared by hierarchical formulation strategy, which preserved ethylene glycol
molecular layers over ZnO nanoparticles surface. The inuence
of nanoparticle concentration and temperature on thermal conductivity and viscosity of ZnOEG and ZnOEGwater nanouids
revealed increased thermal conductivity and reduced viscosity.
ZnOEG and ZnOEGwater nanouids showed thermal conductivity of 33.4% and 17.26% enhancements in thermal conductivity
and 39.2% and 17.34% reduction in viscosity at particle volume
concentrations of 4 and 2 vol.% respectively. Thickness of ethylene
glycol layers of ZnO nanoparticles increased at lower temperatures
resulting in higher thermal conductivity under such conditions.
Liquid layering of molecules contributed to thermal conductivity
enhancements in ZnOEG nanouids, while liquid layering as well
as Brownian motion to temperature independent thermal conductivity of ZnOEGwater nanouids. Empirical models were developed to predict the transport properties of the nanouids. Our
results on transient heat transfer experiments using ZnOEG and
ZnOEGwater nanouids demonstrate their superior cooling
capability in comparison with the respective base uids due to
their increased thermal conductivities.
Acknowledgements
This work is supported by (i) INSPIRE fellowships (Reg. Nos.:
IF110312, IF130529) of Department of Science and Technology
(DST), India. (ii) PG teaching Grant No.: SR/NM/PG-16/2007 of
Nano Mission Council, Department of Science & Technology
(DST), India (iii) Grant No.: SR/FT/ET-061/2008, DST, India and
(iv) Research & Modernization Project #1, SASTRA University,
India. The authors thank SASTRA University for the infrastructural
support extended during the work.
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