Journal Pre-proof

An experimental investigation into the effect of particle mixture

ratio on specific heat capacity and dynamic viscosity of
Al2O3-ZnO hybrid nanofluids

Ifeoluwa Wole-Osho, Eric C. Okonkwo, Doga Kavaz, Serkan

Abbasoglu

PII: S0032-5910(20)30014-0
DOI: https://doi.org/10.1016/j.powtec.2020.01.015
Reference: PTEC 15083

To appear in: Powder Technology

Received date: 19 September 2019

Revised date: 17 December 2019
Accepted date: 6 January 2020

Please cite this article as: I. Wole-Osho, E.C. Okonkwo, D. Kavaz, et al., An experimental
investigation into the effect of particle mixture ratio on specific heat capacity and dynamic
viscosity of Al2O3-ZnO hybrid nanofluids, Powder Technology(2019), https://doi.org/
10.1016/j.powtec.2020.01.015

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An experimental investigation into the effect of particle mixture ratio on specific

heat capacity and dynamic viscosity of Al2O3-ZnO hybrid nanofluids.
Ifeoluwa WOLE-OSHO1, Eric C. OKONKWO2*, Doga KAVAZ3, Serkan
ABBASOGLU1
1
Department of Energy Systems Engineering, Cyprus International University, North Cyprus,
via Mersin-10, Turkey.
2
Division of Sustainable Development, College of Science and Engineering, Hamad Bin
Khalifa University, Education City, Qatar Foundation, Doha, Qatar.
3
Department of Bioengineering, Cyprus International University, North Cyprus, via Mersin-
10, Turkey
*Corresponding author’s email: iwole@gmail.com
Abstract

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Hybrid nanofluids are gaining a wide range of applications due to their reported

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improvement in heat transfer properties. This study presents an experimental
investigation into the specific heat and viscosity of Al2O3-ZnO water hybrid
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nanofluids at three mixture ratios. The specific heat and viscosity measurements are
taken over different temperatures at different volume concentrations. The study
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compared the experimental data to classical models and observed that the specific
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heat model overestimated and the viscosity model underestimated experimental

obtained values. According to results, the particles mixture ratio has a significant
effect on both specific heat and viscosity of the hybrid nanofluids. Viscosity increases
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while specific heat decreases by increasing the volume concentration. Al2O3-ZnO

water hybrid nanofluids at 2:1 mixture ratio have a maximum viscosity increase of
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96.37% and maximum specific heat decrease of 30.12% at a temperature of 25°C and
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volume concentration 1.67%.

Keywords: nanoparticles, hybrid nanofluids, specific heat, viscosity, Al2O3, ZnO

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1. Introduction
Nanofluids are a colloidal suspension of nanosized particles into a fluid; this class of
fluid was first proposed by Choi and Eastman [1]. These nanofluids have shown
remarkable results in thermal and mechanical applications. For instance, Oil-based
nanofluids have shown improved load-carrying capabilities, wear-resistance and
antifriction ability compared to pure engine oils [2–4]. Nanofluids have also improved
the thermal efficiencies of flat plate [5], evacuated tube [6], heat pipe [7] and
parabolic trough solar collectors [8,9] when compared to conventional heat transfer
fluids.

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Thermal and rheological properties of nanofluids like density, specific heat, thermal

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conductivity and viscosity, determine the performance of nanofluids in thermal
related applications [10]. These thermal and rheological properties are dependent on
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variables like agglomeration, nanoparticle size, nature of the base fluid, packing
fraction, nanolayers, particle distribution, pH, temperature, and volume concentration.
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The specific heat and viscosity of nanofluids are particularly important properties of
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nanofluids. There have been several studies conducted to correlate the specific heat
capacity of nanofluids with temperature and volume concentration of the nanofluids.
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From research, temperature and the specific heat of nanofluids are linearly dependent
[11]. However, the numerical relationship between specific heat capacity and volume
concentration is not clear. There have been several models to determine this
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relationship [12,13]. Yet, there is still no consensus model that captures the
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relationship between the volume concentration and the specific heat capacity of
nanofluids. Experimental measurements have observed several unique relationships
between specific heat capacity and volume concentration. Using SiO2 nanoparticles
with an average size of 21 nm Akilu et al. [14] found that specific heat of nanofluids
decreased with an increase in volume concentration of the nanoparticle. Kumaresan
and Velraj [13] observed that for MWCNT water-ethylene glycol nanofluids the
specific heat of the nanofluid reaches its maximum at 0.15% volume concentration,
after which it decreases with further increase in the MWCNT concentration. Hamid et
al. [15] observed that the specific heat of hybrid TiO2–SiO2 nanofluids in water-
ethylene glycol tends to reduce with an increase in the volume concentration of
nanoparticles.

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The effect of nanoparticle size on the specific heat capacity of nanofluid was
investigated by Angayarkanni et al. [16] using Fe2O3 nanoparticles. The nanoparticle
size varied between 3.6 nm to 8.6 nm and the specific heat capacity of the nanofluid
decreases with increase in particle size within the considered range. The effect of
diameter on both the thermal conductivity and dynamic viscosity of Fe/water
nanofluid was also studied by Esfe et al [17]. The study found that at a constant
volume fraction, the smaller the nanoparticle diameter the higher the dynamic
viscosity of the nanofluid.
The viscosity of nanofluid also affects the stability and heat transfer property of the
fluid. Several experimental studies have observed that the viscosity of nanofluids

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increases with an increase in the nanoparticles volume concentration [18]. Studies

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have also shown that the viscosity of nanofluids reduces with an increase in the
temperature of the fluid. This is because an increase in temperature reduces the
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intermolecular attraction between the nanoparticles and the base fluids [18].
Nanofluids with high base fluid viscosity are increasingly more stable than nanofluids
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with lower base fluid viscosity; this is because base fluid with high viscosity tend to
reduce the Brownian motion which results in less agglomeration as nanoparticles are
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less likely to collide. Also, nanofluids with highly viscous base fluids suspend
particles easier because of the higher hydrodynamic drag at higher viscosity [19].
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While nanoparticle agglomeration appears not to affect the viscosity of nanofluids,

agglomeration tends to change its effective volume concentration [20]. Also, while an
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increase in nanoparticles concentration, improves viscosity, this increase negatively

affects the heat transfer of the fluid in many thermal systems [21,22].
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Several studies have also investigated the relationship that exists between particle size
and viscosity. However, there appears to be no direct correlation between an increase
in particle size and the viscosity of nanofluids as the relationship seems to change
dependent on the nanoparticle dispersed in the based fluid. There have been
seemingly contradictory results about the effects of particle size in Al2O3-water.
Nguyen et al. [23] compared Al2O3-water nanofluids with particle sizes of 36 nm and
47 nm and observed that at a constant volume concentration, dynamic viscosity
increased with an increase in particle size. Contrary results from Anoop et al. [24]
shows that viscosity increases with a decrease in particle size for Al2O3-water
nanofluids using 45 nm and 150 nm at a constant concentration. These contradictory
findings could be as a result of the difference in the range considered. These plain

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contradictions are observed across nanofluid types. While an increase in particle size
tends to increase viscosity in TiO2 [25] particle size increase leads to viscosity
reduction in SiO2 [26].
Hybrid nanofluids are a distinct class of nanofluids where the based fluid contains
dispersions of more than one nanoparticle. Over the last decade, there have been
several investigations into the rheological properties of hybrid nanofluids. Suresh et
al. [27] investigated the rheological properties of Al2O3-Cu hybrid nanofluids with
mixture ratios of 90:10 and at volume concentrations between 0.1% and 2%. The
results showed that both viscosity and thermal conductivity of the hybrid nanofluids
increases with nanoparticles volume concentration. However, the viscosity increase is

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substantially higher than the thermal conductivity increase with an increase in particle

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loading. Also, Aparna et al. [28] synthesized Al2O3-Ag water hybrid nanofluid at
three different mixture ratios of Ag and Al2O3 (30:70, 50:50: 70:30) when volume
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concentration was between 0.005% and 0.1%. The results show that 50:50 had the
best thermal conductivity compared with the other mixture ratios.
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There have also been investigations into the rheology of both ZnO-Ag/water [29]
hybrid nanofluid and ZnO–TiO2/EG [30] hybrid nanofluids at volume concentrations
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of 0.125-2% and 0-3.5% respectively. In both studies, the thermal conductivity of the
hybrids improved with an increase in temperature and volume concentration. The
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rheological behaviour of the hybrid nanofluid of MWCNT–alumina/water (80%)–

ethylene-glycol (20%) nanofluid was studied by Afshari et al [31]. The study found
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that the hybrid nanofluid showed Newtonian behaviour when the volume
concentration was between 0 and 0.5%. However, when volume concentration
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reached 0.75% the hybrid nanofluid began to show pseudoplastic non-Newtonian

behaviours.
Sharma et al. [38] compared numerical models to the experimental viscosity values of
CeO2-Cu water hybrid nanofluid, Al2O3-Cu water hybrid nanofluid, TiO2-Cu water
hybrid nanofluid and SiO2-Cu water hybrid nanofluid at a mixture ratio of 4:1 and
volume concentration between 0.5%-3%. Results showed that viscosity increased
with an increase in volume concentration but reduced with an increase in temperature.
The study also observed that the experimental values exceeded the predicted values of
the considered numerical models.
There have been several numerical models to predict viscosity and specific heat
capacity of nanofluids. Einstein proposed the first model for predicting the viscosity

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of spherical particles dispersed in liquid [34]; however, this model often significantly
deviates from experimental results for nanoparticle dispersions [38]. Several other
models have been proposed for viscosity prediction. Models proposed by Mooney
[35], Krieger and Dougherty [36], Nielsen [37], and Batchelor [38] represent classical
models for the prediction of the viscosity of nanofluids. There have also been several
predictive models to estimate the specific heat capacity of nanofluids [12] [39].
Due to the inaccuracy of these classical models, several researchers have proposed
several correlation models to predict the relationship between the thermal and
rheological properties of nanofluids with parameters like temperature, volume
concentration, particle size etc. In the last two years, empirical correlations have been

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developed to predict the thermal conductivity of silica/water-ethylene glycol (40%–

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60%) nanofluid [40], water-ethylene glycol/TiO2-MWCNTs hybrid nanofluid [41]
and ZnO–Ag (50%–50%)/water hybrid [42]. An empirical correlation has also been
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developed to predict the dynamic viscosity of CeO2- ethylene glycol nanofluid [43],
silver/ethylene glycol nanofluid [44], and MWCNTs/ZnO-SAE40 hybrid nanofluid
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[45].
As observed from literature, a lot of focus has been placed on the thermal
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conductivity property of nanofluids, while thermal conductivity is relevant, the

specific heat capacity and viscosity of nanofluids are also significant as well. Specific
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heat is exceptionally substantial because it is an essential parameter in analyzing the

energy content of thermal systems. The viscosity, on the other hand, determines the
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resistance of fluid flow. It is therefore vital that researchers completely understand

both the specific heat capacity and viscosity behaviours compared to parameters like
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temperature, volume concentration and mixture ratio. Investigation on the influence

of mixture ratio and its effect on the specific heat capacity and viscosity are limited in
the literature. Moreover, while there are several works on hybrid nanofluids,
investigation of Al2O3-ZnO water hybrid nanofluid has not been performed.
The particle mixture ratio is a unique parameter of hybrid nanofluids because the
nanoparticles in a hybrid can be configured in several different mixture ratios at the
same concentration. This study presents a novel investigation into the specific heat
capacity and viscosity behaviours of a hybrid nanofluid at three different mixture
ratios; 1:2 (33.34 vol.% Al2O3: 66.66 vol.% ZnO), 1:1 (50 vol.% Al2O3: 50 vol.%
ZnO) and 2:1 (66.66 vol.% Al2O3: 33.34 vol.% ZnO) of Al2O3-ZnO at varying
volume concentrations and temperatures. The experimentally obtained results were

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also compared to classical theoretical models obtained from literature and new
correlation models are proposed.

2. Synthesis and characterization of nanoparticles in hybrid

Al2O3 and ZnO nanoparticles (NP) were individually synthesized with different
synthesis techniques. Al2O3 NP was manufactured using a green synthesis technique
proposed by Manikandan et al [46]. This synthesis technique produced Al2O3 with an
average particle size 29 nm. ZnO NP, on the other hand, was synthesized using a
method proposed by Romadhan et al[47]. From the particles XRD analysis, the

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average size of ZnO NP was 70 nm. Figure 1(a) and (b) show the SEM image of

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Al2O3 and ZnO nanoparticles. The reflections in the XRD pattern corresponded with
the structural properties of the dry Al2O3 and ZnO nanoparticles as seen in Figure 2.
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From the XRD image, the red line represents the pattern obtained for the ZnO
nanoparticles. The diffraction was recorded using Cu Kα radiation (1.5406
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Angstrom) and the XRD pattern was taken at 2θ for values ranging from 20° - 80°.
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All evident peaks observed were referenced with the zinc oxide wurtzite structure
(JCPDS Data Card No: 36-1451) and as seen, the ZnO (red line) peaked at 32°, 36°,
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39°, 48°, 57°, 63°, 68°, and 69°, these reflected the (100), (002), (101), (102), (110),
(103), (112) and (201) and showed good agreement with the reference data. The XRD
pattern for Al2O3 nanoparticles (green line) appeared to peak at 32°, 39°, 48°, 57°,
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62°, and 68° all correspond to the characteristic reflection of (220), (222), (400),
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(422), (511) and (440) which are well-coordinated with JCPDS card no. 02-1420.
These peaks also signify the high purity of the nanoparticles. The blue line represents
a mixture of both nanoparticles and corresponding peaks are evident of both ZnO and
Al2O3.

2.1. Preparation of hybrid nanofluids

The two-step method was used in the preparation of the hybrid nanofluids. The first
part of the preparation involves dispersing the nanoparticles in distilled water, which
was used as the base fluid. The average diameter of the Al2O3 and ZnO used was 29
nm and 70 nm, respectively. For proper dispersion of nanoparticles in water, an
ultrasonic vibrator (400 W, 24 kHz) was used on the nanofluid for about 3 hours
without dispersant. Also, pH modulation was done to determine the optimal stability

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of the hybrid nanofluids. The two-step preparation method was used because of its
ability to control volume concentration [48]. The experiments were conducted at three
nanoparticle mixture ratios (Al2O3: ZnO) of 1:2 (33.34 vol.% Al2O3: 66.66 vol.%
ZnO), 1:1 (50 vol.% Al2O3: 50 vol.% ZnO) and 2:1 (66.66 vol.% Al2O3: 33.34 vol.%
ZnO). These mixture ratios were considered at five different volume concentrations
0.33%, 0.67%, 1%, 1.33% and 1.67%. For the hybrid nanofluids, the volumetric
concentration was determined using equation (1) and (2) below.
𝑊𝑛𝑝
𝜌𝑛𝑝
% 𝑉𝑜𝑙𝑢𝑚𝑒𝑡𝑟𝑖𝑐 𝑐𝑜𝑛𝑐𝑒𝑛𝑡𝑟𝑎𝑡𝑖𝑜𝑛 = 𝑊𝑛𝑝 × 100 (1)
[ ]+𝑉𝑏
𝜌𝑛𝑝

φ = φ𝑎 + φ𝑧 (2)

of
where 𝑊𝑛𝑝 , 𝜌𝑛𝑝 , 𝑉𝑏 , φ𝑎 , φ𝑧 represents the weight of the nanoparticle, the density of

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the nanoparticle, the volume of the base fluid, the concentrations of Al2O3 and ZnO
respectively.
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2.3. Stability of nanofluid
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As nanoparticles undergo Brownian movement they tend to collide with each other.
Van der Waals force of attraction aids the particles to aggregate upon collusion,
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which, in turn, increases particle size and particle density [49]. Ultimately the particle
density of the aggregated particle exceeds that of the base fluid and begins to
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crystalize. This phenomenon is known as agglomeration. Due to the agglomeration of

nanoparticles in the nanofluids, the stability of the nanofluid reduces with time.
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Stability of nanofluids can be measured by the sedimentation method or zeta potential

test. In this study, the zeta potential test was used to measure the stability of
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nanofluids. pH meter and Malvern zeta sizer nano zs90 model was used to measure
pH and zeta potential respectively.
Zeta potential analysis was performed on the samples at 1.67% volume concentration
for pH values of 1, 4, 7, 10 and 12. The zeta potential stability test results are shown
in Table 1. From Table 1 it is observed that Al2O3- ZnO water-based hybrid nanofluid
is most stable when pH=12, as the higher absolute value of the zeta potential the more
stable the nanofluid [50]. This is in agreement with literature as nanofluids are
significantly more stable as the pH moves further away from the isoelectric point.

2.4. Specific heat and Viscosity measurement technique

Brookfield DV-I PRIME digital viscometer was used to measure the fluid viscosity in

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this work. The viscometer equipped with a temperature bath kept the samples at a
constant temperature as viscosity measurements were taken. Measurements were
taken at different temperature conditions (25, 35, 45, 55, 65 °C). According to the
manufacturer, the accuracy and repeatability of the digital viscometer is ±2% and
±5% respectively. The viscosity of distilled water was measured at different
temperatures to determine measurements accuracy and was validated with ASHRAE
standard [51] the results showed a near-perfect agreement.
In this study, Mettler Toledo 823 model differential scanning calorimeter was used to
measure the specific heat capacity of the nanofluids according to the ASTM standard
[52]. The protocol requires comparing the heat flux in an empty aluminium pan (the

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baseline), reference material (sapphire standard) and nanofluid samples at the set
temperature. Heating was performed between 25 oC to 80 °C at a 20 °C/min heating

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rate. The protocol includes a three-step procedure:
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(1) Equilibrate and remain isothermal at 25 °C for 4 mins; (2) Ramp to 80 °C at 20
°C/min also, (3) Remain isothermal at 80 °C for 4 mins.
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2.5. Uncertainty Analysis

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It is an accepted principle that both systematic and random errors are likely made
during any experimental analysis. Therefore in this study, all measured quantities
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were subject to an acceptable level of uncertainty. This uncertainty was analyzed

using the Shaw measurement uncertainty method [53]. Measurement of the errors in
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volume, temperature, weight, specific heat capacity and viscosity was considered.
Probable errors in the measurement parameters were calculated and the estimated
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uncertainties associated viscosity and specific heat capacity was 4% and 5%

respectively.

3. Theoretical models and limitation

Accurately predicting the rheological properties of nanofluids will considerably
improve how nanofluids are applied and understood. While many models have been
proposed to predict these rheological properties, many of them have shown to be
limited by their significant inaccuracies.

3.1. Theoretical models for viscosity prediction

Many researchers have proposed model equations to predicting the viscosity of

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dispersion in liquids. Einstein [34] first postulated the viscosity behaviour of “small
rigid spheres suspended in a liquid”, Many equations, however, have been proposed
to improve theoretical prediction of viscosity. Table 2 explains the limitations of
classical models for predicting the viscosity of solid spheres dispersed in solution.
All of these proposed models were long before the discovery of nanoparticles and
only considers microparticles. Masoumi et al. [54] first developed a model for the
viscosity of nanofluids by considering the Brownian motion effect of the particles.
Their proposed model is presented in equation 3.

𝜌𝑝 ∗ 𝑉𝐵 ∗ 𝑑𝑝2 (3)
𝜇𝑛𝑓 = 𝜇𝑏𝑓 . (1 + 2.5𝜑𝑒 + )

of
72 ∗ 𝛿 ∗ 𝐶𝑓
where 𝜇𝑏𝑓 , 𝜌𝑝 , 𝑉𝐵 , 𝑑𝑝 , 𝐶𝑓 𝑎𝑛𝑑 𝛿 represents the viscosity of nanofluids, density of the

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particle, Brownian velocity, diameter of the particle, correlation factor and distance
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between particles. The Brownian velocity, the distance between particles, and the
correlation factor is defined by equation (4), (5) and (6) respectively.
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18 ∗ 𝑅 ∗ 𝑇 (4)
𝑉𝐵 = √
𝜋 ∗ 𝑁𝐴 ∗ 𝜌𝑝 ∗ 𝑑𝑝3
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where R, T, and 𝑁𝐴 represent a universal gas constant, temperature, and Avogadro

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constant respectively.
(5)
𝜋 ∗ 𝑑𝑝3
3
𝛿= √
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6∗𝜑
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−1
𝐶𝑓 = 𝜇𝑏𝑓 (𝑇 ∗ 10−10 ∗ 𝜑 −0.002𝑇−0.284 ) (6)

Udawattha et al. [55] further improved Masoumi et al.[54] viscosity model to

consider hybrid nanofluids assuming equation (2).
𝑛𝑛𝑝 𝑛𝑛𝑝
(7)
𝜇𝑛𝑓 = 𝜇𝑏𝑓 . (1 + 2.5 ∑ 𝜑𝑒𝑖 + ∑ 𝜇𝑑𝑦𝑖 )
𝑖=1 𝑖=1

where np and φ represent the number of nanoparticles and volume concentration of

nanoparticles respectively.
2
𝜌𝑝𝑖 ∗ 𝑉𝐵𝑖 ∗ 𝑑𝑝𝑖 (8)
𝜇𝑑𝑦𝑖 = )
72 ∗ 𝛿𝑖 ∗ 𝐶𝑓

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By increase the variables considered, this proposed model is considered to be a more

accurate viscosity model than those proposed in Table 2.
Figure 3 shows the relationships between the viscosity of various Al2O3-ZnO
nanoparticle mixture ratios with temperature for volume concentration between
0.33% and 1.67% compared with the predictive model proposed by Udawattha et al.
[55].
From Figure 3, it can be observed that the predictive model grossly underestimates
the viscosity of the nanofluids. While the model accounts for the Brownian properties
and size of the particles, the resulting equation is a variance of Einstein's model. As
seen in Table 2, Einstein models cannot accurately predict models above 0.02 volume

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concentration; this was not reflected in the model report accurately[55]. Also from

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Figure 4, it is observed that the model does not account for the effect of nanoparticle
mixture ratio as the lowest viscosity obtained from the model was at 2:1 (Al2O3: ZnO)
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mixture ratio while the least measured viscosity exists at 1:1 (Al2O3: ZnO). The
deeping effect observed from the measured data could not be seen from the model.
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3.2. Specific heat numerical predictive models

Accurately predicting the specific heat capacity of the nanofluids would help
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researchers to improve their understanding of heat retaining properties of the

nanofluids. Table 3 explains the limitations of classical models for predicting the
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specific heat capacity of solid spheres dispersed in solution.

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From studies, it has become clear that the thermal equilibrium models which assume
that a thermal equilibrium exists between the base fluid and the nanoparticle are a
better numerical predictor of specific heat capacity than the mixture theory. Zhou [56]
postulated another thermal equilibrium model for the specific heat capacity of
nanofluid which is presented in equation (9)
𝜑𝜌𝑛𝑝 𝐶𝑛𝑝 + 𝐶𝑏𝑓 𝜌𝑏𝑓 (1 − 𝜑) (9)
𝐶𝑛𝑓 =
𝜑𝜌𝑛𝑝 + (1 − 𝜑)𝜌𝑏𝑓
where 𝜌𝑛𝑝 , 𝜌𝑏𝑓 , 𝐶𝑏𝑓 , and 𝐶𝑛𝑝 represents the density of nanoparticle, density of base
fluid, specific heat capacity of base fluid and specific heat capacity nanoparticle.
In hybrid nanofluids, the density and specific heat capacity of the composite
nanoparticles are given by equation (10) and (11) respectively.

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∑𝑛𝑛𝑝
𝑖=1 𝜑𝑖 𝜌𝑖
(10)
𝜌ℎ𝑛𝑝 =
∑𝑛𝑛𝑝
𝑖=1 𝜑𝑖

∑𝑛𝑛𝑝
𝑖=1 𝜑𝑖 𝜌𝑖 𝐶𝑝𝑖
(11)
𝐶ℎ𝑛𝑝 =
𝜌ℎ𝑛𝑝 ∗ ∑𝑛𝑛𝑝
𝑖=1 𝜑𝑖

Figure 5 shows, a comparison between experimentally measured results for specific

heat and results from the model proposed by Zhou et al. [56]. The model predicts that

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an increase in volume concentration leads to a decrease in the specific heat for all the
hybrid nanofluids. However, the model does not accurately predict the specific heat

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performance of the hybrids. The Zhou et al. [56] model tends to overestimate the
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value of specific heat, at all concentrations and temperatures for each of the hybrid
nanofluids ratios. From the experimental data, the specific heat capacity of the
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nanofluids gradually increases with an increase in temperature, the model predicts
that the specific heat capacity stays fairly constant with increase in temperature.
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Figure 6 shows the effective specific heat capacity of hybrid (i.e. the specific heat
capacity of the nanofluid divided by the specific heat capacity of the base fluid)
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against varying mixture ratios of Al2O3. While the experimental analysis shows that
specific heat of hybrid peaks when the ratios of ZnO and Al2O3 are equal. The
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numeric model does not reflect this phenomenon and inaccurately predicts that the
specific heat capacity of the hybrid peak at the least volume ratio of ZnO.
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The theoretical model’s inaccuracies are a result of several factors that are not
considered by the thermal equilibrium equation. Thermal equilibrium tends to
assume the specific heat capacity of materials as an absolute value. However, Wang,
Zhou, and Peng [57] show that the specific heat of nanoparticles is transient. This
means that the specific heat of the nanoparticle increases with temperature and can
exceed the specific heat of the bulk material by as much as 25%. Also, the model does
not account for particle size. The size of the nanoparticle has a significant effect on
specific heat. As nanoparticles below 10 nm are influenced by the quantum effect [57]
and nanofluids with particles above 10 nm tend to decrease monotonically with an
increase in size [12]. The model also fails to consider the effect of the Rankine-
Hugoniot jump conditions in the solid-solid interface of the hybrid particles [58] and

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the liquid-solid interface with the nanofluids [59].

3.3 Proposed model for prediction the relative viscosity of hybrid nanofluid
As shown in the section above, classical equations have shown significant
inaccuracies in predicting both the specific heat and the viscosity of hybrid nanofluid
at different volume concentrations, temperatures and mixture ratios. Using the
experimental results obtained for Al2O3-ZnO water hybrid nanofluid within the
temperature range of 25–65 0C and the volume concentration range of 0.33% to
1.67%. A correlation model was developed to calculate the specific heat and the
dynamic viscosity of the hybrid nanofluid. The polynomial additive models for

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specific heat capacity and viscosity are presented in equation 12 and equation 13
respectively. The value of the constants in equations 12 and 13 are given in Table 4.

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The specific heat capacity of nanofluid is given by:
𝐶𝑝 𝑛𝑓 = (𝑎1 + 𝑎2 𝑇𝑓 + 𝑎3 𝑇𝑓2 + 𝑎4 𝑅 + 𝑎5 𝑅 2 + 𝑎6 𝜑 + 𝑎7 𝜑 2 )𝐶𝑝 𝑏𝑓 (12)
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The viscosity of the nanofluid is given by:
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𝜇𝑛𝑓 = (𝑎1 + 𝑎2 𝑇𝑓 + 𝑎3 𝑇𝑓2 + 𝑎4 𝑅 + 𝑎5 𝑅 2 + 𝑎6 𝜑 + 𝑎7 𝜑 2 )𝜇𝑏𝑓 (13)
The statistical validation of the model is determined using the root mean square
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(RMS) and the coefficient of determination (R2). The R2 value of the correlation
model presented both equation (12) and (13) is observed as 0.993 and 0.933 with
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RMS values of 0.005 and 1.62 respectively. The experimental data is in good
agreement with the predicted values obtained from equation (12) and (13) based on
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the statistical analysis shown in Figure 7.

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4. Results and discussions.

4.1. Specific Heat of Al2O3-ZnO water hybrid nanofluids

The specific heat capacity (Cp) of fluid is actually quite significant in determining
heat content or rate of heat transfer in thermal systems. Figure 8 shows the specific
heat against volume concentration within the range of 0.33% to 1.67% for ZnO,
Al2O3 and Al2O3: ZnO at 2:1, 1:1 and 1:2 nanofluids at 25 °C and 65 °C.
From Figure 8, the specific heat of the nanofluids reduces as volume concentration
increases. This decrease in specific heat with increasing volume concentration is
reasonably consistent with the literature on various nanofluids [60,61]. Since the
specific heat capacity of the nanoparticles is far less than the base fluid water, the

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increase in nanoparticles volume concentration in nanofluids will naturally reduce the

specific heat capacity of the nanofluids.
When the temperature was between 25 °C and 65 °C for volume concentrations at
0.33% and 1.67%, Figure 9 shows the specific heat capacity for Al2O3 nanofluid, ZnO
nanofluid and various mixture ratios of Al2O3-ZnO hybrid nanofluid. For the
considered range of volume concentration, 0.33% and 1.67% present the maximum
and minimum values for specific heat capacity. As temperature increases within the
considered range, the specific heat capacity also increases for all the nanofluids. The
specific heat capacity of water tends to reduce slightly with an increase in
temperature. Therefore the increase in the specific heat with temperature observed in

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Figure 9 is attributed to the nanoparticles present in the base fluids. The imperfect

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geometrical nature of the nanoparticles affects the specific heat of nanoparticles,
ultimately creating a difference between the specific heat capacity of the particles and
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the bulk material [62]. As temperature increases, the specific heat capacity of the
nanoparticles rises and can exceed that of the bulk material by as much as two times
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[57].
Figure 10 shows the specific heat capacity of nanofluids as ZnO mixture ratio is
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increased in the hybrid from 0-100% (Al2O3 mixture ratio reduced from 100-0%) for
(a) volume concentration of 1.67% (b) temperature at 25 °C. Considering the hybrid
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nanofluids in Figure 10 (a), Al2O3-ZnO Hybrid at 1:1 ratio shows the highest specific
heat capacity while Al2O3-ZnO hybrid at 2:1 ratio shows the least value for specific
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heat capacity for all of the temperature ranges considered at 1.67% volume
concentration. Compared to base fluid, the maximum decrease in the specific heat of
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Al2O3-ZnO water hybrid nanofluids was 30.12%, 21.68% and 17.46% for mixture
ratios of 2:1, 1:2 and 1:1 respectively. The results also show that Al2O3-water
nanofluids have a lower specific heat compared to ZnO-water nanofluids at the same
temperature. Also, as the difference in ratios of Al2O3 and ZnO increase in the
hybrid, the specific heat capacity decreases and the rate of decrease is higher when
Al2O3 ratio exceeds ZnO ratio. This non-linear relation between nanoparticle mixture
ratio and specific heat capacity can be a function of the difference between the
particle sizes of the constituent nanoparticles; with Al2O3-ZnO hybrid at 1:1 particle
mixture having the least number of particles and Al2O3-ZnO hybrid at 2:1 has the
most number of particles and smaller sized Al2O3 particles.

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4.2 Viscosity of Al2O3-ZnO water hybrid nanofluids

As outlined in the introduction, several parameters affect the properties of nanofluids.
As such, many nanofluids can present both Newtonian and non-Newtonian
behaviours. Therefore, It is important to note that from experimental findings Al2O3-
ZnO hybrid nanofluid at all selected mixture ratios exhibited Newtonian behaviour at
all the volume concentration and temperature values considered.
From Figure 11 and Figure 12 it is observed that both volume concentration and
temperature have a significant effect on the viscosity of the nanofluids. The effect of
volume concentration on dynamic viscosity of nanofluids at 25 °C and 65 °C is shown
in Figure 11. The viscosity of the nanofluids increases with an increase in volume

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concentration from 0.33% to 1.67% for the hybrid nanofluids, Al2O3 nanofluid and

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ZnO nanofluid. The phenomenon was observed at both 25 °C and 65 °C and is also
similar to the results of other studies [63,64]. This is probably because an increase in
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the particles in the fluid leads to a higher degree of agglomeration within the fluid, as
the particles begin to cluster, the viscosity of the fluids increases.
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Figure 12 shows the relationship between dynamic viscosity and temperature at a
volume concentration of 0.33% and 1.67%. For the considered volume concentration
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range, 0.33% and 1.67% present the minimum and maximum values for viscosity.
The viscosity of the nanofluid is seen to decrease with an increase in temperature
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between 25 °C and 65 °C. This is noticed for all the mixture ratios of the Al2O3-ZnO
hybrid nanofluid, the Al2O3 nanofluid and the ZnO nanofluid. First, an increase in
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temperature is certain to increase entropy within the fluid, as the fluid molecules and
nanoparticles gain kinetic energy. The increase in kinetic energy within the fluid
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reduces the viscosity in the nanofluid. Secondly, an increase in temperature increases

the intermolecular distance between nanoparticles and base fluid which in turn
reduces the viscosity of the nanofluids. Figure 12a and 12b show the nanofluids at a
volume concentration of 0.33% and 1.67% respectively. It is observed that while the
viscosity of the ZnO water nanofluid is the least at all the considered temperatures,
Al2O3 water nanofluid is only less than Al2O3-ZnO water hybrid nanofluid at 2:1
mixture ratio. This may be due to the total number of nanoparticles present in
nanofluids and their average particle sizes.
Figure 13 provides the variation of dynamic viscosity with the percentage mixture
ratios for the content of ZnO in the Al2O3-ZnO hybrid nanofluids. The 1:1 ratio shows
the least value for viscosity at all temperatures. The dynamic viscosity of composite

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nanofluids increases on either side of the 1:1 ratio with the gradient seen to increase
with a higher ratio of Al2O3. It can be concluded that the distribution of dynamic
viscosity for all mixture ratios is always higher than that of the 1:1 ratio at all
temperatures studied. The maximum viscosity increase was 96.37%, 95.87% and
95.1% for mixture ratios of 2:1, 1:2 and 1:1 respectively. The relationship between
viscosity and mixture ratios is observably non-linear as a “deeping effect” is noticed
at a 1:1 mixture ratio. This “deeping effect” can probably be caused by the difference
in the shear flow resistance of the different nanoparticles present in the hybrid and the
difference between sizes of the nanoparticles.
For heat transfer, fluids are often expected to have high specific heat capacity, high

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thermal conductivity and low viscosity. Therefore, of the three mixture ratios

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considered, the Al2O3-ZnO hybrid nanofluid at 1:1 mixture ratio has the most specific
heat capacity and the least viscosity which makes Al2O3-ZnO hybrid nanofluid at 1:1
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mixture ratio the most ideal for heat transfer applications.
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5. Conclusion and recommendations
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This work presents an experimental investigation of the specific heat capacity and
viscosity of Al2O3-ZnO water hybrid nanofluids for three different mixture ratios at a
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volume concentration of 0.33%, 0.67% 1.00%, 1.33% and 1.67% and temperatures
ranging between 25 °C and 65 °C. The experimentally measured results for the hybrid
nanofluids were compared to theoretical models obtained from literature with the
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following significant findings:

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 The classical numerical models do not accurately predict the experimentally

obtained values of both specific heat capacity and viscosity. This might be
because these models do not contain all the factors that affect the rheological
behaviours of these nanofluids.
 The specific heat capacity of the hybrid nanofluids reduces with an increase in
volume concentration and also increases with rising temperature values.
 At all volume concentrations and temperature range considered, Al2O3-ZnO
hybrid nanofluid at 1:1 (50 vol.% Al2O3: 50 vol.% ZnO) ratio presents the
highest value for specific heat capacity when compared to 2:1(66.66 vol.%
Al2O3: 33.34 vol.% ZnO) and 1:2 (33.34 vol.% Al2O3: 66.66 vol.% ZnO)
mixture ratio. Also, the gradient of specific heat capacity is steeper when the

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ratio of Al2O3 exceeds the ratio of ZnO.

 The specific heat capacity model used in the study could somewhat accurately
predict the relationship between the nanoparticle volume concentration and the
specific heat capacity of the nanofluids. The model, however, grossly
overestimates the value of specific heat and cannot account for the “peaking
effect” observed at a 1:1 (50 vol.% Al2O3: 50 vol.% ZnO) mixture ratio.
 The viscosity of the hybrid nanofluids increases with an increase in the
volume concentration and decreases with decreasing temperature values.
 At all volume concentrations and temperature ranges considered, Al2O3-ZnO
hybrid nanofluid at 1:1 (50 vol.% Al2O3: 50 vol.% ZnO) ratio presents the

of
least viscosity values compared to the other mixture ratios of 2:1 and 1:2.


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The viscosity model used in the study significantly underestimates the value of
viscosity of the nanofluids and cannot account for the “deeping effect”
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observed at the 1:1 mixture ratio.
 Of the three mixture ratios considered, the Al2O3-ZnO hybrid nanofluid at 1:1
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mixture ratio has the most specific heat capacity and the least viscosity:
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making it the most ideal mixture ratio for heat transfer applications.
 The correlation models presented for both the specific heat capacity and
viscosity of the hybrid nanofluids accurately accounts for the effect of
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nanoparticle mixture ratio and shows a high R2 value of 99.2% and 93.34%
respectively.
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Acknowledgement
The authors would like to acknowledge the assistance of Hacettepe University
Advanced Technologies Research and Application Centre in Ankara, Turkey in
carrying out this study.

Nomenclature
Cf : Correlation factor
Cp : Specific heat capacity (kJ/kg.K)
d: Diameter of nanoparticles (nm)
h: Nanolayer thickness (m)
NA: Avogadro constant
k: Thermal conductivity (W/m.K)

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R Universal gas constant

r: radius of nanoparticle (m)
Vol: Volume (ml)
W: weight (gram)

Greek symbols
𝛿 distance between particles (nm)
μ dynamic viscosity (Pa s)
ρ density (kg/m3)
φ volumetric fraction of nanoparticles (%)

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Subscript/ superscript
a Alumina

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bf base fluid
nf nanofluids -p
np nanoparticles
z Zinc Oxide
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Abbreviations
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ASHRAE American Society of Heating, Refrigeration and Air-condition engineers

MWCNT Multi-wall carbon nanotubes
na

NP Nanoparticles
SEM Scanning electron microscope
XRD X-ray diffraction
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Chemical Formula
Al2O3 Aluminum Oxide
CuO Copper Oxide
Fe Iron
SiO2 Silicon oxide
ZnO Zinc Oxide

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Figure 1: SEM image of (a) Al2O3 (b) ZnO nanoparticles.
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Figure 2: XRD characterization for ZnO, Al2O3, and Al2O3 - ZnO water nanofluids.

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Figure 3: Comparison of the predictive model and experimental model for the
dynamic viscosity of the hybrid nanofluids.
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Figure 4: Viscosity comparison between predictive model and experimental model for
varying mixture ratio in Hybrid.
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Figure 5: Comparison between the predictive model and experimental model for the
specific heat capacity of hybrid of Al2O3: ZnO at (a) 1:1 (b) 1:2 and (c) 2:1

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Figure 5: Comparison between the predictive model and experimental model for the
specific heat capacity of hybrid of Al2O3: ZnO at (a) 1:1 (b) 1:2 and (c) 2:1
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Figure 6: Experiment and model comparison for the effective specific heat capacity of

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Al2O3-ZnO hybrid nanofluids at varying mixture ratios.

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Figure 7: Comparison between experimental results and the results of (a) Specific
heat model and (b) Viscosity model

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Figure 8: Specific heat capacity variation with volume concerntration (a) at 25OC (b)
at 65OC

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Figure 9: Specific heat capacity variation with temperature (a) at 0.33% (b) at 1.67%

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Figure 10: Specific heat varying mixture ratio in Hybrid (a) at volume concentration
1.67% (b) at 25oC

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Figure 11: Viscosity variation with volume concentration (a) at 25 °C (b) at 65 °C.

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Figure 12: Viscosity variation with Temperature (a) at 0.33% volume concentration
(b) at 1.67% volume concentration

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Figure 13: Viscosity varying mixture ratio in Hybrid at 25oC
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Table 1: Zeta potential analysis.

Zeta Potential analysis at 1.67% vol. conc.
pH of solution 1 4 7 10 12

Zeta potential (mV)

Al2O3 32 26 12 -28 -39

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ZnO 31 28 14 -20 -25
Al2O3: ZnO (1:2) 28 25 6 -23 -32

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Al2O3: ZnO (2:1) 32 29 8 -15 -27
Al2O3: ZnO (1:1) 35 33 6 -23 -39
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Table 2. Limitations of classical models for viscosity predictions of hybrid nanofluids.

Models Viscosity formula Factors considered Model Limitations
1 Einstein [34] 𝜇𝑒𝑓𝑓 𝜑<0.0245 Einstein predictive model is limited to
= 1 + 2.5𝜑
𝜇𝑓
volume concentration below 0.0245.
Also, the equation’s only dependent

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and cannot distinctly differentiate
between φ𝑎 𝑎𝑛𝑑 φ𝑧 .

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2 Mooney 𝜇𝑒𝑓𝑓 2.5𝜑 Improved on Einstein for The only dependent variable
= 𝑒 1−𝑘𝜑
Model [35] 𝜇𝑓 higher concentration
-p considered by the equation is the total
where k is a constant volume concentration and cannot
(1.35<k<1.91) distinctly differentiate between
φ𝑎 𝑎𝑛𝑑 φ𝑧 concentration ratios
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3 Krieger- 𝜇𝑒𝑓𝑓 𝜑 −2.5𝜑𝑚 Consider the shear This predictive model has shown
= 1−
Dougherty 𝜇𝑓 𝜑𝑚 viscosity of mono- considerable deviation from
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Model [36] dispersed particles where experimental studies

𝜑𝑚 is the maximum
particle packing fraction,
na

which varies from 0.495

to 0.54
𝜑
4 Nielsen Improved on Einstein for While this model performs
𝜇𝑒𝑓𝑓 = (𝑒 1−𝜑𝑚 ).𝜇𝑓
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Power-law higher concentration significantly better than

model [37] considering a Poisson's Einstein Model at higher
ratio of less than 0.50 concentration it still deviates from
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experimentally measured data

5 Brinkman 1 The model combined The only dependent variable
𝜇𝑛𝑓 = 𝜇𝑏𝑓 .
model [48] (1 − 𝜑)2.5 Darcy’s law and the considered by the equation is the total
Navier-Stokes equations volume concentration and cannot
to account for distinctly differentiate between
dissipation of kinetic φ𝑎 𝑎𝑛𝑑 φ𝑧 concentration ratios
energy.
6 Batchelor 𝜇𝑒𝑓𝑓 = (1 + 2.5𝜑 + 6.5𝜑2 )𝜇𝑓 Modified Einstein The equation only dependent variable
Model [38] equation accounting for considers only Total volume
Brownian motion concentration and cannot distinctly
properties within the differentiate between φ𝑎 𝑎𝑛𝑑 φ𝑧
fluid concentration ratios

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Table 3. Limitations of models for specific heat capacity predictions of hybrid

nanofluids.
Models Specific heat capacity formula Model Limitations
1 Mixture Theory 𝐶𝑛𝑓 = 𝐶𝑛𝑝 𝜑 + 𝐶𝑤 (1 − 𝜑) Specific heat capacity model

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[39] significantly deviates from
experimental test [46].

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2 Thermal 𝜌𝑛𝑓 𝐶𝑛𝑓 = 𝜌𝑛𝑝 𝐶𝑛𝑝 𝜑 + 𝐶𝑏𝑓 𝜌𝑏𝑓 (1 − 𝜑) Shows wide deviations as high as 7%
equilibrium -p [52]
model [51]
3 Thermal 𝜑𝜑𝑛𝑝 𝐶𝑛𝑝 + 𝜑𝑏𝑓 𝜌𝑏𝑓 𝐶𝑏𝑓 Shows significant deviation from
𝐶𝑝,𝑡 =
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equilibrium 𝜑𝑛𝑝 𝜌𝑛𝑝 + 𝜑𝑛𝑓 𝜌𝑛𝑓 experimental results.
model [14]
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Table 4: Thermo-physical model regression constants

Regression constants Model
accuracy
a1 a2 a3 a4 a5 a6 a7 R2 rms
Cp -0.29993 0.00227 1.52321E-06 2.82505 - -2.95909 -27.55833 99.28 0.005
model 3.05882

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μ 349.2042 - 0.00235 - 234.274 235.0495 14376.132 93.34 1.62
model 1.68272 217.9377 3

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Highlights
 The specific heat and viscosity of Al2O3-ZnO dispersed in water is
investigated.
 Al2O3-ZnO water nanofluids at 2:1 mixture ratio have a maximum viscosity
increase of 96.37%.
 Maximum specific heat decrease of the Al2O3-ZnO water nanofluids was
30.12%.
 Al2O3-ZnO hybrid nanofluid at 1:1 mixture ratio is most ideal for heat transfer
application.
 Theoretical models do not account for the effect of mixture ratio in the
nanofluid.

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