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Tailoring the viscosity of water and ethylene glycol based TiO2 nanofluids

Abu Musa Abdullah, Aminur Rashid Chowdhury, Yingchen Yang, Horacio Vasquez,
H. Justin Moore, Jason G. Parsons, Karen Lozano, Jose J. Gutierrez, Karen S.
Martirosyan, M. Jasim Uddin
PII: S0167-7322(19)34132-7
DOI: https://doi.org/10.1016/j.molliq.2019.111982
Reference: MOLLIQ 111982

To appear in: Journal of Molecular Liquids

Received Date: 24 July 2019

Revised Date: 9 September 2019
Accepted Date: 20 October 2019

Please cite this article as: A.M. Abdullah, A.R. Chowdhury, Y. Yang, H. Vasquez, H.J. Moore, J.G.
Parsons, K. Lozano, J.J. Gutierrez, K.S. Martirosyan, M.J. Uddin, Tailoring the viscosity of water and
ethylene glycol based TiO2 nanofluids, Journal of Molecular Liquids (2019), doi: https://doi.org/10.1016/
j.molliq.2019.111982.

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1 Tailoring the Viscosity of Water and Ethylene Glycol Based

2 TiO2 Nanofluids

3 Abu Musa Abdullah1,3, Aminur Rashid Chowdhury1,2, Yingchen Yang3, Horacio Vasquez3, H.

4 Justin Moore4, Jason G. Parsons2, Karen Lozano3, Jose J. Gutierrez2, Karen S. Martirosyan5, M.

5 Jasim Uddin1,2 *

1
6 Photonics and Energy Research Lab, The University of Texas Rio Grande Valley, 1201 W

7 University Drive, Edinburg, Texas 78539, USA

2
8 Department of Chemistry, The University of Texas Rio Grande Valley, 1201 W University

9 Drive, Edinburg, Texas 78539, USA

3
10 Department of Mechanical Engineering, The University of Texas Rio Grande Valley, 1201 W

11 University Drive, Edinburg, Texas 78539, USA

4
12 Science, Technology, Engineering & Mathematics Division, Naugatuck Valley Community

13 College, 750 Chase Parkway, Waterbury, Connecticut 06708, USA

5
14 Department of Physics and Astronomy, The University of Texas Rio Grande Valley, 1201 W

15 University Drive, Edinburg, Texas 78539, USA

16

17 *Corresponding Author: M. Jasim Uddin, mohammed.uddin@utrgv.edu

18
19 Abstract

20 Nanofluids have garnered significant attention in the scientific and engineering research

21 communities due to their enhanced heat transfer properties when compared to conventional

22 thermal fluids. Nanofluids comprised of titanium dioxide (TiO2) nanoparticles have a wide range

23 of applications due to their excellent thermophysical properties like thermal conductivity and

24 viscosity, environmentally friendly nature, and low cost. This article reviews major research

25 advances in homogeneous water (H2O) and ethylene glycol (EG, HO(CH2)2OH) based TiO2

26 nanofluids compared to hybrid TiO2 nanofluids. This review focuses on viscosity measurements

27 and rheological behavior of the aforementioned nanofluids at various temperatures and TiO2

28 particle concentrations. Besides, the effect of sonication time, particle size, and base fluid

29 mixture on the viscosity of TiO2 nanofluids has been included in this study. The classical and

30 experimental models of viscosity have been reviewed as well. Furthermore, nanofluid

31 preparation methods, characterization, and measurement techniques have been examined and

32 discussed. Previous studies clearly show that the viscosity of TiO2 nanofluids is a noteworthy

33 function of both temperature and nanoparticle concentration. Viscosity is observed to

34 significantly increase with particle concentration and decrease with temperature. Nanofluids are

35 also observed to exhibit dissimilar rheological behaviour under different experimental

36 conditions. Additionally, increases in viscosity has also been discussed with respect to the base

37 of nanofluids. The hybridization of TiO2 nanofluids, as well as combinations of ethylene glycol

38 and water, have shown substantial effects on the viscosity of the nanofluids. These results

39 provide important characteristics that should be considered during various engineering

40 applications of TiO2 nanofluids.

41 Keywords
42 Viscosity, TiO2 Nanofluids, Rheological Behavior, Ethylene Glycol, Water, Nanoparticles
43
44 Introduction
45 The rapid progress of nanotechnology has begun a revolution in scientific research and

46 technological development continuously revealing new breakthroughs. Nanofluids are one class

47 of engineered compounds that have come to light during this recent scientific revolution [1] . In

48 1873, Maxwell first mentioned about utilizing metallic particles in conventional heat transfer

49 fluids to increase the electrical and thermal conductivity of the fluids [2]. Later in 1993, Masuda

50 et al. used ultra-fine Al2O3, TiO2 and SiO2 particles to alter the thermal conductivity and

51 viscosity of the base liquid [3,4]. After the pioneering work by Choi and Eastman in 1995 to

52 increase the thermal conductivity of a fluid using nanoparticles, research on a broad variety of

53 nanofluids rapidly emerged [5]. A nanofluid, as a heat transfer fluid, is an engineered colloidal

54 suspension of nanoparticles ranging in size from 1-100 nm in a liquid medium. The colloidal

55 particles are stabilized and dispersed in a base fluid [6,7]. Solvents such as water, ethylene

56 glycol, methylene glycol, ethanol, mineral oil, paraffin oil, methanol, and several others, are

57 generally used as base fluids [6,8–10]. Solid particles such as the oxides of different metals (e.g.,

58 Al, Fe, Cu, Zn, Ag, Mg, Ti, etc), carbon nanotubes, graphene, aluminium nitride (AlN), and

59 silicon carbide (SiC) nanoparticles are used as solutes in the nanofluid [4,11–14]. These new

60 generation engineered fluids have myriad applications across numerous systems and engineering

61 devices, which include cooling systems in electronic components, solar collectors, heating

62 systems, fluids used in machining systems, lubrication systems, industrial cooling systems, heat

63 exchangers, car radiators, drug delivery systems, nuclear systems, microelectronics, fuel cells,

64 thermosyphons and geothermal heat pumps [10,15–27]. Incorporating nanofluids with enhanced

65 thermophysical properties in the aforementioned devices have displayed increased efficiencies

66 and improved performance compared to the conventional heat transfer fluid, which have

67 indirectly promoted sustainable development [28–30].

68 Enhancing the thermophysical properties of nanofluids has led to increasing diversity in

69 the applications of these materials as well as long-term colloidal stability. Viscosity is perhaps

70 the characteristic thermophysical property that is most important for fluid flow applications [31].

71 It can be described as an the resistance of a fluid to flow over a surface [11,32]. Viscosity is

72 highly affected by a variety of parameters such as temperature, nanoparticle concentration,

73 sonication, shear rate, preparation method, and nanoparticle size [4,18,33,34].

74 The present article reviews recent experimental studies and the characterization of the

75 influence of temperature, particle concentration and sonication time on the viscosity of ethylene

76 glycol (EG) and water-based TiO2 nanofluids. Metallic oxide nanoparticles have broader

77 applications than other nanoparticle types due to their easy preparation and chemical stability

78 [35,36]. Correspondingly, due to titanium dioxide’s good heat transfer characteristics, high

79 stability, easy availability, low cost, and environmentally friendly character, TiO2 is a promising

80 choice for researchers to employ in nanofluids [37–39]. A timeline on TiO2-based nanofluids

81 research is shown in Figure 1(a). The base fluids, ethylene glycol and water, have been widely

82 utilized due to their good heat transfer, ease of availability, and stability under a wide range of

83 temperatures [37,40]. Figure 1(b) demonstrates the number of publications on the use of TiO2-

84 based nanofluids since 2004 according to the Web of Science [41]. From this data, it is evident

85 that research interest in TiO2-based nanofluids has exploded over the last 15 years.

86 This review also focuses on the rheological analysis of TiO2 nanofluids with variable

87 shear rate at different nanoparticle concentrations. Additionally, some of the classical and

88 popular empirical models used to determine the viscosity of nanofluids are presented in this
89 study. Many of these investigations have studied the influence of the temperature and

90 nanoparticle concentration on viscosity. However, some experiments have also demonstrated the

91 effect of shear rate, sonication time, nanoparticle size, and base fluid mixture ratios as well. In

92 addition, the prime outcomes of these experiments and the scope of potential future research of

93 nanofluids are also discussed.

94

95

96

97 Figure 1: (a) A brief timeline regarding research on TiO2 nanofluids and, (b) Number of

98 publications reported on TiO2 Nanofluids research throughout years [41].

99

100
101

102 Preparation, Characterization and Measurement Techniques

103 Nanofluid preparation deals with dispersion of a solid nanoparticle into a base fluid.

104 Although water and ethylene glycol are the preferred base fluid in most studies, a variety of

105 solvents have been used for the preparation of nanofluids, namely methanol, ethanol, propylene

106 glycol, coconut oil and paraffin oil [6,42]. Studies have also shown the use of a binary mixture of

107 fluid as well as hybrid solutes are commonly used for nanofluid development [43,44]. In general,

108 there are two methods or processes to generate nanofluids; the single-step method and the two-

109 step method [10]. In the single-step method, the nanoparticles are simultaneously prepared and

110 dispersed into the base fluid. Whereas, in the more utilized two-step method, the nanoparticles

111 are synthesized and subsequently dispersed into the base fluid [10,18,45]. One of the biggest

112 challenges in the development of nanofluids is related to maintaining long term colloidal stability

113 [46]. Colloidal stability can be defined as avoiding agglomeration of the nanoparticles due to

114 their high surface activity and inherent Van Der Waals forces [46,47]. In order to stabilize

115 colloidal suspensions, electrostatic and electrosteric surface stabilization methods have been

116 developed [47]. Additionally, surfactants may be used to overcome agglomeration and to

117 provide colloidal stabilization and ultra-sonication, homogenization, high shear mixing and ball

118 milling have been used for stabilized mixing of the nanofluids [6,10,11,35,44,46,48]. Although

119 the one-step method provides increased stability to nanofluids, the two-step methods are more

120 readily employed due to their lower cost and industrial applicability [10,42]. Table 1 summarizes

121 important key experimental parameters used for the development and characterization of

122 nanofluids prepared through the two-step method.

123
124

125 Table 1: Parameters for the Preparation of TiO2 nanofluid using the two-step method.

Base Fluid NP* NPS** Concentration Homogenization Reference

/Stabilization

Water TiO2 21nm 0.2-2 vol% Ultrasonic vibration [49]

(2h)

Water TiO2 72-76nm 1-35 wt% Sonication (1h) [50]

Water TiO2 30nm 0.5-1.5 vol% Ultrasonic vibration [51]

(TiO2), 0.5 vol% (30min)
Al2O3 43nm Al2O3

EG TiO2 10-30nm 5-25% by mass Ultrasonic [37]

(rutile), Homogenization

10-25nm
(anatase)

EG TiO2- <25nm 0.5-2vol% Stirring, Ultrasonic [52]

CuO/C (TiO2), Processor

18-25nm

(CuO/C)

Water/EG, TiO2, 21nm 1-4 vol% Ultrasonic vibration [53]

(20/80wt%) Al2O3 120nm (2h)

Water /EG , TiO2- 50nm 0.5-3 vol% Sonication (90min) [54]

(60 /40vol%) SiO2 (TiO2),

22nm
(SiO2)

126 Note: *NP - nanoparticle, ** NPS - average nanoparticle size

127

128 The size, shape and atomic arrangement within nanoparticles used to produce TiO2

129 nanofluids have been characterized using Transmission Electron Microscopy (TEM) and

130 Scanning Electron Microscopy (SEM) [36,37,53–59]. Figure 2(b) shows the TEM image of

131 irregular flake shaped TiO2 nanoparticles used in experimental study by Shu et al. [38]. The

132 images of this type provide information on particle size and agglomerations [60]. X-ray

133 diffraction (XRD) is also used to determine the structure and crystalline phase of TiO2-based

134 nanofluids [38,52,55]. Figure 2(a) shows a powder XRD pattern for anatase TiO2 nanoparticles.
135 The diffraction peaks depicted in the diffraction pattern correspond to the (101), (004), (200),

136 (105), (211), (204), (116), and (220) crystal planes of the TiO2 anatase phase [38,61]. The inset

137 of Figure 2(a) shows a schematic of anatase TiO2 crystalline structure. Although TiO2 anatase

138 nanoparticles are commonly used, TiO2 rutile nanoparticles have been used as well [37]. The

139 viscosity of the nanofluids has been measured using different rheometers [51,54,55] and

140 viscometers [62]. Figure 2(c) and 2(d) show diagrams of an MCR (Modular Compact Rheometer)

141 302 rotational rheometer and a Psl-Rheotek viscometer, respectively.

142

143
144

145 Figure 2: (a) XRD pattern (inset: anatase structure of TiO2 [63]) and (b) TEM image of TiO2

146 nanoparticles [38]. (c) Schematic diagram of MCR 320 rotational rheometer for measuring

147 viscosity [52]. (d) A U-tube viscometer by Psl-Rheotek.

148

149

150 Viscosity Models and Theories of Nanofluid

151 Viscosity has been described by a variety of models starting from Einstein’s classical

152 model from 1906 [64,65]. Einstein measured the effective viscosity of fluid comprised of

153 spherical particles at low concentration by considering particle removal energy relative to the

154 surrounding fluid and obtained the following correlation

155

156  =  (1 + 2.5∅) (1)

157

158 where µ n and µ b are the viscosity of the fluid suspension and base fluid, respectively, and Ø is

159 the particle concentration. Since then, there have been several models developed to describe the

160 viscosity of nanofluids under different conditions. Classical forms of those correlations are

161 shown below in Table 2.

162

163 Table 2: Classical viscosity models used to describe viscosity of nanofluids.

Sl. Model Develop Year Remarks

ed by

1  =  (1 + 2.5∅) Einstein 1906 µ n= viscosity of fluid suspension

[64]
µ b= viscosity of base fluid
(1)
ø= volume concentration of particles.

Applicable for low (less than 2%)

concentration of nanoparticles

2  =  (1 + 4.5∅) Hatschek 1913 Applicable for 40% concentration of

[66] solid particles in fluid for a two-phase
 (2) system

3  =  (1 − ∅). Brinkma 1952 The equation was developed for 4 vol%

n [67] concentrations of particles. It is a
modified version of Einstein’s model
(3)

4.   (1 + 1.5∅) ∅/(∅) Krieger 1959 øm = Maximum particle concentration.

and
Doughert Applicable for any particle
(4) y[68] concentration. A semi-empirical relation
was explained for shear viscosity
through this model.

5   (1 + 1.5∅) ∅/(∅) Nielsen 1970 Can be used for nanofluids with more
[69] than 2 vol% concentration. It is also
known as Power Law Model.
(5)

6  =  (1 + 2.5∅ + 6.25∅ + (∅ )) Lundgre 1972 Viscosity can be determined with the
n [70] help of Taylor series through this
model.
(6)

7  =  (1 + ∅) Brenner 1974 r = aspect ratio of the particles

and
Condiff The correlation was developed for the
(7) [71] viscosity of rod-like particles in low
concentration solution and high shear
 = (0.312/(ln 2 − 1.5)) + 2 − rate.
(0.5/(ln 2 − 1.5)) − (1.872/)

(8)

#
8  =  (3 + (∅  / ln($/∅)) Jeffrey 1976 The equation was developed for the
 and viscosity of rod-like particles in high
Acrivos concentration solution.
(9) [72]

9  =  (1 + 2.5∅ + 6.5∅ ) Batchelo 1977 Brownian motion of particles was

r [73] assumed for this model to determine
viscosity.
(10)

10 Graham 1981 h= inter-particle spacing

 =
[74]
dp= radius of the particle
 (1 + 2.5∅ +
4.5(1& )) Particle diameter and inter-particle
(%(2 + %)(1 + %) spacing was considered in this model.
For a lower concentration of
(11) nanoparticles, the model is supportive to
Einstein’s model.

% = ℎ&(
)
 ∅
11  =  (1 − * +) Kitano[7 1981 Developed to determine the viscosity of
∅ 5] a two-phase solution.

(12)

12 , 1 1  White[31 1991 µ o= reference value of viscosity

ln * -+ ≈ % + 0 * .+ + 2 * .+
,. 1 1 ]
To= reference value of temperature
(13)
a, b and c = certain values of certain
fluid provided by White.

Provides a relation between viscosity of

base fluid and temperature.

13  =  (1 + 34 ∅ + 35 ∅ ) Bicerano 1999 kv = Virial co-efficient

[76]
kh = Huggins co-efficient
(14)
The equation was developed to reflect
the volumetric effect of viscosity.

14  =  (1 + 7.3∅ + 123∅ ) Wang 1999 A simple model to determine the

[77] viscosity.
(15)

164

165 The models presented in Table 2 are, for the most part, theoretical approaches to predict

166 the viscosity of fluids. However, observations show that most of these models fail to predict the

167 viscosity of nanofluids as these models were developed before the invention of nanofluid, thus

168 these models do not consider parameters regarding nanofluid characteristics such as nanolayer,

169 pH, sonication time, particle size, interparticle spacing, particle magnetic properties etc

170 [18,35,78]. Viscosities measured from these models are only the functions of base fluid viscosity

171 and volumetric concentration of the particles. So, they are limited to specific particle

172 concentration, shape and size only [18,78–80]. Therefore, viscosity measured from these models

173 deviates notably with respect to the practical value at an extensive range of particle concentration

174 [80].
175

176 Figure 3: Graphical representation of relative viscosity at different particle concentration

177 according to the Einstein model, Brinkman model and experimental co-relation by Chen et al.

178 and Williams et al.

179

180 Figure 3 provides a graphical representation of relative viscosity with respect to particle

181 concentration ranging from 1 to 10 % according to the classical models by Einstein (Eq. 1) and

182 Brinkman (Eq. 3), as well as the co-relations by Chen et al. (Eq. 22) from the study with ethylene

183 glycol-based TiO2 nanofluid and from the study by Williams et al. (Eq. 26) with water-based

184 ZrO2 nanofluid where the relative viscosity increases linearly for both of the classical models.

185 However, it shows an exponential increase for the experimental co-relations significantly

186 deviating from the classical models. On the other hand, Table 3 lists some viscosity models that

187 have been developed based on experimental approaches to describe the viscosity of nanofluids.

188

189 Table 3: Experimental viscosity models used to characterize nanofluids

Sl. Model Defined Year Remarks
by
1 ∅ Noni et 2002 Developed to predict viscosity of
 =  (1 + 0( )) )
1 − ∅6 al. [81] a ceramic solution.

(16)

2  =  × 13.47 ×  .89∅ Tseng 2003 Based on the experiment on TiO2

and Lin nanofluid where TiO2
[82] nanoparticles dispersed into water.
(17)

3  =  (1 + 3, ∅) Prasher 2006 kµ = Co-efficient of viscosity

et al. [83] enhancement.
(18) Based on the study on
alumina/propylene glycol
nanofluids

4 1 Kulkarni 2006 a, b = f(ø)

ln( ) = % : < − 0
; et al. [84]
The equation was developed from
the experiment on water-based
(19) CuO nanofluid at 5o to 50oC.

5 log( ) = 2 ?1 Namburu 2007 c, d = f(ø)

et al. [85]
The correlation was proposed
(20) based on water/ethylene glycol
based alumina nanofluids.

6 ∅ %@ . Chen et 2007 aa = Effective radius of aggregates.

 =  (1 − : < : < ).
0.605 % al. [79]
an= Radius of nanoparticles
(21)
An updated version of Krieger-
Dougherty model

7  =  (1 + 10.6∅ + 112.36∅ ) Chen et 2007 The correlation was defined based

al. [86] on the experiment on ethylene
glycol-based TiO2 nanofluid.
(22)

8  =  × 0.904 ×  B.#9∅ Nguyen 2007 The equations were based on the

et al. [32] study of water-based alumina
nanofluids of 47nm and 36nm
(23) respectively.

 =  (1 + 0.025∅ + 0.015∅ )

(24)

9  =  (1.475 − 0.319∅ + Nguyen 2007 The equation was proposed based

et al. [32] on the experiments on CuO
0.51∅ + 0.0093∅ ) nanoparticles dispersed in water.

(25)
 10  =  (1 + 46.8∅ + 550.82∅ ) Williams 2008 The equation was developed
et al. [87] based on water-based ZrO2
nanofluids.
(26)

11 ∅ @ . Kole and 2011 A, B, C = Curve Fitting constants.

 =  (1 − * + * C+ ).
B. @D Dey [88]
Based on curve fitting of the
(27) viscosity data from the analysis on
gear oil-based CuO nanofluid.
One is without the temperature
consideration and the other is with
temperature consideration
ln  = E + 1000F/(; + G) respectively.

(28)

12  =  (1 − 34.87(% − Corcione 2011 an = diameter of nanoparticle

et al. [89]
% )B. ∅.B ) ab = equivalent diameter of base
fluid molecule
(29)
The equation to measure the
viscosity of nanofluids with
spherical shaped nanoparticles.

13  =  (1 + ∅)B.H9 Sundar 2012 Both relations are based on

et al. magnetic Fe3O4 nanoparticles in
[90] ethylene glycol and water
(30) mixture. The first one is for 40:60
and 20:80 ratios of EG and water
mixture and the second one is for
60:40 mixture of base fluid.

 =  (1 + ∅).B

(31)

14  = B (G + G  IJ1 ) Murshed 2013 C1, C2 and C3 are dimensionless

et al. [91] empirical co-efficients which are
functions of type of nanoparticles
(32) and concentration.

The correlation was developed

from the study on Si oil based
TiO2 nanofluid.

1 N @P Q
 = B (1 + KLM * + ∅O * + ))
15 Sharifpur 2015 Ω = System parameter
1. 5 et al.
[92] [µ] = Intrinsic viscosity
(33)
ap = Diameter of nanoparticle

h = Thickness of the capping layer

α, β, γ = Curve fitting constants.

The equation was obtained with

dimensional analysis based on the
experiment on Ethylene Glycol
based Alumina nanofluid.

190
191 Experimental Discussion

192 Water-Based TiO2 Nanofluid

193 Water-based TiO2 nanofluids are popular for engineering applications and numerous

194 investigations have analyzed the thermophysical properties of these nanofluids [40,57]. Most of

195 these studies are performed under variable temperatures and variable concentrations of

196 nanoparticles. In 2009, Duangthongsuk et al. performed an experiment to measure the

197 thermophysical property of a water based TiO2 nanofluid [49]. The measurements of viscosity

198 were taken with 0.2 to 2 vol. % particle concentration at 15 oC, 25 oC and 35 oC. The results

199 showed that the viscosity of the nanomaterial is a function of both the nanoparticle concentration

200 and temperature. With the increase in temperature, the viscosity of the nanofluid decreased.

201 However, the viscosity of the nanofluid increased by 4-15 % due to higher nanoparticle

202 concentration. Besides, it was also mentioned that measured viscosity exhibited similar results

203 when compared to the viscosity obtained from the analysis performed by He et al. [93] and there

204 was significant deviation from the analysis by Murshed et al.[94]. According to the authors the

205 most likely reasons for the deviation were the differences between particle size, shape and

206 measurement techniques in their experiment. Also, the nanofluids showed higher viscosity when

207 compared to the classical Einstein, Brinkman, and Batchelor equations. Based on the

208 experimental data, the authors proposed the following correlation for measuring viscosity:

209

210  =  (% + 0∅ + 2∅ ) (34)

211

212 where a, b and c are constant values from the experimental data.
213 In a similar study, Turgut et al. observed increase of the viscosity by 7.4 % with respect

214 to the base fluid when using a 3 vol. % concentration of deionized water with TiO2 nanoparticles

215 at 13 oC [95]. The experiment was performed at 13 oC, 23 oC, 40 oC and 55 oC while the particle

216 concentration was varied from 0.2 to 3 vol. %. Like the previous studies, the viscosity of the

217 nanofluid increased with increased particle size and decreased with increased temperature. Also,

218 when compared to the classical viscosity models like the Einstein, Brinkman, and Krieger-

219 Doughetry models, they determined viscosity was higher. The authors describe this increase in

220 the viscosity of the nanofluid due to the high interactions between the titania nanoparticles in the

221 base fluid.

222 In another study, Naina et al. investigated the viscosity of TiO2/water nanofluids over a

223 temperature range from 10 oC – 40 oC with nanoparticle concentration ranging from 0.5 to 2.5

224 vol. % [96]. These authors reported a maximum 50 % rise in the viscosity of the fluid at 2.5 vol.

225 % concentration of nanoparticles compared to the solvent at a temperature of 10 oC. The relative

226 viscosity of the system rises exponentially which was represented in the following equation:

227

228  =  (2.924 expL0.136∅ − 316.06/;M) (35)

229 In conjunction with the effect of temperature and volumetric particle concentration in the

230 base fluid, Silambarasan et al. also measured the effect of sonication time on the viscosity of

231 water-based TiO2 particle fluid system [97]. Although the TiO2 particles in the experiment were

232 more than 100nm in size, the measured viscosity of the fluid with respect to particle

233 concentration, temperature and sonication time can play a role to develop an effective system of

234 TiO2 nanofluid. The sub-micron titania particles were prepared using stirred bead milling and

235 ultrasonication processes. A linear increment of viscosity was observed with an increase in the
236 particle concentration of TiO2. The increase in viscosity was described as a result of increased

237 resistance of the fluid to deform at particular shear stress. Also, it was noted that the viscosity of

238 the fluid is affected by particle size and shape and state of aggregation according to previous

239 literature [79]. Sonication process disintegrates the particles into the solvent with sound energy

240 resulting in finer and more uniform nanoparticles [98]. Since this process affects the particle size,

241 it affects the viscosity. The results showed that the fluid provided lower viscosity for 7 h

242 sonication when compared to 6 h and no sonication of the fluid. The viscosity of the fluid was

243 observed to decrease with the increase in temperature from 29 oC to 55 oC.

244

245 Figure 4: (a) Dynamic viscosity water-based TiO2 nanofluid at different temperatures and

246 nanoparticle concentration. (b) Comparison of viscosity ratio of the experiment with various

247 models for water-based TiO2 nanofluid [62].

248 In 2013, Yiamsawas et al. conducted an experiment to measure the viscosity and

249 observed the rheological behavior of water-based TiO2 and Al2O3 nanofluids [62]. The

250 nanofluids were synthesized by dispersing the alumina and titania nanoparticles into water and

251 varying the nanoparticle concentration from 1 to 8 vol. %. The addition was followed by
252 ultrasonication of nanofluid for 2 hours. The experiment was performed under temperatures

253 ranging from 15 – 30 oC. It was observed that the viscosity decreased with increasing

254 temperature (Figure 4(a)). The results also presented a constant increase of viscosity with the

255 increase of volumetric concentration of nanoparticle. TiO2/water nanofluids also showed a lower

256 viscosity compared to the observed viscosity of an Al2O3 nanofluid at 4 vol. % particle

257 concentration. The authors concluded that the higher viscosity of Al2O3 was due to its larger size.

258 The authors also compared the viscosity ratio of the study with the Einstein, Brinkman,

259 Batchelor and Corcione models in which the TiO2 nanofluids showed higher viscosity than the

260 Einstein, Brinkman and Batchelor models and lower than the Corcione model (Figure 4(b)).

261 Based on the analysis the authors proposed the following correlation:

262

263  = %∅ ; U  (36)

264

265 where a, b and c are constants from the analysis which are different for both nanofluids.

266 In numerous studies, researchers investigated the rheological behaviour of TiO2

267 nanofluids. Some of these nanofluids showed Newtonian behavior while others displayed non-

268 Newtonian behavior. In a recent study, Bobbo et al. synthesized water based single wall carbon

269 nanohorn (SWCNH) and TiO2 nanofluids and examined their rheological behavior and the effect

270 of temperature and particle concentration [99]. The nanofluids were prepared using the two-step

271 method, with concentrations of 0.01, 0.1 and 1 % of nanoparticle by mass. The TiO2 and

272 SWCNH nanofluids were stabilized with PEG and sodium n-dodecyl sulphate (SDS),

273 respectively. The concentrations of additives used were 0.02, 0.2, and 2 % by mass for PEG and

274 0.03, 0.1, and 2 % by mass for SDS. The results showed that at 0.1 mass % and 0.01 mass %,
275 TiO2 nanoparticles have almost no influence on the base fluid as they provided almost a similar

276 value as the base fluid. On the other hand, the TiO2 nanofluid with a 1 % mass concentration

277 showed a 7 % rise of viscosity compared to the base fluid. Similarly, the SWCNH nanofluid with

278 1 % mass concentration of nanoparticles showed 13 % increase of viscosity compared to the base

279 fluid. However, the addition of nanoparticles by 0.01 mass % and 0.1 mass % showed similar or

280 lower viscosity than that of pure water. It was concluded by the authors that low mass

281 concentration of nanoparticles had very little effect on the viscosity of the nanofluid.

282 Furthermore, it was shown that both fluids displayed Newtonian behavior since the shear stress

283 increased linearly at a constant rate while the viscosity remained constant for shear rates from

284 200 s-1 to 1600 s-1.

285 Fedele et al. conducted an investigation on the rheological behavior and dynamic

286 viscosity of water based TiO2 nanofluids at 283-343 oC [50]. The nanoparticle concentration was

287 varied from 1 wt. % to 35 wt. %. The results showed that the nanofluid exhibited a Newtonian

288 behavior as the shear stress was observed to follow a linear function of shear rate between 400-

289 1400 s-1. It was also observed that the nanofluid showed water-like behavior at 1 wt%

290 concentration while the viscosity increased significantly at higher concentrations. The data

291 showed an increase in viscosity up to 243 % respect to the based fluid at 343 K and a

292 concentration of 35 wt. %.

293

294 Figure 5: Graphical representation of Viscosity and Shear stress vs Shear rate of TiO2/water

295 nanofluids at different concentrations of nanoparticles [100].

296 Similar results were reported by Arulprakasajothi et al., who observed that TiO2/water

297 nanofluids showed Newtonian behavior for 0.1 vol. % to 0.75 vol. % concentration of TiO2

298 nanoparticle [101]. However, at higher particle concentration, higher values of viscosity were

299 observed with a maximum increase of 13.2 % observed at 0.75 vol. % nanoparticle

300 concentration. In another study by Said et al., the TiO2/water nanofluid showed both Newtonian

301 and non-Newtonian behavior [100]. The experiments were performed at 25-80 oC with water

302 based TiO2 nanofluid containing nanoparticles at concentrations ranging from 0.05 to 0.3 vol. %

303 The nanofluid was synthesized using the two-step method. The nanofluid exhibited Newtonian

304 characteristics at 0.3 % particle concentration. The viscosity remained constant and the shear

305 stress increased linearly with shear rate. However, at 0.1 percent concentration, the nanofluid

306 showed non-Newtonian behavior at temperatures below 55 oC. Figure 5 shows the effect of shear
307 rate on viscosity and shear stress at different concentrations of the nanofluid. In addition, the

308 authors observed a hysteresis behavior of nanofluid from these experiments. As the nanofluid

309 with concentrations of 0.1vol. % and 0.3 vol. % were cooled down, the viscosity deviated and

310 followed a different path when compared to path observed during the heating process. This

311 hysteresis effect was small compared to the hysteresis reported by Nguyen et al. who performed

312 studies for higher concentration nanofluids [102]. Das et al. studied the effect of surfactants on

313 the viscosity of TiO2/water nanofluid at various particle concentrations and temperatures [103].

314 The nanoparticle concentration was varied from 0.1 to 2 % by volume while the temperature

315 ranged from 20 oC to 60 oC. Four type of surfactants were used in this study. Only cetyl trimethyl

316 ammonium bromide (CTAB) and acetic acid (AA) were proven effective in stabilizing the

317 suspension. The nanofluid stabilized with CTAB showed higher viscosity compared to the

318 nanofluid stabilized with AA at 20 oC with values of 1.65 mPa·s and 1.54mPa·s for 2 vol. % of

319 particle concentration, respectively. This represented a marginal increase in viscosity with

320 increase of particle concentration. However, at higher temperature this increase was negligible

321 showing less effect of surfactants on the viscosity of nanofluid at higher temperatures. In

322 agreement with the studies discussed above, the viscosity was observed to increase with

323 increased particle size and decrease with increased temperature. The authors also pointed out

324 shear thinning of the nanofluids at shear rates below 400 s-1 from the experimental measurement

325 of the nanofluid viscosity at 76 s-1 to 760 s-1 shear rate. However, shear thickening was observed

326 for shear rates above 400 s-1 as viscosity gradually increased with increased shear rate. The

327 change of viscosity with shear stress suggest non-Newtonian behavior of the nanofluid.
328

329 Figure 6: Viscosity vs Shear rate of water based Al2O3/TiO2 hybrid nanofluid [51].

330

331 Moldoveanu et al. reported the preparation and rheological study of a water-based

332 Al2O3/TiO2 hybrid nanofluid [51]. Accordingly, aqueous dispersions of TiO2 nanoparticle at

333 concentrations 0.50 vol. %, 1.00 vol. % and 1.50 vol. % and 0.50 vol. % were prepared. The

334 rheological behavior of the nanofluid was studied at shear rates varying from 10 s-1 to 1000 s-1 at

335 25 oC . Experiments with TiO2 and Al2O3 nanofluids individually were conducted for

336 comparison. The results showed an increase in viscosity with increased concentration of TiO2

337 nanoparticles in the nanofluids. Interestingly, the viscosity of the nanofluid containing 0.5 vol. %

338 Al2O3 and 0.5 vol. % TiO2 was higher than the the viscosity of suspensions containing higher

339 concentrations of TiO2 at 1 vol. % and 1.5 vol. % with 0.5 vol. % of Al2O3 (Figure 6). The

340 hybrid nanofluid also showed non-Newtonian and shear thinning behavior similar to the simple

341 alumina and titania nanofluids.

342 Ethylene Glycol Based TiO2 Nanofluid

343 Ethylene glycol (EG) has been used as the base fluid in the preparation of TiO2

344 nanofluids because of its heat transfer characteristics and wide availability. In 2011, Cabaleiro et

345 al. studied the rheological behaviour of EG-based TiO2 nanofluids between 293.15 K and 313.15

346 K using the anatase and rutile forms of the nanoparticles [37]. The nanoparticles were used in 5-

347 25 % concentration by mass, which was also noted as 1.51-8.83 vol. % concentration for the

348 anatase nanoparticle and 1.36-8.08 vol. % concentration for rutile nanoparticle. The nanofluid

349 employing the rutile structure showed higher viscosity compared to the nanofluid using anatase

350 at same temperatures and same mass concentrations. It was observed that the viscosity decreased

351 with temperature. However, the viscosity was independent of temperature at a shear rate of 10 s-
1
352 . The nanofluids containing either polymorph showed shear thinning non-Newtonian behaviour,

353 in disagreement with the Newtonian behaviour of EG based TiO2 nanofluid with 0.5 to 0.8 %

354 reported by Chen et al. [79].

355 In another study using TiO2/EG nanofluid, Khedkar et al. reported Newtonian behavior

356 as well as shear thinning of the nanofluid [55]. The study was conducted at temperatures ranging

357 from 283 to 323 oC with 0-7 vol. % of nanoparticle concentration in the nanofluid. The nanofluid

358 was prepared using the two-step method and included ultrasonication of nanoparticle under sol-

359 gel method. The shear viscosity was constant with increasing shear rate but decreased with

360 increasing temperature. Increasing the concentration of nanoparticles caused an increase of the

361 viscosity as well as shear thinning behavior of the nanofluid. The highest increase in viscosity

362 (27 % respect to the base fluid) was observed at 5 vol. % of nanoparticles.

363 Shu et al. reported Newtonian pseudoplastic transition for EG based titania nanofluids

364 with 0-35 wt% of TiO2 nanoparticles from 25 to 45 oC [38]. Below 5 wt. %, viscosity remained
365 almost fairly constant at different shear rates. On the other hand, the nanofluid exhibited

366 pseudoplastic behaviour at concentrations between 5 and 25 wt. %. Both shear thinning and

367 Newtonian behavior was observed within this range (Figure 7). The nanofluids exhibited only

368 shear thinning behaviour at concentrations above 25 wt. %. The authors also noted that

369 temperature had very little effect on the viscosity of the nanofluid compared to the base fluid.

370

371 Figure 7 : Viscosity vs Shear rate of EG based TiO2 nanofluid at 0-35 wt. % concentration of

372 nanoparticle [38].

373 Akilu et al. reported the preparation and rheological and thermal properties of EG-based

374 TiO2-CuO/C hybrid nanofluids [52]. The wet mixing approach was used to synthesize TiO2-

375 CuO/C nanocomposite maintaining the ratio of TiO2 and CuO/C 80:20 by weight. The

376 nanocomposite was dispersed in EG by the two-step method using 0.5%, 1%, 1.5% and 2%

377 concentration by volume at temperatures between 303.15 and 333.15 K. The results showed that

378 viscosity was a direct function of temperature and particle concentration as reported in the
379 literature. The viscosity was observed to decrease rapidly at higher temperatures. The authors

380 suggested that the decrease in viscosity was due to the weakening of Van Der Waals forces,

381 which resulted in less resistance during fluid flow. The relative viscosity was observed to be

382 independent of the temperature of the experiment. A maximum increase of 80 % in viscosity of

383 the nanofluid was reported for 2 vol. % particle concentration at 313.4 K. The authors attributed

384 the enhancement of viscosity with particle size to the interaction between the nanocomposite and

385 EG. Also, the relative viscosity of the nanofluid was recorded as 1.13, 1.31, 1.56 and 1.77 for

386 0.5%, 1%, 1.5% and 2% nanofluid concentration, respectively. Furthermore, the authors showed

387 the nanofluid exhibited Newtonian behavior as the viscosity remained constant with shear rate

388 from 20 s-1 to 200 s-1. Based on the results of the study the authors proposed the following co-

389 relation to measure the viscosity of EG based TiO2-CuO/C nanofluid.

390

,D ∅ .9 1
391 = 0.9653 + 77.5667 * + ( )B.H99 (37)
,- BB 

392 Ethylene Glycol/Water Based TiO2 Nanofluid

393 Yiamsawas et al. studied the rheology of EG/water based TiO2 and Al2O3 nanofluid at a

394 temperatures from 15 to 60 oC [53]. The EG-water mixture base fluid was chosen because of its

395 enhanced heat transfer and thermophysical properties. The authors utilized TiO2 and Al2O3

396 nanoparticles of 21 and 120 nm, respectively dispersing them into the 20:80 wt. % EG/Water

397 mixture. The resulting nanofluids were 1%, 2%, 3% and 4% by volume. The results showed that

398 the dynamic viscosity increased with increasing nanoparticle size whereas the dynamic viscosity

399 decreased with increasing temperature. The nanofluid was also determined to behave as a

400 Newtonian fluid. In addition, it was observed that the Al2O3 nanofluid exhibited higher dynamic
401 viscosity than the TiO2 nanofluid. The authors attributed this behavior to the higher particle size

402 of Al2O3. It was also stated that a higher complex flow pattern and inertia could be the reason for

403 higher resistance for particles more than 100nm. Furthermore, the classical models failed to

404 describe the viscosity of the nanofluid, since they are more suitable for low concentration

405 nanofluids. The authors proposed the following correlation to measure the viscosity of the

406 EG/water based Al2O3 and TiO2 nanofluid.

407

408  = E∅V ; I  W (38)

409

410 The coefficients A, B, C and D are different for Al2O3 and TiO2 nanofluids. In a similar

411 study, Hamid et al. observed exponential decrease of the dynamic viscosity of the nanofluid with

412 temperature for TiO2 nanofluid containing nanoparticles of 0.5, 1 and 1.5 % volume

413 concentration dispersed in a mixture of EG and water by 40:60 volume ratio [104]. The dynamic

414 viscosity of the nanofluid was observed to be higher than the ASHRAE data at a temperature

415 range of 30-70 oC [105].

416

417 Figure 8 : (a) Dynamic viscosity and (b) Relative viscosity of EG/Water based TiO2-SiO2 hybrid

418 nanofluid at different temperature [54].

419

420 Nabil et al. performed studied the rheological behavior of EG/water based TiO2-SiO2

421 hybrid nanofluid at a temperature range from 30 to 80oC [54]. The nanoparticle concentration of

422 the mixture varied from 0.5 to 3% by volume while the volumetric ratio of water to EG was

423 maintained at 60:40. The nanofluid showed Newtonian behavior as the shear stress increased

424 linearly at a constant rate with the shear rate from 25 s-1 to 175 s-1 at 30 and 50 oC temperature.

425 An exponential decrease of dynamic viscosity with the increase of temperature was also

426 observed. Figure 8 shows the dynamic viscosity (a) and relative viscosity (b) of nanofluid
o
427 between 30 and 80 C. The authors attributed this phenomenon to the weakening of

428 intermolecular bonding of the molecules due to the increase in temperature. In addition, both the
429 dynamic viscosity and the relative viscosity of the nanofluid increased with the increase in

430 particle concentration. The authors observed 62.5 % increase of relative viscosity for 3 vol. %

431 concentration of nanofluid. The higher viscosity of the nanofluid with respect to the base fluid

432 was attributed to the increase of the internal shear stress of the fluid from dispersing

433 nanoparticles into the base fluid. Furthermore, the fluctuation of relative viscosity over the

434 temperature range was reasoned to be due to the difference in the thickness and structure of the

435 diffused fluid layers. Based on the experimental results discussed above the Table 4 summarizes

436 some of the findings.

437

438 Table 4: Some Experimental Findings on the Viscosity of Water and EG based TiO2 Nanofluids.

Nanofluid Viscosity with increasing Maximum rise of viscosity observed for Rheological Reference
temperature nanoparticle application Behaviour

Water based Decreases linearly 15% - [49]

TiO2

Water based Decreases exponentially 7.4% - [95]

TiO2

Water based - 13.2% Newtonian [101]

TiO2

EG based TiO2 Decreases exponentially 27% Newtonian [55]

EG based TiO2 - 329 times Newtonian and non- [38]

Newtonian

EG/Water based Decreases exponentially 55% - [53]

TiO2

EG/Water based Decreases exponentially 62.5% Newtonian [54]

TiO2

439

440

441

442
443

444 Conclusions

445 This article provides an overview of the recent investigations into the Ethylene Glycol,

446 Water and EG/Water based TiO2 nanofluids. Some of the classical and new experimentally

447 developed models are discussed herein. It is evident from the literature that temperature and

448 nanoparticle concentration are important parameters in determining the viscosity of nanofluids.

449 In the majority of the experiments discussed in this review, the viscosity of the TiO2 nanofluids

450 was observed to decrease with increasing temperature. The viscosity of the nanofluid was found

451 to increase with the addition of TiO2 compared with the base fluid. Furthermore, the viscosity of

452 the nanofluids was found to increase with the increase of nanoparticle concentration in the

453 majority of the studies reported. The Newtonian and non-newtonian behaviour of TiO2

454 nanofluids respect to shear rate has also been extensively investigated. The outcomes from these

455 investigations are significant to the applications of TiO2 nanofluids. Although these experiments

456 are mostly focused on the effect of temperature and concentration on the viscosity of TiO2

457 nanofluid, more experiments can be performed to thoroughly understand the effect of pH,

458 aggregation, particle size and base fluid mixture. Further, more types of TiO2 based hybrid

459 nanofluids can be synthesized with different metal oxides and investigated to gain a better

460 understanding of viscosity and expected fluid flow characteristics. Effective study of hybrid

461 nanofluids can result in new type of nanofluids with better rheological properties that can

462 ameliorate the heating, cooling and lubricating system and contribute towards better efficiency in

463 industrial processes.

464
465

466

467 Acknowledgement

468 The authors would like to acknowledge the Graduate College, University of Texas Rio

469 Grande Valley (UTRGV) for the Presidential Graduate Research Assistantship to Abu Musa

470 Abdullah. Besides, the authors are thankful to the College of Science, UTRGV for the Dean’s

471 Research Assistantship to Aminur Rashid Chowdhury. Also, the authors thank the College of

472 Computer Science and Engineering for their support. The Department of Chemistry at the

473 UTRGV is grateful for the generous support provided by a department grant from the Welch

474 Foundation (Grant No. BX-0048).

475

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765

766
Highlights
• Viscosity of TiO2 nanofluid at variable physical parameters has been reviewed
• Classical and experimental viscosity models of nanofluids have been discussed
• Preparation techniques of TiO2 nanofluid have been discussed
• Viscosity of TiO2 nanofluid can increase by 329 times compared to the base fluid
• Viscosity of TiO2 nanofluid decreases significantly with increasing temperature