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Articulo Newthermophysical Properties of Water Based TiO2 Nanofluid—the Hysteresis Phenomenon Revisited
Articulo Newthermophysical Properties of Water Based TiO2 Nanofluid—the Hysteresis Phenomenon Revisited
a r t i c l e i n f o a b s t r a c t
Available online 3 September 2014 Homogeneous stable suspensions acquired by dispersing dry Al2O3 and TiO2 nanoparticles in controlled pH
solution and distilled water, respectively, were prepared and investigated in this study. First of all, the mean
Keywords: nanoparticle diameters were studied by dynamic light scattering (DLS) technique, and the nanofluid stability
Nanofluid was analyzed by zeta potential measurements. The nano-crystalline structures were characterized by scanning
Thermal conductivity electron microscope and transmission electron microscope. The rheological behavior was determined for both
Viscosity
nanofluids at nanoparticle volume concentrations up to 0.3%. The effect of temperature for the heating and
Hysteresis
Density
cooling phases was analyzed from 25 °C to 80 °C. Furthermore, the influence of temperature, pressure drop,
Pumping power pumping power, zeta potential, size and densities were analyzed for fresh prepared samples as well as for
samples used in a flat plate solar collector over a period of 30 days. The thermal conductivity enhancement of
the two nanofluids demonstrated a nonlinear relationship with respect to temperature and volume fraction,
with increases in the volume fraction and temperature. All resulted in an increase in the measured enhancement.
Existence of a critical temperature was observed beyond which the particle suspension properties altered dras-
tically, which in turn triggered a hysteresis phenomenon. The hysteresis phenomenon on viscosity measurement,
which is believed to be the first observed for Al2O3/water and TiO2/water-based nanofluids, has raised serious
concerns about the use of nanofluids for heat transfer enhancement. The pressure drop and pumping power of
the nanofluid flows are found to be very close to those of the base liquid for low volume concentration. It may
be concluded that nanofluids can be utilized as a working medium with a negligible effect of enhanced viscosity
and/or density. Our findings provide a view on the thermo physical properties of nanofluids that is compared
with that in the literature, and new findings (such as viscosity, hysteresis phenomenon and pumping power)
have been presented, which are not available in literature as yet.
© 2014 Elsevier Ltd. All rights reserved.
1. Introduction are immersed in base fluids. The main reason for this is to enhance
the heat transfer characteristics of conventional fluids by improving
Conventional fluids, such as water, engine oil, and ethylene their thermal conductivity. In the previous decade, nanofluids have
glycol, are usually used as heat transfer fluids. Their poor heat trans- achieved considerable devotion due to their enhanced thermal con-
fer rate is understood as an obstacle for enhancing efficiency of heat ductivities. In this regard, Eastman et al. [1] reported that the ther-
exchangers. A novel type of heat transfer fluids called “nanofluids” is mal conductivity of the conventional fluid upsurges by 40%, when
recognized for enhancement of heat exchanges for better perfor- 0.3% of copper nanoparticles were suspended in ethylene glycol.
mance. Nanofluids are two phase fluids where solid nanoparticles Pak and Cho [2] carried out an experimental work for the determina-
tion of forced convection heat transfer coefficients with 13 nm Al2O3
and 27 nm TiO2 sub micron particles dispersed in water. For a fixed
Abbreviations: FESEM, field emission scanning electron microscopy; SEM, scanning Reynolds number, the convective heat transfer coefficient was
electron microscopy; TEM, transmission electron microscopy. improved by 75% for an Al2O3 particle concentration of 2.78%. Heat
☆ Communicated by W.J. Minkowycz. transfer coefficients were also observed to increase with concentra-
⁎ Corresponding author at: Department of Mechanical Engineering, Faculty of
tion. Such outcomes have driven both the industrial and scientific
Engineering, University of Malaya, 50603 Kuala Lumpur, Malaysia.
E-mail addresses: saidur@um.edu.my, saidur912@yahoo.com, zaffar.ks@gmail.com community to examine the heat transfer and rheological properties
(R. Saidur). of nanofluids.
http://dx.doi.org/10.1016/j.icheatmasstransfer.2014.08.034
0735-1933/© 2014 Elsevier Ltd. All rights reserved.
86 Z. Said et al. / International Communications in Heat and Mass Transfer 58 (2014) 85–95
Table 1
Analytical models on the thermal conductivity of nanofluids [23,26–30].
3
Yu and Choi [27,28] kpe þ 2kb þ 2 kpe −kb ð1−β Þ ϕ Modified Maxwell model, modified Hamilton–Crosser model
;
kpe þ 2kb − kpe −kb ð1 þ β Þ3 ϕ
nϕeff A
1þ ð2Þ
1−ϕeff A
2
Xie et al. [29] 2Θ2 ϕT Effect of nanolayer is included
1 þ 3ΘϕT þ ð3Þ
1−ΘϕT
knf
Effective medium theory [23,30] ¼ 1 þ 3φ ð4Þ
k0
2.2. Nanofluid preparation and characterization 2.3. Thermal conductivity calculation and measurement
The nanofluids were prepared following a two-step method. Ultra- Presently, there is no reliable theory to predict the anomalous ther-
sonicator and high pressure homogenizer (capacity of up to 2000 bar) mal conductivity of nanofluids. From the experimental results of many
were used to dissolve the nanoparticles (0.1% and 0.3%v/v) into distilled researchers, it is recognized that the thermal conductivity of nanofluids
water. depends on parameters, including the thermal conductivities of base
Field emission scanning electron microscopy (FESEM) from the fluid and nanoparticles, volume fraction, surface area, shape of nanopar-
SIGMA Zeiss instrument (Carl Zeiss SMT Ltd., UK) and transmission ticles, and temperature. To predict the effective thermal conductivity of
electron microscope (TEM) were used to achieve the morphological nanofluids, a number of theoretical and empirical models have been
characterization of the nanoparticles. A zeta-seizer Nano ZS (Malvern) proposed [12,22–25]. Table 1 contains some popular models, which
was used to analyze the average size of the nanoparticles in base will be used to compare our experimental results later. KD2 Pro thermal
mediums. It gave the hydrodynamic radius of the particles dispersed property analyzer (Decagon, USA) was used to measure thermal con-
in a medium using DLS approach. ductivity of the nanofluids.
Table 2
Most cited correlations of nanofluid viscosity [25,34–39].
Einstein [34] μ nf ¼ μ bf :ð1 þ 2:5ϕÞ ð5Þ Valid for very low volume concentrations
(ϕ ≤0.02) and spherical particles
Brinkman [35] 1 Formulated by two corrections of Einstein's model
μ nf ¼ μ bf : ð6Þ
ð1−ϕÞ2:5
Batchelor [36] 2 Considered the effect of Brownian motion.
μ nf ¼ μ bf : 1 þ 2:5ϕ þ 6:5ϕ ð7Þ
Extension of the Einstein model.
Abu-Nada et al. [37] μ Al2 O3 ¼ expð3:003−0:04203T Includes temperature T and volume fraction ϕ.
2 Modified model of Nguyen.
−0:5445ϕ þ 0:0002553T
2 −1
−0:0534ϕ −1:622ϕ Þ ð8aÞ
μ H2 O ¼ −81:1 þ 98:75 ln ðT Þ
2 3
−45:23 ln ðT Þ þ 9:71 ln ðT Þ
4 5
−0:946 ln ðT Þ þ 0:03 ln ðT Þ ð8bÞ
Masoud Hossein et al. [38] T Based on Nguyen et al. [25] experimental data.
μ nf ¼ μ bf : exp m þ α þ β ð ϕÞ
T0
dp
þγ ð9aÞ
1þR
R ¼ 1nm ð9cÞ
2
Maiga model [39] μ nf ¼ μ bf : 123ϕ þ 7:3ϕ þ 1 ð10Þ Derived from Al2O3/water nanofluids.
88 Z. Said et al. / International Communications in Heat and Mass Transfer 58 (2014) 85–95
ρV 2 Δl ρV 2
Δp ¼ f þK ð11Þ
2 d 2
The loss coefficient K is often taken from table's results from tests or
calculated using formulas that consist of the density and kinematic
Fig. 1. Particle diameter distribution, according to the intensity, for water–Al2O3 0.1% viscosity of the heat transfer fluid. V is the mean flow velocity of
nanofluids with pH 9, just after preparation, after 7 days and after 30 days. nanofluids in the system, and is given by
ṁ
V¼ ð12Þ
ρnf πD2H =4
64
f ¼ for laminar flow
Re
0:079
Fig. 2. Particle diameter distribution, according to the intensity, for water–TiO2 0.1% f ¼ for turbulent flow:
nanofluids, just after preparation, after 7 days and after 30 days. ðReÞ1=4
Fig. 3. Particle diameter distribution (Z-Average size: 196.4 nm), according to the intensity, for water–Al2O3 0.1% nanofluids with pH 9, after running for 30 days in a system.
Z. Said et al. / International Communications in Heat and Mass Transfer 58 (2014) 85–95 89
Fig. 4. Particle diameter distribution (Z-Average size: 225.9 nm) according to the intensity, for water–TiO2 0.1%v/v nanofluids, after running for 30 days in a system.
3. Results and discussions for water–Al2O3 was (Z-Average size: 109.4 nm) with an initial zeta
potential value of 58.4 (mV), whereas the particle diameter increased
Fig. 1 shows the particle size distribution according to the intensity to (Z-Average size: 196.4 nm), with an increment of 87 nm and zeta
obtained from the zeta-seizer at a different interval of days while TEM potential value reduced to 40.2 (mV) after the solution was used in
and SEM images are indicated in Figs. 2 and 3, respectively. a flat plate solar collector for 30 days. In the case of water–TiO2 0.1%
Fig. 1 shows a size distribution graph of the aggregates in the nanofluids, the initial particle diameter was (Z-Average size: 126.9 nm)
nanofluid at different times after preparation. The peak of the distri- with an initial zeta potential value of 48.6 (mV), whereas the particle
butions is at almost identical horizontal position. Their intensity, diameter increased to (Z-Average size: 225.9 nm), with an increment of
however, increases vertically witnessing an increase in population 99 nm and zeta potential value reduced to 36.7 (mV) after the solution
of aggregates. was used in a flat plate solar collector for 30 days.
Similar pattern as in Fig. 1 is observed here in Fig. 2. The elevation of
the distributions is at almost identical horizontal position; however, 3.1. Thermal conductivity
their intensity rises vertically witnessing a growth in population of
aggregates, which is larger compared to Al2O3–water. Therefore, it can Experimentally calculated thermal conductivity of the pure base
be said from the particle diameter graph that Al2O3–water nanofluid is fluids with our device presented a good agreement with the available
more stable compared to TiO2–water. literature data. From Figs. 7 and 8, it is witnessed that the thermal con-
Figs. 3 and 4 represent the particle diameter distribution of water– ductivity grows with the increment in volume fraction, which is almost
Al2O3 0.1% nanofluids with pH 9 and water–TiO2 0.1% nanofluids, after linear. A small dissimilarity is detected in measured thermal conductiv-
running for 30 days in a system, respectively. Initial particle diameter ity associated with the projected values obtained from the effective
Fig. 5. (a) SEM image of Al2O3 nanoparticles, (b) SEM image of TiO2 nanoparticle, (c) TEM image of Al2O3 nanoparticles with controlled pH and (d) TEM image of TiO2 nanoparticles.
90 Z. Said et al. / International Communications in Heat and Mass Transfer 58 (2014) 85–95
Fig. 6. Visual images of Al2O3 & TiO2 right after preparation and after being used in a flat plate solar collector for 30 days with 0.1% and 0.3% volume fraction.
medium theory [19,42]. As perceived from the TEM images in Fig. 5, that material properties of both particle and carrier fluid was attributed to
the particles are not wholly spherical, thus, resulting in a lower thermal the long impact range of the antiparticle potential, which influenced the
conductivity. For spherical nanoparticles and a lower volume fraction, particle motion. Visual images of Al2O3 & TiO2 right after preparation
thermal conductivity was projected to be greater compare to other and after being used in a flat plate solar collector for 30 days with 0.1%
shaped nanoparticles. and 0.3% volume fraction are presented in Fig. 6. No sign of sedimentation
It is perceived from these models that the projected values were not was noticed for this period of study, through visual means as well.
nearly comparable to the experimental values. The thermal behavior of Fig. 7 shows the thermal conductivity enhancement in water with
the nanofluids is depended on the Brownian motions at nano-scale and Al2O3 nanoparticles suspended in it with respect to different volume
molecular level, which was reported by Jang et al. [43]. concentration, which is similar with the results published in the
In summary, it is problematic to classify a recognized theory to predict literature [23,46,47]. The deviation of the experimental values of the
precisely heat transfer characteristics of nanofluids. Numerous investiga- estimated values of thermal conductivity of Al2O3/water nanofluids is
tors deal with the nanofluids as single-phase fluid rather than a two phase considerably high. Effective medium theory estimates a high value. Al-
mixture. The particle–liquid interaction and the movement between the though Timofeeva et al. [51] concluded in their work that the effective
particle and liquids, however, play significant parts in affecting the con- medium theory is adequate for measuring the thermal conductivity of
vective heat transfer performance of nanofluids [44]. The strong depen- nanofluids, which was found to be applicable for Al2O3/EG nanofluids
dence of the effective thermal conductivity on the temperature and [5] rather than Al2O3/water nanofluids.
Fig. 8 shows the effects of temperature and different volume concen-
trations. It is observed from the figure that the thermal conductivity
Fig. 9. Uncertainty in experimental data of viscosity of Al2O3–water nanofluid with 13 nm, 0.1% volume concentration and at 35 °C.
increases with the increasing volume concentration as well as the rising Uncertainty in viscosity measurement of water based alumina
temperature. These results followed a similar pattern as that of Fedele nanofluid is presented in Fig. 9 and uncertainty in viscosity measure-
et al. [45]. The experimental results demonstrated a peak in the en- ment of water based titanium nanofluid is presented in Fig. 10. The ef-
hancement factor in this range of volume fractions in the temperature fect of temperature and volume fraction on viscosities of Al2O3–water
range evaluated, which implies that an optimal size exists for different nanofluid is presented in Fig. 11. For the nanofluid samples after the
nanoparticle and base fluid combinations. This phenomenon can be use in a system over a period of 30 days, the water-based alumina
neither predicted nor explained using the theoretical models currently nanofluid at 0.3%v/v showed Newtonian behavior below temperature
available within the literature. 30 °C, whereas above this temperature, non-Newtonian behavior was
observed, as shown in Fig. 11.
3.2. Rheological behavior of nanofluids For the nanofluid sample with 0.1%v/v, the water-based alumina
nanofluid behaved as a Newtonian fluid above 40 °C, whereas below
As discussed earlier, only a few numbers of studies have been carried this temperature, it behaved as a non-Newtonian fluid, presented in
out about the rheological behavior of nanofluids in the past decade, and Fig. 12. As it is observed from the figure, with continuous running of
there are contradictions such as Newtonian and non-Newtonian behav- the solution in the system, the viscosity of the solution became almost
iors stated for the similar nanofluid as well as inconsistencies in the effects a constant value with few changes compared with the viscosity of the
of temperature, particle size, shape and great shear viscosity values solution, which was taken right after preparation with higher changes
[48–51]. In this context, an important matter is to achieve nanofluid phys- in values with the same temperature.
ical information, and one of the possible techniques is through a compre- From 55 °C, the TiO2 nanofluid with 0.1% volume fractions was
hensive rheological investigation [52]. In this experiment, three kinds of Newtonian, whereas below this temperature, TiO2 nanofluid with 0.1%
studies, namely viscosity as a function of shear rate, temperature as well was non-Newtonian, presented in Fig. 14. For 0.3%v/v of TiO2, a
as at different mass concentrations, have been conducted. Newtonian behavior was observed in the entire temperature range in
It is worth noting that the aforementioned equations were Fig. 13.
established to relative viscosity as a function of particle volume fraction
only. There is no equation to narrate temperature. Furthermore, these 3.3. Hysteresis loop
equations are for homogenous fluid and do not take into account parti-
cle agglomeration effect. Nanofluids showed lower viscosities when the We have noted that the viscosity of nanofluid reduces with an in-
nanoparticles were dispersed in base fluids. crease in the temperature without coming back through the same
In a Newtonian fluid, the relation between the shear stress and the path but was deviated upward when it was allowed to cool down. The
shear rate is linear, passing through the origin; the constant of propor- phenomena are presented in Figs. 15 and 16.
tionality is called the coefficient of viscosity. In a non-Newtonian fluid, For water based alumina nanofluids with 0.1%v/v concentrations, the
the line never passes through the origin. intersection point occurs at 80 °C, whereas in case of water based
Fig. 10. Uncertainty in experimental data of viscosity of TiO2–water nanofluid with 13 nm, 0.1% volume concentration and at 35 °C.
92 Z. Said et al. / International Communications in Heat and Mass Transfer 58 (2014) 85–95
the impact of hysteresis was very low, compared to higher volume con-
centrations, which was investigated by Nguyen et al. [25,26]. The temper-
ature difference from the point of interaction was noticed for the same
volume concentration before and after using the solutions in the system.
The reason behind this shift could be a possible result from the aggrega-
tion of the nanoparticles, which have shown increment in their particle
size diameter over a period during a month (as indicated in Figs. 1 to 4
as well as the effect of rusting on the nanoparticles, which affected the
pH of the solution and hence resulted in particle aggregation and
affecting the stability of the solution for the long-term in a system.
The experimental results reveal that the path for 0.1% intersects at a
temperature of 65.2 °C for the TiO2/water nanofluid and for 0.3%, the
path intersects at 68 °C. Such a phenomenon still remains not very
well understood. It was noted from the measured results that the
extraordinary improvement of nanofluid viscosity happened through
Fig. 11. Effect of temperature and volume fraction on viscosities of Al2O3–water
nanofluids. the cooling phase of the suspensions. No work is accessible to clarify
this behavior of nanofluids.
alumina nanofluids with 0.1% & 0.3%v/v concentrations, the intersection
point occurs at 67 °C and 82 °C, respectively. Hence, one can say that the 3.4. Pumping power and pressure drop
temperature level, at which the suspensions were heated, was very sig-
nificant for the possible impact of the viscous behavior of nanofluids. It is vital to study the flow resistance of nanofluids in order to im-
Since very low volume concentrations of nanoparticles was considered, prove their heat-transfer characteristics, so that the nanofluid can be
Fig. 12. Viscosity and shear stress versus shear strain rate for 0.05%v/v & 0.1%v/v Al2O3/H2O nanofluids at 35 °C.
Fig. 13. Viscosity of TiO2–water nanofluid with different volume concentrations and different temperatures.
Z. Said et al. / International Communications in Heat and Mass Transfer 58 (2014) 85–95 93
Fig. 14. Viscosity and shear stress versus shear strain rate of 0.05% to 0.5%v/v TiO2/H2O nanofluids at 40 °C.
appropriately used in the solar collector. The pressure drops of water at temperatures ranging from 25 °C to 80 °C. We have also listed some
and EG/water mixture based alumina nanofluids in a flat plate solar col- key concluding remarks as follows:
lector were theoretically examined considering the laminar flow.
Nanofluids with Al2O3 & TiO2 nanoparticle volume concentrations a. The effect of pH on the stability of the Al2O3–H2O suspension was
are engaged in the pressure drop calculation. Fig. 17 presents a variation critical. At pH 9.0, a good dispersion of alumina particles was obtain-
of the pumping power and the pressure drop with volume concentra- ed, which was attributed to the charge build up on the surface of
tion, respectively, while the effect of the volume flow rate on the alumina particles due to the controlled pH solution. The highly
pumping power, and the pressure drop is shown in Fig. 18 for the lam- charged formation around alumina particles and a valid dispersion
inar flow. These two parameters were calculated using Eqs. (11)–(14) of suspension was verified at pH 9.0.
and (Tables 3 and 4). b. Nanofluids containing small quantities of nanoparticles (below
Apparently, the friction factors of the nanofluids are nearly the same 0.3%) have substantially higher thermal conductivity than those of
to those of water under the comparable nanoparticle volume fraction. base fluids. The use of Al2O3 and TiO2 nanoparticles can significantly
Therefore, the effect of pumping power using nanofluids with a low improve the thermal conductivity of the solution, and the improve-
volume fraction is comparable to that of water [53]. No considerable ment rises with the growing particle concentration in this subject
accumulation to the pressure drop for the nanofluids is found on all area.
sequences of the investigation, which discloses that nanofluids will c. It has been found that the nanofluid viscosity strongly depends upon
not require an added disadvantage over the pumping power. It is the volume concentration and temperature as well as the base-fluids
witnessed that the friction factor relationship of the single-phase flow used. The hysteresis behavior was also observed for all the nano-
can be used for nanofluids. fluids.
d. Almost negligible effect in the pumping power and pressure drop is
4. Conclusions noticed for low concentration nanofluids. The zeta potential is an im-
portant basis for selecting the conditions of dispersing particles.
In this paper, we have experimentally investigated the preparation, There is a good correlation between the stability and the zeta poten-
thermal conductivity, viscosity and hysteresis phenomenon of water tial. The higher the value of the zeta potential is, the greater the
based Al2O3 & TiO2 nanofluids of low concentrations (0.05 to 0.3%v/v) stability of the solution is.
Fig. 15. Hysteresis observed for Al2O3/water for 13 nm, particle volume fractions of 0.1% and 0.3%, for fresh samples and samples after being used for a month in a flat plate solar collector.
94 Z. Said et al. / International Communications in Heat and Mass Transfer 58 (2014) 85–95
Table 3
Physical characteristic of metal oxides nanofluids and Water [9,42,43,54].
Table 4
Environmental and analytical conditions for the flat plate solar collector.
Fig. 16. Hysteresis observed for TiO2/water for ~21 nm, particle volume fractions of 0.1% Parameters of collector Value
and 0.3%.
Type Black paint flat plate
Glazing Single glass
Agent fluids Water, Al2O3 and TiO2 nanofluids
Absorption area, Ap 1.51 m2
Wind speed 2 m/s
Collector tilt, βo 20°
Apparent sun temperature, Ts 4350 K
Optical efficiency, o [44] 0.84
Glass thickness, t 4 mm
Insulation thermal conductivity, ki 0.06 W/m K
Inner diameter of pipes, d 0.01 m
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