Journal of Thermal Analysis and Calorimetry (2019) 137:879–901

https://doi.org/10.1007/s10973-019-08006-0
(0123456789().,-volV)(0123456789().
,- volV)

Effects of temperature and particles volume concentration

on the thermophysical properties and the rheological behavior of CuO/
MgO/TiO2 aqueous ternary hybrid nanofluid

Experimental investigation

S. M. Mousavi1 • F. Esmaeilzadeh1 • X. P. Wang2

Received: 23 November 2018 / Accepted: 3 January 2019 / Published online: 17 January 2019
 Akadémiai Kiadó, Budapest, Hungary 2019

Abstract
In the present study, the impacts of nanoparticles volume concentration and temperature on the thermophysical properties and
the rheological behavior of water-based CuO/MgO/TiO2 ternary hybrid nanofluids were elucidated. Five types of CuO/MgO/
TiO2 aqueous THNFs (ternary hybrid nanofluids) including A (33.4 mass% CuO/33.3 mass% MgO/33.3 mass% TiO2),
B (50 mass% CuO/25 mass% MgO/25 mass% TiO2), C (60 mass% CuO/30 mass% MgO/10 mass% TiO2), D (25 mass%
CuO/50 mass% MgO/25 mass% TiO2) and E (25 mass% CuO/25 mass% MgO/50 mass% TiO2) were fabricated. All
experiments were performed under the temperature range of 15–60 C in the solid volume concentration range of 0.1–0.5%.
The experimental results demonstrated that the rheological and the thermophysical properties of THNFs depend not only on
the nanoparticles volume concentration, but also on the temperature of THNFs. All the THNFs demonstrated Newtonian
behavior. The dynamic viscosity and the thermal conductivity of THNFs increased with enhancing solid particles volume
concentration and temperature. The highest increment in thermal conductivity as compared to distilled water was obtained for
the C type of THNFs at 0.5 solid vol% in 50 C. The specific heat capacity of THNFs first decreased up to 35 C and then
increased with raising temperature. The highest reduction of specific heat capacity of THNFs was found for the C type of
THNFs. The surface tension of B and C types of THNFs increased with the particles volume concentration enhancement. In
the cases of low particles volume, the surface tension of THNFs was lower than that of the distilled water, for a concentration
of the nanoparticles of 1.0%. Four new correlations were developed to predict the viscosity, thermal conductivity, specific
heat capacity and density of the THNFs. All the proposed correlations had a satisfactory accuracy of ± 1%.

Keywords Ternary hybrid nanofluids  Thermal conductivity  Viscosity  Specific heat capacity  Volume concentration

List of symbols Subscripts

Cp Specific heat capacity, J (gK)-1 bf Base fluid
K Thermal conductivity, W (mK)-1 nf Nanofluid
T Temperature, C np Nanoparticles

Abbreviations
& X. P. Wang DW Distilled water
wangxp@xjtu.edu.cn SDS Sodium dodecyl sulfate
1
Department of Chemical and Petroleum Engineering, School
NPs Nanoparticles
of Chemical and Petroleum Engineering, Enhanced Oil and THNFs Ternary hybrid nanofluids
Gas Recovery Institute, Advanced Research Group for Gas
Condensate Recovery, Shiraz University, Greek symbols
Shiraz 7134851154, Iran
q Density, g cm-3
2
Key Laboratory of Thermo-Fluid Science and Engineering, u Volume fraction
Ministry of Education, Xi’an Jiaotong University,
Xi’an 710049, Shaanxi, People’s Republic of China
l Dynamic viscosity, mPa s

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880 S. M. Mousavi et al.

Introduction range of 15–50 C with the particles volume concentra-

tions of less than 0.8%. The results showed that the thermal
Nanofluid is a word that was introduced by Choi [1] to conductivity of CuO–water/EG nanofluid is higher than
create stable colloidal suspensions of nanoparticles in usual that of Al2O3–water/EG nanofluid. Additionally, a new
base fluids such as oil, water and ethylene glycol. empirical correlation was proposed for the thermal con-
Nanofluids that were made by dispersing nanoparticles into ductivity of each of the nanofluids. Sundar et al. [15] ful-
some conventional liquids were suggested as a new heat filled an experimental work on MWCNT/Fe3O4–water
transfer fluid. Nanofluids offered better potentials to hybrid nanofluid at the temperature range of 20–60 C with
improve the thermo-physical and the rheological properties the particles volume fractions of less than 0.003. The
relative to the conventional liquids. Therefore, nanofluids results showed that the effective thermal conductivity and
have attracted great attention due to their potential the dynamic viscosity of the nanofluids enhanced by 29%
advantages in many applications such as microelectronics, and 1.5 times at 0.3 vol% and 60 C, respectively.
energy supply and transportation. Madhesh et al. [16] experimentally performed the thermal
Also, low dynamic viscosity of some nanofluids has conductivity and the friction factor of Cu/TiO2–water
made them appropriate for the pumping applications, but hybrid nanofluid at 5–80 C under the volume concentra-
only a few studies have been conducted on the thermo- tions range of 0.1–1 vol%. They concluded that the hybrid
physical and rheological properties of the hybrid nanofluids improved the thermal and rheological properties
nanoparticles [2–8]. The opinion of fabricating hybrid of the base fluid as compared to the singular nanofluid. In
nanofluids is to favor an additional improvement of heat another work, GNP/Ag–water hybrid nanofluid was pre-
transfer and pressure drop characteristics by trade-off pared by Yarmandet et al. [17], and its thermal conduc-
among advantages and disadvantages of individual sus- tivity and viscosity were measured. The results showed that
pension, attributed to a high aspect ratio, superior thermal its thermal conductivity and viscosity enhanced by 22.22%
network and synergistic impact of nanoparticles. By and 1.3 times at 0.1 mass% of nanoparticles in 40 C,
selecting an appropriate combination of particles manu- respectively. Soltani et al. [18] studied the dynamic vis-
factured hybrid nanofluid that positive features can be cosity of MWCNT/MgO-EG hybrid nanofluid. The vis-
recovered, and infelicities can be hidden owing to their cosity of these nanofluids at various particles volume
synergistic impact [9, 10]. fractions of 0.1–1% was measured at 30–60 C. The results
Baghbanzade et al. carried out a laboratory study on the indicated that the relative viscosity enhances when the
effective thermal conductivity of SiO2/multiwall carbon solid volume concentration increases from 0 to 1%.
nanotubes (MWCNTs)–water hybrid nanofluid at the Takabi et al. [19] evaluated the thermal behavior of Al2O3/
temperature range of 25–40 C for the solid volume con- Cu–water hybrid nanofluid at 30 C with the solid volume
centration of 0.1, 0.5 and 1% [11]. Their results showed fractions of less than 2%. Hybrid nanofluid indicated better
that the effective thermal conductivity increases with results than Al2O3/water and Cu/water nanofluids, individu-
enhancing the particles volume concentration. The per- ally. The thermal conductivity of GNP/Pt/water nanofluid
centage of thermal conductivity of hybrid nanofluid was investigated by Yarmand et al. [20]. The results
enhancement was reported between the percentage of demonstrated an enhancement of 17.7% at 0.1 mass% of
thermal conductivity enhancement of MWCNT–water nanofluids in 40 C. An experimental investigation was
nanofluid and SiO2–water nanofluid. Fabrication of SiO2/ carried out on ZnO/Ti-EG nanofluid by Toghraie et al. [21]. It
MWCNTs–water hybrid nanofluid improved the thermal could be seen that the thermal conductivity enhancement of
properties of water than silica–water nanofluid. Amiri et al. hybrid nanofluid at higher volume fractions of nanoparticles
[12] investigated the stability, dynamic viscosity, shear is more than that at lower volume fractions.
stress and thermal conductivity of multiwall carbon nan- Eshgarf et al. [22] studied the rheological behavior of
otubes/Ag-gum arabic and multiwall carbon nan- MWCNT/SiO2-EG/water hybrid nanofluid functionalized
otubes/cysteine-gum arabic hybrid nanofluids. High by COOH at the temperature range of 27.5–50 C, con-
thermal conductivity, fairly good stability and appropriate centration range of 0.0625–2 vol% and the shear rate range
viscosity of MWCNTs/Ag-gum arabic nanofluid make it a of 0.612–122.3 s-1. Their results revealed that the hybrid
suitable nanofluid as a superior cooling agent in thermal nanofluid had a pseudo-plastic rheological behavior.
systems. Aravind et al. [13] prepared graphene/MWCNT- Sekhar et al. [23] measured the viscosity and the specific
DW/EG hybrid nanofluid at 25 C in solid volume con- heat capacity of water-based Al2O3 nanofluid at the solid
centration of less than 0.4%. Sundar et al. [14] experi- volume concentration of 0.01–1% under the temperature
mentally examined the thermal conductivity of Al2O3– range of 25–45 C. Their results demonstrated a nonlinear
water/EG and CuO–water/EG nanofluid at the temperature increase in dynamic viscosity with increase in volume
fraction; however, the specific heat capacity of this

123
Effects of temperature and particles volume concentration on the thermophysical properties… 881

nanofluid declined by enhancing volume fraction. The are not accurate in foretasting the thermal conductivity of
reasons for viscosity enhancement and heat capacity nanofluids. The incidence of convection has to be refrained
decrement were the aggregation of nanoparticles and in base fluids to prosperously evaluate their thermal con-
thermal diffusivity enhancement, respectively. The effect ductivity. Furthermore, the attendance of dispersed
of CuO-distilled water nanofluids on the thermo-physical nanoparticles in base fluids can bring a main difficulty for
properties of distilled water was experimentally investi- evaluation of the values of viscosity, and thermal con-
gated at the solid volume concentration of 0.1–0.5% under ductivity as the uniformity of the medium is to be held.
the temperature range of 20–80 C by Kumar et al. [24]. The Eapen’s mean-field model [35] interference the
Their results showed that the nanofluid density increases nanoparticles shapes in parallel or perpendicular to the
from 0.93 to 1.66% by increasing the volume fraction of direction of heat flux. The parallel model was expressed as:
nanoparticles and decreases with the temperature knf ¼ ð1  uÞkbf þ uknp ð4Þ
enhancement. Also, the viscosity increased from 10.5 to
65.2% with increasing the volume fraction and decreasing Lu and Li [36] model introduced the correlation for
the temperature. The heat capacity of nanofluids decreased predicting the viscosity of nanofluids by considering near-
at first and then increased with increasing temperature. and far-field pair interaction which is presented as follows:
Additionally, it decreased with enhancing the nanoparticles  
knf ¼ kbf 1 þ 2:25u þ 2:27u2 ð5Þ
concentration. The dynamic viscosity of CuO/water
nanofluids increased about 0.68–2% with decreasing tem- where lnf, lbf, knf, kbf and u are the viscosity of the
perature. The results also showed that the thermal con- nanofluid and the base fluid, thermal conductivity of
ductivity of the nanofluids increased about 22.22% and nanofluid and base fluid and the volume fraction, respec-
their viscosity enhanced relative to the base fluid. Zyla [25] tively. Lu and Li model applied for spherical and non-
experimentally studied the thermo-physical properties of spherical nanoparticles. These models were not able to
yttrium aluminum garnet-ethylene glycol nanofluid under predict the thermal properties, accurately.
the temperature range of 0–60 C and the shear rate of 10 Considering the main subject, various methods have
to 1000 s-1 in the volume concentrations of less than 6%. been suggested to evaluate the values of thermal conduc-
Their results indicated that the nanofluids had Newtonian tivity of nanofluids over the preceding few years. The most
behavior and their viscosity increased with the nanoparti- prevalent methods for the evaluation of the values of effi-
cles volume fraction enhancement and decreased with cient thermal conductivity of nanofluids are the tempera-
increasing the temperature. ture oscillation procedure [37], transient hot-wire technique
There are some theoretical studies on the dynamic vis- [38], cylindrical cell technique [39], steady-state procedure
cosity and the thermal conductivity of nanofluids as a [40], and 3-omega technique [41–46]. Sixty-eight per-
function of volume fraction and temperature [26–29]. centage of the published literature had used the transient
Some theoretical models have been presented to predict the hot-wire method [47]. The researchers suggested some
thermal conductivity and dynamic viscosity of nanofluiuds. correlations for thermal conductivity and viscosity in
However, these models cannot predict exactly the experi- accordance with the experimental data [48].
mental data, so it is essential to peruse about the nanofluids Literature studies showed that a few studies were con-
viscosity and thermal conductivity increment mechanisms. ducted on the thermo-physical and the rheological prop-
Pak and Cho proposed a correlation for the prediction of erties of the binary hybrid nanofluids, but there was not any
nanofluid viscosity as a function of nanoparticles concen- work on the rheological and the thermo-physical properties
tration and base fluid viscosity as follows [30]: of the ternary hybrid nanofluids. Therefore, the plans of the
  present study were to investigate the thermophysical and
lnf ¼ lbf 1 þ 2:5u þ 6:2u2 ð1Þ
the rheological properties of A, B, C, D and E types of
Batchelor predicted the dynamic viscosity for isotropic THNFs. The dynamic viscosity, thermal conductivity,
suspensions as follows [31]: specific heat capacity and density of THNFs were experi-
  mentally measured at the temperature range of 15–60 C
lnf ¼ lbf 1 þ 39:11 þ 533:9u2 ð2Þ
with the solid volume concentration of 0.1–0.5%. In
Wang et al. [32] obtained a correlation for measuring the addition, four new correlations were proposed for the
dynamic viscosity of nanofluids: prediction of the viscosity and thermo-physical properties
  of THNFs in the temperature range of 15–60 C with the
lnf ¼ lbf 1 þ 0:723u þ 123u2 ð3Þ
solid volume concentration of 0.1 to 0.5%.
There are several classical approaches like Maxwell’s
theory [33] and Hamilton and Crosser approach [34] which

123
882 S. M. Mousavi et al.

Materials and methods 2400

2200
2000

Synthesis of the hybrid nanocomposite 1800

Intensity
1600
1400

Five types of hybrid nanocomposites containing A (33.4 mass% 1200

1000
CuO/33.3 mass% MgO/33.3 mass% TiO2), B (50 mass% CuO/ 800

25 mass% MgO/25 mass% TiO2), C (60 mass% CuO/30 mass% 600

400
MgO/10 mass% TiO2), D (25 mass% CuO/50 mass% MgO/25 20 30 40 50 60 70 80
2θ°
mass% TiO2) and E (25 mass% CuO/25 mass% MgO/50 (a)
mass% TiO2) were fabricated by the thermochemical procedure
including of spray-drying, oxidation of precursor powder,
reduction by hydrogen and homogenization. Copper oxide
nitrate, nitrates of magnesium oxide and titanium dioxide were
first added to water and mixed the solution vigorously. After-
ward, ammonium hydroxide was added into the solution under
stirring drop by drop. This solution was filtrated, and the sedi-
ment was washed by distilled water. The mixture was then dried
at 170 C by a spray dryer (SPD-P-111, Techno Search
Instrument Company, India) to obtain the precursor powder. (b)

This powder was then heated at 680 C for 80 min by SiC 2400
2200
electric heating elements (RX2, MHI (Micropyretics Heaters 2000
1800
International Company, USA) to form a powder combination of
Intensity
1600
1400
CuO, MgO and TiO2 nanocomposite with different mass per- 1200
cents. Next, these hybrid nanocomposites were heated at 540 C 1000
800
Cu Cu
Mg
in the presence of hydrogen gas by a furnace (EX.1700-3L, 600
Nb Si S Al
K N C
400
Ti a Ti a
Extiton Company, Iran). The hybrid nanocomposites were then Cu0 1 2 3 4 5 6 7 8 9 10
Energy/eV
ball milled in 80 min for obtaining the homogeneous hybrid (c)
nanocomposites.
Fig. 1 a TEM image of C-type nanocomposite, b XRD pattern of
C-type nanocomposite and c EDS pattern of C-type nanocomposite
Characterization of CuO/MgO/TiO2 hybrid
nanocomposite

TEM image (Transmission Electron Microscope), EDS Table 1 Certificate of analysis

Element mass%
of C-type nanocomposite by
analysis (Energy-Dispersive X-ray Spectroscopy) and XRD EDS OK 18.14
analysis (X-Ray Diffraction, Siemens D-500, 45 kV and
Cu K 34.98
40 mA, h: 20–80) images of the C-type nanocomposite
Mg K 22.45
are demonstrated in Fig. 1.
Ti K 20.76
The reflections in the XRD pattern were identified as
corresponding to the cubical phases of MgO, TiO2 and Si L 0.67
CuO nanoparticles using Joint Committee on Powder Ca L 0.64
Diffraction Standards. The average size of the C-type Na L 0.28
nanocomposite was calculated to be 100 nm using Scherrer KL 0.72
correlation. TEM image of the C-type nanocomposite SL 0.36
shows that its morphology is somehow spherical and the C Nb L 0.43
type of nanocomposite diameter is 25 nm. The information Al L 0.57
about the hybrid chemical composition of C type of THNFs Totals 100.00
was obtained by EDS analysis as shown in Fig. 1 and
Table 1. The results confirm the presence of magnesium,
titanium, copper and oxygen elements in the C type of
nanocomposite combination. Properties of CuO nanoparticles, MgO nanoparticles,
TiO2 nanoparticles and C-type nanocomposite were
experimentally measured and are given in Table 2.

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Effects of temperature and particles volume concentration on the thermophysical properties… 883

Table 2 Properties of the metal oxides (CuO, MgO and TiO2) and C-type nanocomposite
Parameter CuO MgO TiO2 C-type nanocomposite

Purity, vol% 99% 99% 99% 99%

Color Black White White Black
APS (average particle size), nm 40 25–45 18–23 25
Morphology Nearly spherical Nearly spherical Nearly spherical Nearly spherical
True density, g cm-3 6.41 3.57 3.95 6.23
Thermal conductivity, W m-1K-1 69 5.11 5.41 71.56
Specific heat capacity, J kg-1K-1 535 0.852 0.835 456.755

Fabrication of hybrid nanofluid measured six times for each temperature, and the average
values were reported.
In the present study, all THNFs with different solid parti-
cles volume concentrations from 0.1 to 0.5% were fabri- Dynamic viscosity measurement
cated using two-step method by dispersing a specified
amount of hybrid nanocomposites in distilled water toge- DV-II? Pro Brookfield viscometer (DV-II? Pro, Brook-
ther with SDS as a surfactant by using an ultrasonic field Company, USA) connected to a water bath was used
homogenizer (ultrasonic homogenizer UP400A, 400 W, to measure the viscosity of THNFs at the temperature range
20 kHz, UTDC, Iran). To get a uniform mixture, the of 15–60 C with the solid volume concentration range of
nanofluids were stirred by a magnetic stirrer for 90 min. 0.1–0.5%. The Brookfield viscometer was calibrated with
The solid particles volume concentration could be calcu- distilled water at the room temperature which showed an
lated by the following formula [49]. acceptable accuracy (± 1.0%). All the experiments were
h i carried out in the shear rate range of 10–80 s-1. The
wCuOþMgOþTiO2
qCuOþMgOþTiO2 dynamic viscosity and shear stress data were recorded to
;  100 ¼ hw i h i ð6Þ
CuOþMgOþTiO2
þ wwater investigate the rheological behavior of THNFs.
qCuOþMgOþTiO2 qwater

qCuOþMgOþTiO2 Density measurement

   
ðqCuO  wCuO Þ þ qMgO  wMgO þ qTiO2  wTiO2
¼ Anton Paar digital density meter (DMA 4500M, Anton
wCuO þ wMgO þ wTiO2 Paar Company, Austria) was used to measure the amounts
ð7Þ of THNFs density at the temperature range of 15–60 C
where u is the volume concentration of nanocomposite, w with the solid volume concentration of 0.1–0.5%. For
denotes the mass of nanocomposite, and q is the density. confidence, the density of DW was measured and com-
pared with the literature data [50]. The accuracy of the
Thermal conductivity measurement instrument was reported about 5 9 10-5 g cm-3.

The thermal conductivity of THNFs was measured using a Specific heat capacity measurement
KD2 Pro thermal properties analyzer (Decagon Devices,
Inc., USA) under the temperature range of 15–60 C and A differential scanning calorimeter (DSC1 STAR, Mettler
nanoparticles volume concentration of 0.1–0.5 vol%. The Toledo, USA) was used to measure the specific heat
measurement technique of KD2 Pro thermal properties capacity of THNFs. The differential scanning calorimeter
analyzer for thermal conductivity of nanofluids is hot-wire (DSC) is the most frequently device used for thermal
method. This device consists of a handheld controller and analysis technique. The DSC measures the enthalpy
various sensor needles. The KS1 sensor needle is used for changes of samples due to the changes in specific heat
measuring the thermal conductivity of THNFs. The accu- capacity of THNFs as a function of temperature. In order to
racy of the sensor was within 5%. This device was cali- dry THNFs, water was evaporated by an oven and then the
brated with distilled water which had good agreement with dried samples were placed in the aluminum pans. The
standard data [50]. The mentioned properties were specific heat capacity was calculated from heat flow
experimental data points using the Stare software of

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884 S. M. Mousavi et al.

Mettler Toledo DSC1 system. A standard method for Table 3 Zeta potential for THNFs at various ultrasonication times for
measuring the specific heat capacity is Sapphire as a ref- 5 days after preparation of THNFs
erence. At first, the heat capacity of Sapphire was measured THNFs Solid volume concentration (vol%) Zeta potential
to investigate the validity of this method. The accuracy of
Sonic. time
temperature for this instrument is ± 0.2 K. The DSC
instrument was calibrated with indium, aluminum and melt 120 min 150 min
transition of cyclohexane. In order to estimate the heat A type 0.1 46.46 52.53
capacity of THNFs, the two sample pans were kept empty
0.5 47.34 49.68
to reach the baseline heat flux (QO). Then, one of the two
B type 0.1 41.23 42.12
pans was filled with the reference sample, and the other one
0.5 37.54 39.22
was kept empty. The reference heat flux was measured
C type 0.1 44.22 46.74
(Qref), and finally, a pan was filled with the dried THNF.
0.5 41.11 43.33
Then, two pans were placed into the calorimeter, and the
D type 0.1 34.23 30.12
sample heat flux was recorded (Qsample). The thermal cycle
0.5 32.33 27.11
for all steps was fixed. The heat capacity of the sample was
E type 0.1 34.56 29.98
calculated from following equation [51]:
  0.5 32.34 26.67
Qsample  QO  
Cp;sample ¼ mref  msample Cp;ref ð8Þ
ðQref  QO Þ
where Cp,ref, mref and msample denote the specific heat
capacity of sapphire, the mass of sapphire and the mass of Table 4 Zeta potential for THNFs at various ultrasonication times for
10 days after preparation of THNFs
sample, respectively.
THNFs Solid volume concentration/vol% Zeta potential
Sonic. time
Results and discussion 120 min 150 min

Stability of THNFs A type 0.1 44.35 50.17

0.5 45.88 47.23
Stability is one of the important factors that has an effect B type 0.1 39.88 41.77
on the performance of THNFs. A THNF with low stability 0.5 36.65 38.17
tends to deposit due to the agglomeration of nanocom- C type 0.1 42.89 44.11
posites in the base fluid [52]. This phenomenon causes to 0.5 40.69 41.96
develop challenges such as clogging of pipelines and the D type 0.1 32.76 28.96
decrement of thermal conductivity of nanofluids. There- 0.5 30.76 25.89
fore, it is vital to study the stability of the fabricated E type 0.1 32.11 26.45
THNFs. To do so, SDS as a surfactant along with an 0.5 30.75 25.46
ultrasonic homogenizer is applied to amend the distribution
of suspended nanoparticles. Various amounts of SDS were
dispersed in THNFs to attain the optimum value of SDS potential. If the zeta potential close be to ± 30 mv, the
concentration. Ultrasonication time was one of the impor- nanofluid is comparatively stable. The stability is favor-
tant parameters on the stability of THNFs. The stability able, whenever it ranges between ± 30 and ± 45 mv, and
time of THNFs was determined by means of taking SEM higher than this value up to ± 60 mv, an excellent stability
images at various ultrasonication times and also measuring for nanofluids can be acceded.
zeta potential. Zeta potential was measured by using the The zeta potential of THNFs for various ultrasonication
Zetasizer apparatus (Nano ZS90, Malvern Instruments Ltd, times with different volume concentrations is given in
UK) working based on the laser Doppler micro-elec- Tables 3–9. All nanofluids have good stability, except D
trophoresis, dynamic light scattering and static light scat- and E types of THNFs. Also, the influence of ultrasoni-
tering methods. Ghadimi et al. [53] demonstrated that the cation time and the mass percent of SDS on the stability of
high zeta potential shows a stable suspension, while THNFs are demonstrated in Figs. 2 and 3. The optimum
THNFs with low Zeta potential make a quick deposition of values of ultrasonication time for A type, B type, C type, D
nanoparticles. Vandsburger [54] reported the stability of type and E type of THNFs are found to be about 170, 160,
nanofluids changes depending on the quantity of zeta 120, 120 and 150 min, respectively. The optimum values
of SDS concentration in mass% and stability time for A

123
Effects of temperature and particles volume concentration on the thermophysical properties… 885

type, B type, C type, D type and E type of THNFs are Table 5 Zeta potential for THNFs at various ultrasonication times for
found to be 0.4 mass%, 0.44 mass%, 0.49 mass%, 0.52 15 days after preparation of THNFs
mass% and 0.5 mass%, respectively. THNFs Solid volume concentration/vol% Zeta potential
The stability and dispersion characteristics of THNFs
Sonic. time
were investigated by taking SEM images before and after
the sonication operation as shown in Fig. 4. 120 min 150 min

A type 0.1 41.78 49.38

Rheological behavior of THNFs 0.5 42.23 46.56
B type 0.1 37.45 39.48
Effect of temperature and solid volume concentration 0.5 35.22 37.32
on dynamic viscosity of THNFs
C type 0.1 41.76 43.36
0.5 37.44 38.67
The dynamic viscosity of all the THNFs with solid volume
D type 0.1 39.11 36.73
concentrations of 0.1%, 0.2%, 0.3%, 0.4% and 0.5% was
0.5 28.44 23.26
measured at the temperature ranges between 15 and 60 C.
E type 0.1 30.54 25.77
The results are presented in Fig. 5. It is obvious that the
0.5 28.09 22.67
dynamic viscosity of THNFs decreases with increasing
temperature due to the reduction in intermolecular inter-
actions between the molecules of THNFs. The dynamic
viscosity increases with the solid volume concentration
enhancement. It is found that the viscosity of THNFs Table 6 Zeta potential for THNFs at various ultrasonication times for
increases as compared to the base fluid at all temperatures 20 days after preparation of THNFs
and solid volume concentrations. The nano-clusters created THNFs Solid volume concentration/vol% Zeta potential
based on van der Waals forces between the particles would
Sonic. time
cause a greater increment in dynamic viscosity due to
barrier to the movement of base liquid layers on one 120 min 150 min
another [52]. Nanoparticles in water enhance the viscosity A type 0.1 40.42 47.65
of base fluid due to interactions between water molecules 0.5 40.65 44.02
and dispersed nanoparticles. Nanoclusters are created due B type 0.1 33.00 38.35
to the van der Waals forces between the nanoparticles, and
0.5 34.13 36.55
the size of nanoclusters would be larger by increasing the
C type 0.1 39.00 42.03
nanoparticles volume concentration. The nanoclusters
0.5 39.12 38.93
cause a higher enhancement in dynamic viscosity of water
D type 0.1 28.47 27.00
due to barrier the movement of base fluid layers on each
0.5 26.40 21.98
other. The experimental results showed that the viscosity of
E type 0.1 27.54 25.77
nanofluids increased with decreasing temperature. This
0.5 27.32 21.13
enhancement percentage was measured by the following
formula:
 
l  lbasefluid
%Enhancement ¼ nanofluid  100 ð9Þ
lbasefluid Effects of shear rate on shear stress and dynamic viscosity
-1
At shear rate of about 12 s , enhancements of about of THNFs
45.22%, 43.3%, 40%, 38.7 and 36.4% for E type, D type, A
type, B type, and C type of THNFs were obtained with the The influence of shear rate and solid particles volume
solid volume concentration of 0.5 vol% at the temperatures concentration at 55 C on the dynamic viscosity is shown
of 15, 55, 40, 60 and 60 C, respectively. in Fig. 6. The experimental data demonstrated that the
One of the reasons of the viscosity increment can be due dynamic viscosity of all the THNFs keeps almost constant
to the existence of great CuO nanoparticles. To the best of with increasing shear rate. The experimental data of shear
our knowledge, no experimental data have been reported stress at various shear rates and particles volume concen-
for the dynamic viscosity of CuO/MgO/TiO2 THNFs dis- trations at 55 C are also presented in Fig. 7. It is obvious
persed in water as a base fluid. that the rheological behavior of the THNFs is Newtonian.
Because, the variation of shear stress versus shear rate is
linear. Chen et al. [55] showed a significant enhancement

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886 S. M. Mousavi et al.

Table 7 Zeta potential for THNFs at various ultrasonication times for in heat transfer rate by using the Newtonian fluids. As a
25 days after preparation of THNFs result, Newtonian nanofluids are the good choices for the
THNFs Solid volume concentration/vol% Zeta potential heat transfer characteristics improvement.
Sonic. time
Dynamic viscosity correlation for different types of THNFs
120 min 150 min

A type 0.1 39.77 45.23 Figure 8 compares the experimental viscosity data of
0.5 40.00 4323 THNFs with the estimated values from Pak and Cho [42],
B type 0.1 31.25 36.44
Batchelor [43] and Wang [44] models. As can be seen, all
0.5 32.11 36.03
the mentioned models underpredict the dynamic viscosity
of THNFs. It is clear that Pak and Cho [42], Batchelor [43]
C type 0.1 37.64 40.56
and Wang [44] models are not able to estimate the dynamic
0.5 39.03 38.12
viscosity of B and C types of THNFs. However, Pak and
D type 0.1 27.78 25.44
Cho [42], Batchelor [43] and Wang [44] models treat the
0.5 25.13 20.00
experimental data of dynamic viscosity of D and E types of
E type 0.1 25.59 23.23
THNFs well. The results show that average absolute rela-
0.5 24.32 20.19
tive deviations for the models of Pak and Cho [42],
Batchelor [43] and Wang for A, B, C, D and E- types of
THNFs are found to be 14.8%, 16.7%, 21.2%, 2.3% and
2.1%, respectively.
The previous theoretical models presented previously
Table 8 Zeta potential for THNFs at various ultrasonication times for were not able to accurately predict the dynamic viscosity of
30 days after preparation of THNFs THNFs. Therefore, a correlation was developed to estimate
THNFs Solid volume concentration/vol% Zeta potential the dynamic viscosity of THNFs as a function of temper-
ature and particles volume concentration. The coefficients
Sonic. time
of the proposed correlation (Eq. 11) were created by
120 min 150 min minimization of following objective function using the
A type 0.1 37.64 44.87
Levenberg–Marquardt algorithm (LMA), Eq. 10.
PN 2
K¼1 ðlpred;K  lexp;K Þ
0.5 36.43 42.77
B type 0.1 31.12 35.64 LSM ¼ min ð10Þ
N
0.5 30.66 34.45
where lK is the dynamic viscosity in cp and N is the
C type 0.1 35.22 37.71
number of total data points. Subscripts pred and exp rep-
0.5 38.45 36.55
resent the predicted dynamic viscosity from the model and
D type 0.1 26.00 24.40
experimental dynamic viscosity, respectively. The adjusted
0.5 24.00 23.65
R2 of the proposed correlation is 0.992, demonstrating good
E type 0.1 24.05 22.11
accuracy of the equation in prediction of viscosity. The
0.5 22.66 19.10
absolute deviation between the values obtained from the
predicted correlation relative to the experimental data is
less than 1.5%. The results are shown in Fig. 9.

Table 9 Investigation the stability of THNFs at different days after preparation

THNFs Stability
5 days 10 days 15 days 20 days 25 days 30 days

A type Stable Stable Stable Stable Stable Stable

B type Stable Stable Stable Stable Stable Stable
C type Stable Stable Stable Stable Stable Stable
D type At sonic. time = 150 min and 0.5 vol% is unstable At sonic. time = 150 min is Unstable Unstable Unstable Unstable
unstable
E type At sonic. time = 150 min is unstable At sonic. time = 150 min is Unstable Unstable Unstable Unstable
unstable

123
Effects of temperature and particles volume concentration on the thermophysical properties… 887

Fig. 2 Influence of sonication 90

0.1 vol% 0.2 vol%
time on stability time of C-type 90 0.3 vol% 0.4 vol%
of THNFs with the SDS 0.1 vol% 0.2 vol% 0.3 vol% 80 0.5 vol%
80
concentration of a 0.4 mass%, 0.4 vol% 0.5 vol% 70
b 0.45 mass% 70
60
60

Stability time/h
Stability time/h
50
50
40
40

30 30

20 20

10 10

0 0
0 50 100 150 200 0 50 100 150 200
Ultrasonication time/min Ultrasonication time/min
(a) (b)

Fig. 3 Influence of sonication 140 140

time on stability time of D type 0.1 vol% 0.2 vol% 0.3 vol% 0.1 vol% 0.2 vol% 0.3 vol%
of THNFs with the SDS 0.4 vol% 0.5 vol% 0.4 vol% 0.5 vol%
120 120
concentration of a 0.4 mass%,
b 0.45 mass% 100 100
Stability time/h

Stability time/h
80 80

60 60

40 40

20 20

0 0
0 50 100 150 200 0 50 100 150 200
Ultrasonication time/min Ultrasonication time/min
(a) (b)

lnf ¼ 1:7366342 þ ð0:043695678  T Þ

 
þ ð95:543052  uÞ þ 0:00046772016  T 2
 
þ 29249:903  u2 þ ð1:3496487  T  uÞ
 
þ 1:6016472  106  T 3
   
þ 6832500  u3 þ 337:97403  T  u2
 
þ 0:011498485  T 2  u
ð11Þ

Thermal conductivity of THNFs

Fig. 4 SEM images of DHNF for C types of THNFs at 0.5 vol%
a before sonication, b after sonication
Thermal conductivity measurement

The experimental data of thermal conductivity of THNFs

versus temperature and volume fraction are demonstrated

123
888 S. M. Mousavi et al.

Fig. 5 Experimental viscosity 1.8

1.6
of a C type and b D type of 0.1 vol%
1.6 DW
THNFs at different solid 0.1 vol% 1.4 0.2 vol%
volume concentrations (0.1–0.5 1.4 0.2 vol% 0.3 vol%
0.4 vol%

Viscosity/cp
vol%) and temperatures 0.3 vol% 1.2

Viscosity/cp
1.2 0.5 vol%
(15–60 C) 0.4 vol% DW
0.5 vol% 1
1

0.8 0.8

0.6 0.6

0.4 0.4
0 20 40 60 80 0 20 40 60 80
Temperature/°C Temperature/°C
(a) (b)

Fig. 6 Viscosity variation 0.9 0.69 0.1 vol% 0.2 vol%

against shear rate at constant 0.3 vol% 0.4 vol%
0.85 0.1 vol% 0.2 vol% 0.3 vol% 0.67
0.5 vol%
temperature (55 C) and 0.8
0.4 vol% 0.5 vol% 0.65
different volume concentrations 0.63
0.75 0.61
(0.1–0.5 vol%) for different

Viscosity/cp
Viscosity/cp

0.7 0.59
types of THNF a C type, b D
0.65 0.57
type and c E type
0.6 0.55
0.53
0.55
0.51
0.5
0.49
0.45 0.47
0.4 0.45
0 20 40 60 80 0 20 40 60 80
Shear rate/1/s Shear rate/1/s
(a) (b)
1.65
1.6 0.1 vol% 0.2 vol%
0.3 vol% 0.4 vol%
1.55
1.5
Viscosity/cp

1.45
1.4
1.35
1.3
1.25
1.2
1.15
1.1
0 20 40 60 80
Shear rate/1/s
(c)

in Fig. 10a. The thermal conductivity increases nonlinearly water are found to be 34.6%, 44.1%, 32.1%, 28.5% and
with increasing volume fraction and temperature. The 78.6% at 15 C and 0.1 vol%, respectively.
thermal conductivity of THNFs enhancement is calculated The thermal conductivity enhancement of THNFs at low
from Eq. 12: solid volume concentrations is much greater than that of
  THNFs at high solid volume concentrations as shown in
Knanofluid  Kbasefluid
%Enhancement ¼  100 ð12Þ Fig. 10b. A linear relationship between the thermal con-
Kbasefluid
ductivity and temperature can be attributed to large regions
where Knanofluid and Kbasefluid denote the thermal conduc- of particle-free liquid with high thermal resistances created
tivity of THNF and distilled water, respectively. The by highly agglomerated nanoparticles [52]. The reason for
highest thermal conductivity enhancement of A type, B this is that at low solid volume concentrations, the stability
type, D type, E type and C type of THNFs as compared to and uniformity of nanoparticles in the base fluid would be

123
Effects of temperature and particles volume concentration on the thermophysical properties… 889

Fig. 7 Viscosity variation 0.06

0.1 vol% 0.2 vol% 0.12
against shear rate at constant 0.3 Vol% 0.4 vol% 0.1 vol% 0.2 vol%
temperature (55 C) and 0.05 0.5 vol%
0.1 0.3 vol% 0.4 vol%
different volume concentrations 0.5 vol%

Shear stress/Pa
(0.1–0.5 vol%) for different 0.04

Shear stress/Pa
0.08
types of THNF a C type, b D
0.03 0.06
type and c E type
0.02 0.04

0.01 0.02

0 0
0 20 40 60 80 0 20 40 60 80
Shear rate/1/s Shear rate/1/s
(a) (b)
0.05
0.045 0.1 vol% 0.2 vol%
0.3 vol% 0.4 vol%
0.04 0.5 vol%

0.035

Shear stress/Pa
0.03
0.025
0.02
0.015
0.01
0.005
0
0 20 40 60 80
Shear rate/1/s
(c)

higher than those at high solid volume concentrations. So, enhancement of the thermal conductivity of nanofluids
the higher stability at low solid volume concentrations [52]. Conventional particle-liquid suspensions do not form
leads to a higher thermal conductivity. such nanolayers in which the typical size of particles is less
The reversibility of the thermal conductivity of THNFs than 10 nm. Due to the fact that the layered molecules
which showed good stability after 30 days was evaluated. arrange in an intermediate physical state between the bulk
The values of thermal conductivity of THNFs were almost liquid and a solid, the molecules in nanolayers lead to a
the same values with ± 0.5% error as shown in Fig. 11 and higher thermal conductivity as compared to the bulk liquid.
Table 10. It can be concluded that as long as the THNFs In some cases, nanofluids form clusters over time or when
are stable, the values of thermal conductivity will remain the concentration of nanoparticles is high. The effective
unchanged. surface-area-to-volume ratio, the effective thermal inter-
action area of particles and thus the thermal conductivity of
Proposed correlation fluid decrease with the agglomeration of particles [57].
Figure 12 shows the presented theoretical models [45, 46]
The thermal conductivity of nanofluids depends on that are not able to predict the experimental data in a good
important factors such as thermal conductivity of the base manner.
fluid, thermal conductivity of individual nanoparticles, The coefficients of the proposed correlation (Eq. 14)
solid volume concentration of nanoparticles, shape of were attained by minimization of the following objective
nanoparticles, stability of nanofluid, temperature, size of function using the Levenberg–Marquardt algorithm (LMA)
nanoparticles and interfacial layer [56]. The quantities of with an R2 of 0.997, Eq. 13.
thermal conductivity of THNFs are greater than those PN
ðKest;K  Kexp;K Þ2
obtained from the Eapen’s mean-field [45] and Lu and Lin LSM ¼ min K¼1 ð13Þ
N
[46] models. In their works, the effects of interfacial layer
and particles size on the thermal conductivity of nanofluids where N is the number of total data points and K is the
are not considered. The presence of nanolayers in liquid thermal conductivity in Watt per meter per Kelvin. Sub-
suspension makes them to act as a thermal bridge between scripts est and exp denote the estimated thermal
the solid nanoparticles and bulk liquid, which leads to the

123
890 S. M. Mousavi et al.

2.4 Wang model (288 K) 2.4 Wang model (288 K)

Pak & Cho model (288 K) Pak & Cho model (288 K)
2.2 Batchelor (288 K) 2.2 Batchelor (288 K)
Wang model (323 K) Wang model (323 K)
2 Pak & Cho model (323 K) 2
Pak & Cho model (323 K)
1.8 Batchelor model (323 K) 1.8 Batchelor model (323 K)
Exp. (288 K) Exp. (288 K)
1.6 Exp. (323 K) 1.6 Exp. (323 K)
Viscosity/cp

Viscosity/cp
1.4 1.4
1.2 1.2
1 1
0.8 0.8
0.6 0.6
0.4 0.4
0.2 0.2
0 0
0 0.001 0.002 0.003 0.004 0.005 0.006 0 0.001 0.002 0.003 0.004 0.005 0.006
Volume fraction Volume fraction
(a) (b)
2.6
3 Wang model (288 K)
Wang model (288 K) 2.4 Pak & Cho model (288 K)
2.8
Pak & Cho model (288 K) 2.2 Batchelor (288 K)
2.6
Batchelor (288 K) Wang model (323 K)
2.4 2
Wang model (323 K) Pak & Cho model (323 K)
2.2 Pak & Cho model (323 K) 1.8 Batchelor model (323 K)
2
Viscosity/cp

Viscosity/cp
Batchelor model (323 K) 1.6 Exp. (288 K)
1.8 Exp. (288 K) Exp. (323 K)
1.4
1.6 Exp. (323 K)
1.4 1.2
1.2 1
1 0.8
0.8 0.6
0.6
0.4
0.4
0.2 0.2
0 0
0 0.001 0.002 0.003 0.004 0.005 0.006 0 0.001 0.002 0.003 0.004 0.005 0.006
Volume fraction Volume fraction
(c) (d)
2.6
Wang model (288 K)
2.4 Pak & Cho model (288 K)
2.2 Batchelor (288 K)
2 Wang model (323 K)
Pak & Cho model (323 K)
1.8 Batchelor model (323 K)
1.6 Exp. (288 K)
Viscosity/cp

1.4 Exp. (323 K)

1.2
1
0.8
0.6
0.4
0.2
0
0 0.001 0.002 0.003 0.004 0.005 0.006
Volume fraction
(e)
Fig. 8 Comparison between experimental data and classical models for the dynamic viscosity estimation of different types of THNF a A type,
b B type, c C type, d D type and e E type

123
Effects of temperature and particles volume concentration on the thermophysical properties… 891

Fig. 9 Comparison between

1.8 Proposed model (288 K) Proposed model (308 K)"
experimental data and proposed
Proposed model (328 K)" Exp. (288 K)
model for the dynamic viscosity 1.6
estimation of C-type THNF Exp. (308 K) Exp. (328 K)
1.4

Viscosity/cp
1.2

0.8

0.6

0.4
0 0.001 0.002 0.003 0.004 0.005 0.006
Volume fraction

Fig. 10 Variations of 1.05

experimental thermal 1 DW 0.1 vol% 0.2 vol% 0.3 vol% 0.4 vol% 0.5 vol%
Thermal conductivity/W/m K

conductivity of C-type THNF 0.95

and its enhancement with 0.9
a temperature at different solid 0.85
volume concentrations and 0.8
b different solid volume
0.75
concentrations at 60 C,
0.7
respectively
0.65
0.6
0.55
0.5
10 20 30 40 50 60 70
Temperature/°C
(a)
1.8
1.75
1.7
1.65
1.6
1.55
K nf /K bf

1.5
1.45
1.4
1.35
1.3
1.25
1.2
0 0.1 0.2 0.3 0.4 0.5 0.6
Volume concentration/%
(b)

conductivity from the model and experimental thermal

The experimental data and the obtained values from the
conductivity, respectively.
proposed correlation for thermal conductivity are com-
    
Knf ¼ 0:72768391 þ 9:6816854=T þ 283:69209 T 2 pared as shown in Fig. 13. As can be seen, the proposed
      model is in excellent agreement with experimentally
þ 4718:8713 T 3 þ 43232:493 T 4 measured data. The absolute relative deviation of the
   obtained values from the proposed model as compared to
þ 175433:68 T 5 þ ð274:276  uÞ the experimental data was less than ± 1%.
    As earlier mentioned, higher thermal conductivity of
þ 159781:42  u2 þ 41691000  u3
  nanoparticles in comparison with the base fluid is the most
 3:6405833  109  u4 important factor which enhances the thermal conductivity
ð14Þ of nanofluid. The thermal conductivity of nanocomposite

123
892 S. M. Mousavi et al.

Fig. 11 Comparison between 1

the reversibility of the thermal A-type,1minafter preparation A-type,30 days after preparation
conductivity of THNFs after 0.95 B-type,1 min after preparation B-type,30 days after preparation
1 min and 30 days at 15 C

Thermal conductivity ratio/W/m K

C-type,1 min after preparation D-type, 30days after preparation
0.9

0.85

0.8

0.75

0.7

0.65

0.6
0 0.1 0.2 0.3 0.4 0.5 0.6
Volume concentration/%

Table 10 Reversibility of the

THNFs Thermal conductivity/(W/m K)
thermal conductivity of THNFs
after 30 days at 15 C 1 min after preparation 30 days after preparation
0.1 vol% 0.3 vol% 0.5 vol% 0.1 vol% 0.3 vol% 0.5 vol%

A type 0.6662 0.7120 0.7825 0.6662 0.7118 0.7824

B type 0.6988 0.7537 0.8377 0.6989 0.7535 0.8376
C type 0.7195 0.7838 0.8793 0.7193 0.7835 0.8791

Fig. 12 Comparison between 1.1

B-type 1.2
present work and theoretical B-type
C-type C-type
Thermal conductivity/W/m K

Thermal conductivity/W/m K

models at a 15 C and b 60 C 1 A-type 1.1 A-type

Lu & Lin model Lu & Lin model
Eapen mean field 1 Eapen mean field
0.9 D-type
0.9
0.8
0.8
0.7
0.7
0.6 0.6

0.5 0.5
0 0.002 0.004 0.006 0 0.002 0.004 0.006
Volume fraction Volume fraction
(a) (b)

and the studied nanoparticles were measured at different Mixing effect

temperatures as shown in Fig. 14. The results demonstrated
that C-type THNF and then CuO nanoparticles have the The thermal conductivity of C-type THNF was measured at
highest thermal conductivity values. As a result, they can various ultrasonication times and powers at 60 C with the
enhance the thermal conductivity of the base fluid. Thermal solid volume concentration of 0.5% as shown in Fig. 15.
conductivity data of the studied nanocomposite are also The thermal conductivity of nanofluids enhances with the
given in Table 11. ultrasonication power and time, reaches its maximum value
and then reduces. In this case, nanofluids are in a transient

123
Effects of temperature and particles volume concentration on the thermophysical properties… 893

Fig. 13 Comparison between 1

experimental data and proposed Proposed model (288 K)

Thermal conductivity/W/m K
model for the thermal 0.95 Proposed model (308 K)
conductivity of C-type THNF Proposed model (328 K)
0.9 Exp. (288 K)
Exp. (308 K)
0.85
Exp. (328 K)
0.8

0.75

0.7

0.65
0 0.001 0.002 0.003 0.004 0.005 0.006
Volume fraction

Fig. 14 Thermal conductivity 140

Thermal conductivity of nanoparticles/W/m K

of the studied nanoparticles and TiO2 C-type E-type D-type B-type A-type CuO MgO
nanocomposites at 15 C 120

98.134

96.144
100

69.324
62.114
80

57.994
56.104
60

40

20
2.245

5.421
0

Table 11 Thermal conductivitiy of the nanoparticles at different temperatures

Temp. (C) MgO nanoparticles TiO2 nanoparticles CuO nanoparticles THNFs
D type B type E type C type A type

15 5.421 2.245 69.324 57.994 96.144 56.104 98.134 62.114

20 5.310 2.198 69.265 57.935 96.085 56.045 98.045 62.055
25 5.230 2.122 69.135 57.805 95.955 55.915 97.943 61.925
30 5.110 2.054 69.056 57.726 95.876 55.836 97.901 61.846
35 5.085 1.193 68.923 57.593 95.743 55.703 97.836 61.713
40 5.003 1.189 68.848 57.518 95.668 55.628 97.775 61.638
45 4.976 1.179 68.760 57.430 95.580 55.540 97.711 61.550
50 4.912 1.173 68.637 57.307 95.457 55.417 97.646 61.427
55 4.897 1.167 68.589 57.259 95.409 55.369 97.587 61.379
60 4.856 1.152 68.455 57.125 95.275 55.235 97.501 61.245

state, and nanoparticles are settled in distilled water. The time, ultrasonication power and surfactant concentration in
optimal values of ultrasonication power and time of order to measure the thermal conductivity coefficient of
THNFs are found to be 420 W and 140 min, respectively. nanofluids. The nanoparticles are then detached from the
The effect of nanoparticles recovery on thermal con- base fluid via the centrifuge (EBA21, Hettich Company,
ductivity coefficient of THNFs was also investigated. At Germany) and dried in an oven at 80 C. The recovery of
first, the prepared nanocomposites were dispersed in the nanoparticles is carried out in five times, and their thermal
base fluid under the optimum values of ultrasonication conductivity was measured as shown in Fig. 16. After the

123
894 S. M. Mousavi et al.

Fig. 15 The effect of 0.942 0.943

a ultrasonication power and 0.942
b ultrasonication time on the 0.94

Thermal conductivity/W/m K

Thermal conductivity/W/m K
0.941
thermal conductivity of C-type
THNF at 60 C with the solid 0.938 0.94

volume concentration of 0.5% 0.939

0.936
0.938
0.937
0.934
0.936
0.932 0.935
0.934
0.93
0.933
0.928 0.932
330 360 390 420 450 60 90 120 150 180 210
Sonication power/W Sonication power/W
(a) (b)

0.944
0.9414 0.9414 0.9414
0.942
0.94
0.938
0.938
0.936 0.935
0.934
0.934
0.932
0.93
0.928
Unrecovered First recovery Second recovery Third recovery Fourth recovery Fifth recovery

Fig. 16 Effect of nanocomposites recovery on the thermal conductivity of C-type THNF at 60 C with the solid volume concentration of 0.5%

first and secondary recovery process of THNFs, the thermal Specific heat capacity measurement
conductivity of THNFs did not significantly change.
However, after the third recovery process of THNFs and so Effects of solid volume concentration and temperature
on, a great effect on the thermal conductivity of THNFs
was observed. The most important reason for variations of The experimental data of specific heat capacity of THNFs
thermal conductivity with the recovery process of the are shown in Fig. 17. The highest reduction in specific heat
nanocomposite is the change of functional groups on the capacity as compared to distilled water is 2.13% which
surface of nanoparticles. belongs to C-type THNF. The maximum enhancement for
A, B, D and E types of THNFs is found to be 1.68, 2.0, 1.72
and 1.56%, respectively. The experimental data are

Fig. 17 Experimental specific 4.19

heat capacity of C-type THNF 0.1 vol% 0.2 vol% 0.3 vol% 0.4 vol% 0.5 vol%
at different temperatures
Specific heat capacity/J/g K

4.17

4.15

4.13

4.11

4.09

4.07
0 10 20 30 40 50 60 70
Temperature/°C

123
Effects of temperature and particles volume concentration on the thermophysical properties… 895

4.22
Exp. (323 K) Exp. (288 K) Model 2 (288 K)
4.21
4.2 Model 1 (323 K) Model 2 (323 K) Model 1 (288 K)
Specific heat capacity/J/g K
4.19
4.18
4.17
4.16
4.15
4.14
4.13
4.12
4.11
4.1
4.09
4.08
0 0.001 0.002 0.003 0.004 0.005 0.006
Volume fraction

Fig. 18 Comparison between experimental specific heat capacity data of THNFs and empirical models for the C type

Fig. 19 Comparison between 4.2

experimental data and proposed 4.19
model for the specific heat Proposed model (288 K) Proposed model (323 K) Exp. (288 k) Exp. (323 K)
4.18
capacity of C-type THNF at
Specific heat capacity/J/g K

a 15 C and b 55 C 4.17
4.16
4.15
4.14
4.13
4.12
4.11
4.1
4.09
4.08
0 0.001 0.002 0.003 0.004 0.005 0.006
Volume fraction

compared with the values obtained from models 1 and 2 as Proposed correlation
shown in Fig. 18. Model 1 is the mixing theory for ideal
gas mixtures [35], and model 2 is based on the statistical The coefficients of the proposed correlation were obtained
mechanism where a base fluid and nanoparticles are in by minimization of the following objective function using
equilibrium [35]: the Levenberg–Marquardt algorithm (LMA) [46], Eq. 17.
PN
Cp;nf ¼ uCp;np þ ð1  uÞCp;bf ð15Þ ðCpest;K  Cpexp;K Þ2
    LSM ¼ min K¼1 ð17Þ
u qCp np þð1  uÞ qCp bf N
Cp;nf ¼ ð16Þ where N is the number of total data points and CpK is the
uqnp þ ð1  uÞqbf
specific heat capacity in j/g K. Subscripts est and exp
where Cp,nf, Cp,np, Cp,bf denote the heat capacity of nano- denote the estimated specific heat capacity from the model
fluid, nanoparticles and base fluid, respectively. Model 2 is and experimental specific heat capacity, respectively. The
adopted as a base model in many investigations, but model absolute deviation of the proposed model is less than ±
1 gives poor results due to not considering the density of 1%. The proposed model for the estimation of specific
nanoparticles. heat capacity of THNFs with an R2 of 0.998 is presented in
Eq. 18, and the comparison between its results and
experimental data are shown in Fig. 19. The correlation for

123
896 S. M. Mousavi et al.

Fig. 20 Variations of 1.03

experimental data of density for 1.025 DW 0.1 vol% 0.2 vol% 0.3 vol% 0.4 vol% 0.5 vol%
C-type THNF with temperature 1.02
1.015

Density/g/cm 3
1.01
1.005
1
0.995
0.99
0.985
0.98
10 20 30 40 50 60 70
Temperature/°C

Fig. 21 Comparison between 1.03 1.04

Pak&Cho (288 K)
experimental density data of 1.025 Pak&Cho (288 K)
Pak&Cho (323 K)
THNFs and Pak and Cho model 1.02 1.03 Pak&Cho (323 K)
Exp. (288 K)
for a A type, b B type and c C Exp. (288 K)

Density/g/cm 3
1.015 Exp. (323 K)
type 1.02 Exp. (323 K)
Density/g/cm 3

1.01
1.005 1.01
1
0.995 1

0.99
0.99
0.985
0.98 0.98
0 0.002 0.004 0.006 0 0.002 0.004 0.006
Volume fraction Volume fraction
(a) (b)
1.025
Pak&Cho (288 K)
1.02 Pak&Cho (323 K)
Exp. (288 K)
1.015 Exp. (323 K)
Density/g/cm 3

1.01

1.005

0.995

0.99

0.985
0 0.001 0.002 0.003 0.004 0.005 0.006
Volume fraction
(c)

estimating the specific heat capacity of THNFs is suggested Density measurement

as:
The experimental data of density of THNFs at various
Cp;nf ¼ 4:2028064 þ ð0:0015020303  T Þ
   temperatures (15–60 C) in different solid volume con-
þ 2:0272727  105  T 2 þ ð17:03  uÞ
centrations (0.1–0.5 vol%) are demonstrated in Fig. 20.
ð18Þ The highest decrement in density of THNFs as compared to
distilled water was found to be 2.08% for the C-type THNF
at 55 C with the solid volume concentration of 0.5%. At
the same conditions, the greatest decrement for A, B, D and
E types are 1.38, 1.88, 1.32 and 1.30%, respectively. The
causes for the increase in density of THNFs with enhancing

123
Effects of temperature and particles volume concentration on the thermophysical properties… 897

Fig. 22 Comparison between 1.025

experimental data and proposed Proposed model (288 K)
1.02
model for the density of C-type Proposed model (323 K)
THNF at a 15 C and b 55 C 1.015
Exp. (288 k)
1.01

Density/g/cm 3
Exp. (323 K)

1.005

0.995

0.99

0.985

0.98
0 0.001 0.002 0.003 0.004 0.005 0.006
Volume fraction

solid volume concentration are the chaotic movement of Table 12 Effect of different volume concentrations of nanoparticles
nanoparticles, particles migration and Brownian motion. on the surface tension of THNFs at 50 C
The experimental data of density of THNFs are in good Type of THNF Volume concentration/% r//N m-1
agreement with the values obtained from the mixture
density model as shown in Fig. 21. The mixture density DW ? SDS – 0.0431
values were determined from Pak and Cho correlation [42] B type ?SDS 0.1 0.0403
as follows: 0.3 0.0367
      0.5 0.0384
qhnf ¼ u1 qnp;1 þ u2 qnp;2 þ u3 qnp;3 ðð1  uÞqbf Þ
C type ?SDS 0.1 0.4001
ð19Þ 0.3 0.3711
where qhnf, qnp,1, qnp,2, qnp,3, qbf, u1, u2 and u3 denote the 0.5 0.3765
density of hybrid nanofluids, the density of nanoparticles 1, A type ?SDS 0.1 0.0418
2 and 3 and the solid volume concentration of nanoparticles 0.3 0.0383
1, 2 and 3, respectively. The absolute deviation of exper- 0.5 0.0396
imental data from the mixture density correlation is less D type ?SDS 0.1 0.0440
than 1%. The main cause of difference between experi- 0.3 0.0444
mental data and Pak and Cho correlation is the non-uni- 0.5 0.0456
form variations of density in the interfacial region due to E type ?SDS 0.1 0.0462
having higher van der Waals interactions between the 0.3 0.0469
molecules of THNFs. 0.5 0.0493

Proposed correlation

The coefficients of the proposed correlation were fabri- comparison between its results and experimental data are
cated by minimization of the following objective function shown in Fig. 22. The correlation for estimating the density
using the Levenberg–Marquardt algorithm (LMA) [46], of THNFs is suggested as:
Eq. 20.
PN qnf ¼ 1:0020693 þ ð0:00011319091  T Þ
 
ðqest;K  qexp;K Þ2 þ 3:2636364  106  T 2 þ ð4:0702857  uÞ
LSM ¼ min K¼1 ð20Þ   2 
N þ 15:714286  u
where N is the number of total data points and qK is the ð21Þ
density in g m-3. Subscripts est and exp denote the esti-
mated density from the model and experimental data,
respectively. The absolute deviation of the proposed model Surface tension
is less than ± 1%. The developed model as shown in
Eq. 21 can interestingly estimate the density of THNFs The quantity of surface tension (r) was measured between
with respect to great values of R2, which is 0.999, and the air–water in different states by applying a surface
tension measurement device (DSA-100, Kruss, Germany)

123
898 S. M. Mousavi et al.

Fig. 23 Comparison among MgO TiO2 C-type D-type MgO TiO2 C-type D-type
Prantdl numbers of the studied 14 14
B-type A-type E-type CuO B-type A-type E-type CuO
THNFs at 50 C with the solid
volume concentration of a 0.5% 12 12
and b 0.3% 11.33 10.99 11.33 10.99
10.56 10.56
9.76 9.76
10 9.21 10 9.21

Prandtl number
8.89

Prandtl number
8.89
8.45 8.45
8 7.11 8 7.11

6 6

4 4

2 2

0 0
(a) (b)

at ambient temperature. The results showed that the error is increase in the convective heat transfer. Considering as the
less than ± 1.1%. The surface tension of THNFs was Prandtl number increases in value, the THNFs ability in
measured at the 0.1, 0.3 and 0.5 solid vol% in 50 C. convective heat transfer would be greater. Prandtl number
The surface tension decreased from 0.0713 to of DHNFs was calculated at different volume concentra-
0.0431 N m-1 when SDS was added to distilled water. The tions (0.1–0.5 vol%).
addition of nanocomposites with various mass percents to lCp
the base liquid represents different behaviors. A, C and B Pr ¼ ð22Þ
K
types of THNF create a higher decrement in surface tension
of the base fluid. However, the surface tension enhanced where Pr denotes the Prandtl number. The highest and least
with enhancing solid volume concentration in the other values of Prandtl number are about 7.11 and 13.76 for the
THNFs as compared to distilled water. The results are C-type THNF at 0.3 vol% in 50 C, respectively. Com-
demonstrated in Table 12. parison among Prandtl numbers for all the prepared THNFs
The important reason for the increment surface tension is shown in Fig. 23. As can be seen, the highest value of
with the enhancing solid volume concentration of the Prandtl number belongs to 0.3 vol% of the C-type THNF
nanocomposites is van der Waals forces between which can be considered as an optimum concentration in
nanoparticles at the interface of distilled water/air systems the volume concentration range of 0.1–0.5%.
[52]. Therefore, the surface free energy increases and so Generally, the results indicate that the least value of
enhances the surface tension [54]. Sohel et al. [55] showed surface tension belongs to the C-type THNF and then
that nanofluids reduced the surface tension of the water. belongs to the B-type THNF. Therefore, it is clear that the
Also, Chen et al. [56] found that the surfactants had no best nanofluid for drag reduction in heat systems among the
influence on the nanofluids surface tension. So, the surface nanofluids assessed in this work belongs to the C-type
tension increment or the surface tension decrement is yet THNF with the highest value of Prandtl number.
contradictory. The agglomeration of the nanoparticles at
the air–base liquid interface and the Brownian motion are
the important reasons for this behavior of nanofluids Conclusions
[57, 58]. A possible drag reduction mechanism with adding
A, B and C types of nanocomposites in gas/liquid flow is CuO–MgO–TiO2 aqueous ternary hybrid nanofluids
the main reason for the surface tension decrement between including A (33.4 mass% CuO/33.3 mass% MgO/33.3
air and water systems. mass% TiO2), B (50 mass% CuO/25 mass% MgO/25
mass% TiO2), C (60 mass% CuO/30 mass% MgO/10
Optimization of the THNF composition mass% TiO2), D (25 mass% CuO/50 mass% MgO/25
mass% TiO2) and E (25 mass% CuO/25 mass% MgO/50
The aim of this paper was to find the optimum mass percent mass% TiO2) were fabricated at the solid volume con-
of THNFs leading to the highest heat transfer rate. In other centration range of 0.1 to 0.5 vol%. SDS was added as a
words, finding the best mass percent of THNFs causes the surfactant, and the suspensions become homogeneous
using an ultrasonic homogenizer and a magnetic stirrer.

123
Effects of temperature and particles volume concentration on the thermophysical properties… 899

The thermo-physical properties and rheological behavior of 7. The classical models underpredict the experimental
the CuO-MgO-TiO2/DW THNFs were studied at the tem- data of the dynamic viscosity and thermal conductivity
perature range of 15–60 C. Altogether, these findings of THNFs within 6–24% accuracy. Four new correla-
demonstrate: tions were developed for the prediction of thermo-
physical properties and dynamic viscosity of THNFs
1. The synthesized CuO–MgO–TiO2 NPs were charac-
with an acceptable accuracy of less than ± 1%.
terized using X-ray diffraction (XRD) studies and
8. The results obtained from measuring surface tension
scanning electron microscopy (SEM). XRD confirms
and calculating Prandtl number revealed that the THNF
the formation of CuO–MgO–TiO2 NPs, whereas XRD
containing 0.3 vol% C-type NPs was the most proper
and SEM indicate the sizes in nanometer range. The
one to access the highest convective heat transfer rate
characterization results showed that the NPs morphol-
and drag reduction because of the greatest Prandtl
ogy is nearly spherical and its average particles size
number and the least surface tension, respectively.
would be 45–55 nm.
2. The conclusions of measuring stability time illustrated
further volume concentration of nanocomposites caus- Acknowledgements This work was supported by the National Key
R&D Program of China (Grant No. 2016YFE0204200) and the
ing more sedimentation of nanoparticles in the water. National Natural Science Foundation of China (No. 51776170). The
Zeta potential measurements of THNFs with low NPs authors also would like to express their appreciation to the Shiraz
concentrations (0.1 to 0.3) demonstrate good disper- University and the 111 project (B16038) for the support.
sions of A, B, C, D and E types of NPs in distilled
water. However, THNFs with high solid volume
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