International Communications in Heat and Mass Transfer 98 (2018) 31–40

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International Communications in Heat and Mass Transfer

journal homepage: www.elsevier.com/locate/ichmt

An experimental evaluation on thermophysical properties of functionalized T

graphene nanoplatelets ionanofluids
⁎
Jalal Alizadeh, Mostafa Keshavarz Moraveji
Department of Chemical Engineering, Amirkabir University of Technology (Tehran Polytechnic), Tehran 15875-4413, Iran

A R T I C LE I N FO A B S T R A C T

Keywords: Ionanofluids (ionic liquid-based nanofluids) as newly introduced types of nanofluids with promising potential for
Ionanofluids heat transfer and thermal storage applications are created through complex dispersion of ultrafine nanometer-
Ionic liquid-based nanofluids sized particles in ionic liquids. As innovative agents for development of energy sustainability, ionanofluids are
Graphene nanoplatelets widely employed in some applications, i.e., solar panels, catalysts, heat insulators and so forth. Non-flammability
Viscosity
and non-volatility features of ionic liquids, make them applicable as green working fluids for any chemical
Electrical conductivity
Surface tension
processes. In the present paper, an experimental investigation was conducted on some thermophysical properties
(viscosity, electrical conductivity and surface tension) of graphene based ionanofluid as main effective para-
meters in performance analysis. For this purpose, ionanofluid was prepared at three levels of weight fractions
(1%, 2% and 3%) by adding and dispersing polycarboxylate functionalized graphene nanoplatelets (GNPs) in
BMIM-PF6 (1-Butyl-3-methylimidazolium hexafluorophosphate) with 98 + % purity as the base fluid. The ex-
perimental data was acquired within the temperature range of 293.15 to 333.15 K and at atmospheric pressure
(~101 kPa). The results show that the viscosity of ionanofluid decreases with enhancement of temperature and
nanoparticle concentration. On the other hand, electrical conductivity of ionanofluid augments as temperature
and particle loading increase. For instance, EC at 1% wt. nanoparticles and 303.15 K enhances around 64%
compared to the pure IL. Surface tension of the ionanofluids was also determined experimentally as a function of
temperature for different mass loadings of nanoparticles. The results reveal that surface tension of ionanofluids
decreases slightly as temperature enhances and it reduces with enhancement of nanoparticle fraction as well.

1. Introduction
Introduction of nanofluids as a new generation of industrial working
fluids with superior capability of heat transfer augmentation goes back
to near two decades. Nanofluids are produced by adding and sus-
pending nanoscale (1–100 nm) metallic, metallic oxide, carbon or
composite particles in conventional fluids such as water, ethylene
glycol, mineral oils etc. Offering nanofluids for the first time in 1995,
Choi [1] could made an evolutionary change to heat exchange within
fluids. In fact, a new perspective was introduced on suspensions of solid
particles of nanometer dimensions in liquids. Due to the small size of
suspended particles, some problems in system i.e., corrosion, impurity
and pressure loss have been substantially diminished and stability of
suspensions against sedimentation has been improved as well [2].
Vast number of investigations have been carried out on the eva-
luation of nanofluids with water [3–10], ethylene glycol (EG) [11,12]
and oil [13,14] as base fluid experimentally and numerically. Since
water and ethylene glycol are more proper for use at low temperature
ranges and also oils possess relatively lower thermal stabilities and
higher vapor pressure compared to other frequently used working
fluids, it is needed to fabricate novel nanofluids with another types of
base fluid, i.e., ionic liquids, to be employed in wide range of thermal
conditions. Ionic liquids (electrolytes) are the center of attention in
materials research since the 21st century [15]. Indeed, they are mineral
salts with low melting point (below 100 °C) in the liquid state which can
be utilized in higher temperature ranges (up to about 200 °C). With
higher electrical conductivity (EC) and thermal stability as well as
lower vapor pressure compared to the common liquids, ILs can be al-
ternatively used in a wide variety of industrial applications where using
working fluids with limited thermophysical and chemical properties is
not a feasible option. As a green chemical solvent, they have an effec-
tual role in decrement of using hazardous substances to the environ-
ment. In spite of such interesting advantages, the number of in-
vestigations on the combination of ionic liquids and different
nanoparticles (ionanofluids) [16–18] is extremely lower than ordinary
nanofluids.

⁎
Corresponding author.
E-mail address: moraveji@aut.ac.ir (M. Keshavarz Moraveji).

https://doi.org/10.1016/j.icheatmasstransfer.2018.08.008

Available online 07 September 2018

0735-1933/ © 2018 Elsevier Ltd. All rights reserved.
J. Alizadeh, M. Keshavarz Moraveji
On the other hand, graphene nanoparticles as one of the most
promising candidate for thermal conductivity enhancement have at-
tracted tremendous interest among researchers, insofar as the number
of investigations on nanofluids containing graphene nano-additive
[19–24] has redoubled in the recent years. Also in order to make gra-
phene-based nanofluids more stable and soluble, some practical mea-
sures such as chemical functionalization of graphene nanoparticles and
using surfactants have been so far taken by investigators [25,26].
Performing an experimental study, Liu et al. [17] reported 22.9%
increment in thermal conductivity of HMIM-BF4 (1-Hexyl-3-methyli-
midazolium tetrafluoroborate) through dispersing 0.06% weight con-
centration of graphene nanoparticles at temperature ranging from 25 to
200 °C. They also observed that viscosity of the ionanofluid decreased
around 6.3 cP (0.0063 Pa.s) by enhancement of temperature up to
210 °C in comparison with the base liquid.
In another research, the colloidal stabilities of dispersions of sur-
face-functionalized and unmodified SiO2 nanoparticles in hydrophobic
and hydrophilic imidazolium-based ILs were investigated by Wittmar
et al. [27]. They observed that the unmodified hydrophilic nano-
particles are more compatible with the hydrophilic IL. Also they re-
ported that the colloidal stability of the dispersions in the hydrophobic
IL improves with the surface functionalization of SiO2 with hydro-
phobic groups.
Nanofluids are homogenous suspensions containing nanometer-
sized particles which possess great potential to enhance thermal con-
ductivity, viscosity, electrical conductivity and surface tension of base
liquids. These thermophysical properties play a significant role in im-
provement of heat exchange, pumping power effect and convective heat
transfer coefficients of fluids. With regard to the close relation between
viscosity, shear rate, pumping power and friction factor in a system, an
extensive survey on nanofluids thermophysical behavior has a parti-
cular significance. Numerous research papers have characterized ther-
mophysical properties of different nanofluids including graphene na-
noparticles and carbon nanotubes (CNTs) [28–31] while few
experimental studies have been concerned about those of graphene-
based ionanofluids. One of the common observations in the previous
investigations is changing the viscosity of fluid with increment of na-
noparticles loading as well as temperature.
In fluids with the suspension of nanoparticles, improvement of EC
could be attributed to the charge transfer kinetics enhancement which
is significantly affected by EDL (electrical double layer) effect in solu-
tion [32]. Particles size, nanoparticle concentration, and reference
electrolyte are some important factors affecting electrical conductivity
of suspensions directly. Electrical conductivity of fluids has diverse
industrial and technological usages such as electric-field formation in
colloidal dispersions, sensors, electrically conductive adhesive, etc. In
some original research studies, electrical conduction capability of me-
tals, metal oxides and CNTs has been carefully studied [32,33].
So far a few studies have been accomplished on the electrical con-
ductivity of graphene nanofluids compared to their thermal con-
ductivity [34–36] which all represent remarkable increase in electrical
conductivity of the base fluids with the addition and dispersion of
graphene nanoparticles to them.
In an experimental study, electrical conductivity of aqueous gra-
phene based nanofluid at various volume loadings of nanoparticles (%
vol.) and temperatures was measured by Baby and Ramaprabhu [34].
They reported an enhancement of about 1400% in electrical conduction
of the solution at 0.03% vol. and 25 °C.
Aravind and Ramaprabhu [37] in a research determined the elec-
trical conductivity of graphene nanosheets (GNs) nanofluids. According
to their comparative outcomes at room temperature, electrical con-
ductivity of GNs nanofluid with EG as base fluid enhances around 81
and 190% at 0.008 and 0.14% vol. respectively. Also this parameter
augments about 33% at 0.008% vol. and 55% at 0.14% vol. for the
solution with de-ionized (DI) water as the base fluid.
The interesting features of ILs as well as the significance of
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International Communications in Heat and Mass Transfer 98 (2018) 31–40
Table 1
Physical properties of the GNPs.
Nanoparticles Appearance Molecular Chemical
(color) weight (gr/ composition
mol.)
Polycarboxylate Faint grey to 12.01 Carbon, >
functionalized black 85% wt.
graphene Oxygen, > 3%
nanoplatelets wt.
examining thermophysical characteristics of working fluids for opti-
mized use in energy transport processes specifically thermal and elec-
trical energies, has acted as a keen motivator for the current research
authors to experimentally evaluate the consequence of dispersing
functionalized GNPs at three mass fraction levels (1, 2 and 3%) on
viscosity, electrical conductivity and surface tension of BMIM-PF6 as the
base liquid in the temperature range 293.15 to 333.15 K.
2. Preparation of ionanofluid
Despite inefficiency of the two-step method for preparation of well
dispersed nanofluids with high stability, due to some benefits such as
simplicity, quickness and low cost [38], it is becoming more and more
popular among scholars.
Polycarboxylate functionalized graphene nanoplatelets (GNPs) was
used to create the ionanofluids with BMIM-PF6 (98 + % purity) as the
base liquid at 1, 2 and 3% (by weight) nanoparticle loadings by the two-
step procedure. Both the nanoparticles and the ionic liquid were man-
ufactured by American chemicals company (Sigma-Aldrich). Some
physical properties of the GNPs have been presented in Table 1.
In order to obtain a morphological viewpoint, the X-ray diffraction
(XRD) pattern and SEM (scanning electron microscope) images of the
Polycarboxylate functionalized GNPs at two different magnifications
have been represented in Fig. 1(a), (b) and (c) respectively. Since the
ionanofluids should be more stable and well dispersed for a long period
without any agglomeration, sodium dodecyl sulfate (SDS) was used as a
surfactant to deduct the base liquid adhesion. For preferable dispersion,
after mixing GNPs, the IL and SDS together by a mechanical mixer, the
solution was homogenized in an ultrasonic probe sonicator (Hielscher-
UP200S) for around 90 min. A digital photograph of prepared ionano-
fluid (at 2% wt.) right after ultrasonically dispersion as well as the base
ionic liquid sample (BMIM-PF6) are illustrated in Fig. 2. According to
the observations, stability of the ionanofluid decreases as the nano-
particles fraction rises, so that the prepared ionanofluid at 3% loading
(by weight) was not sufficiently stable and showed the least resistance
against sedimentation compared to other concentrations.
3. Experimental measurements
3.1. Viscosity of ionanofluids
In general, viscosity is defined as a measure of the resistance to flow
of a fluid. Viscosity of the ionanofluids at 1, 2 and 3% wt. was measured
right after preparation by a programmable viscometer (Brookfield-DV-
II + Pro, Fig. 3) with ± 1% accuracy and ± 0.2% repeatability which
was properly connected to a computer for recording the data. For
controlling the temperature or keeping it fixed during the tests, a
temperature control water bath was used. To sense and read the tem-
peratures during the trials PT100 type sensors with ± 0.1 K precision
and a digital k-type thermometer were utilized in the system. To
minimize possible errors and obtain reliable results, prior to the ex-
periments, the viscometer was intently checked and calibrated on the
basis of test results for the standard fluid of known viscosity within a
specified temperature range and accordingly the maximum deviation
of < 0.9% was detected. Under steady-state conditions, the data was
J. Alizadeh, M. Keshavarz Moraveji
Fig. 1. XRD patterns (a) and SEM images of the GNPs at X3000 (b) and X8000 (c) magnifications.
Fig. 2. Sample of pure BMIM-PF6 (left) and prepared ionanofluid at 2% wt.
(right).
acquired three times for each sample at the temperature range from
293.15 to 333.15 K, and then mean values were taken.
3.2. Electrical conductivity of ionanofluids
Electrical conductivity or specific conductance evaluates capability
of a material to direct an electric charge flow. Electrical conduction in
ILs (electrolytes) is done through ions traveling tremendously affected
by concentration. In the present study, electrical conductivity mea-
surements of GNPs/BMIM-PF6 ionanofluid were performed as a func-
tion of both temperature and particles loading. For this purpose, elec-
trical conductivity of prepared ionanofluids was measured at varied
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International Communications in Heat and Mass Transfer 98 (2018) 31–40
Fig. 3. A photograph of the viscometer (Brookfield-DV-II + Pro).
fractions (1–3% wt.) and temperatures (293.15–333.15 K) separately
using a portable conductivity meter (WTW-Cond 3110) with ± 1%
precision and conductivity measuring cells with graphite electrodes
(WTW-TetraCon 325) as well. An image of the conductivity measure-
ment set is represented in Fig. 4. It should be noted that the measuring
range of the conductivity meter has been specified between 0.1 μs/cm
to 200 ms/cm in the SI by its manufacturer. At this stage, a bath water
was employed to arbitrarily adjust temperature of the samples and an
average value was picked as experimental data after three times test
repetition for each case. Also for calibration of the conductivity meter,
the former procedure (standard fluid) was applied.
J. Alizadeh, M. Keshavarz Moraveji
Fig. 4. Picture of the conductivity measurement set.
Stability as homogenous dispersion of suspended solid particles in
base liquids is one of the essential factors for efficient utilization of
ionanofluids (or universally nanofluids) in industrial processes. In ad-
dition to some prevalent methods of checking nanofluids durability,
i.e., visual inspection, zeta potential and spectral absorbency, mea-
surement of electrical conductivity could also be used as a practical
technique. Due to the EDL (electrical double layer) effect in nanofluids,
nanoparticles act as charge carriers in the solution. Therefore, the
number of charge carriers increases as nanoparticles loading enhances
which will lead to significant augmentation of electrical conductivity.
By reduction of nanofluids stability (nanoparticles sedimentation), the
loading of charge carriers (nanoparticles) and as a consequence elec-
trical conduction will lessen. So the durability of nanofluids can be
evaluated from the values of electrical conductivity measured at dif-
ferent times [32].
3.3. Surface tension of ionanofluids
Surface tension which is described scientifically as elastic tendency
of a liquid surface causing it get the least possible surface area, is ori-
ginated from the cohesive forces betwixt fluid molecules. There are
several differing techniques to determine the surface or interfacial
tension of fluids which most of them are applicable to ionic liquids.
However, some methods such as Du Noüy ring (DNR), pendant drop
(PD) and capillary rise (CR) are common for surface tension measure-
ment of ionic liquids. As an advantage, in comparison with the mostly
used technique, i.e., DNR, a very small fluid sample (about 20–60 μL) is
needed in the PD method, hence a pendant drop tensiometer has been
selected for the present research. In such instruments, surface tension
measurement is carried out through using curvature of the sample drop
profile.
Ionanofluids surface tension was measured for each % amount of
dispersed particles at 293.15, 313.15 and 333.15 K by a high-resolution
force tensiometer (see Fig. 5) manufactured by Krüss Company (K100).
Thanks to the internal sensor, this device is capable of controlling and
measuring sample temperature. According to its technical data sheet,
the tensiometer has temperature measurement range of −60 to 450 °C
with 0.01 °C resolution and ± 0.5 °C accuracy.
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International Communications in Heat and Mass Transfer 98 (2018) 31–40
Fig. 5. A photograph of the Tensiometer during measurement of surface ten-
sion.
4. Results and discussion
4.1. Viscosity
Viscosity of Ionanofluids was measured as function of functionalized
GNPs weight fraction and ionanofluid temperature. In the trials, mass
loading levels of GNPs were at 0% (Pure ionic liquid), 1%, 2% and 3%
and also ionanofluid temperature varied between 293.15 and 333.15 K.
As shown in Fig. 6, viscosity of the ionanofluids and the base fluid re-
duces as temperature increases. Unlike the majority of previous reports
based on increment in viscosity of base fluid through nanoparticles
dispersion as an additive, in the present work a totally opposite result
was observed which is in agreement with data reported in some re-
search papers [39,40]. These decrements in viscosity may occur due to
the self-lubricating nature of carbonous materials, i.e., graphene,
carbon nanotubes (CNTs), graphite, and so on. Relatively lower visc-
osity can result in lowering the pressure drop penalty in thermo-fluids
systems and maximizing the hydraulic and energy efficiency as a con-
sequence. The measured viscosities for pure IL (BMIM-PF6) were com-
pared to those determined by Harris and Woolf [41] and Tomida et al.
[42] in the following ranges (see Table 2):
According to Fig. 6, viscosities of the pure IL are in better agreement
with those reported by Harris and Woolf [41] compared to Tomida
et al. [42]. Fig. 7 clearly illustrates that at 293.15 K viscosity of iona-
nofluids containing 1, 2 and 3% wt. GNPs is around 20%, 27% and 43%
lower than that of pure IL, respectively. It also indicates that at a spe-
cific weight loading of nanoparticles, the relative viscosity increases
with enhancement of temperature.
Fig. 8 shows the minimum and maximum errors of roughly 0.3%
and 6% between viscosities of BMIM-PF6 determined by the current
measurements and Harris and Woolf [41] at different temperatures.
These low-level deviances obviously connote to the accuracy of the
experimentally determined data.
J. Alizadeh, M. Keshavarz Moraveji International Communications in Heat and Mass Transfer 98 (2018) 31–40

Fig. 6. Comparison between viscosity of the graphene-based ionanofluid at different weight fractions.

Table 2 line chart provided (see Fig. 9), reveals that the electric conduction
Temperature and pressure range for viscosity measurement of BMIM-PF6 in capability of ionanofluid improves as temperature rises and at a specific
some research studies. temperature, the electrical conductivity of ionanofluid enhances with
Researcher Temperature range (K) Pressure range (MPa) enhancement of nanoparticles concentration. Fig. 9 also depicts the
experimental data for electrical conductivity of pure BMIM-PF6 de-
This study 293.15–333.15 0.1 termined by some papers available in the literature [43–45].
Harris and Woolf [44] 273.15–353.15 0.1 to 249.3
Regarding Fig. 10, the maximum improvement in electrical con-
Tomida et al. [45] 293.15–353.15 0.1 to 20
ductivity of ionanofluid for all three GNPs loadings is acquired at the
lowest temperature (293.15 K) and is reported about 71, 197 and 445%
4.2. Electrical conductivity at 1, 2 and 3% wt., respectively. Thus, it can be concluded that using
the GNPs as electrical conductivity enhancer in the IL (BMIM-PF6) is
Fig. 9 illustrates the electrical conductivity versus temperature of certainly more efficacious within lower temperatures. As previously
ionanofluid at different mass loadings of nanoparticles. A glance at the mentioned, the augmentation in electrical conductivity of the

Fig. 7. Variation of relative viscosity as a function of nanoparticles fraction (by weight) at various temperatures.

35
J. Alizadeh, M. Keshavarz Moraveji International Communications in Heat and Mass Transfer 98 (2018) 31–40

Fig. 8. Comparison between the experimental results for viscosity of pure IL and those reported by Harris and Woolf [41].

ionanofluids in comparison with the pure IL is indeed related to the EDL
interactions which are formed around each nanoparticle.
In Fig. 11, the deflection between electrical conductivity of pure
BMIM-PF6 at various temperatures (293.15–333.15 K) acquired through
the present experiments and that reported by some investigators
[42,43] is represented. It is clearly observed that the data from this
study agrees more to the data reported by Tokuda et al. [44] with
maximum deviation of about 18% rather than Yu et al. [45] with that of
around 47%. Although both studies [44,45] determine the electrical
conductivity of pure IL with almost the same deviances from the current
experimental results at 293.15 K, Tokuda et al. [44] reports far closer
results in the temperature range 303.15 to 323.15 K. For electrical
conductivity of the pure IL at the highest temperature (333.15 K), the
data from Ref. [48] shows a lower inconsistency with the current results

Fig. 9. Comparison between electrical conductivity of the graphene-based ionanofluid at various mass loadings.

36
J. Alizadeh, M. Keshavarz Moraveji International Communications in Heat and Mass Transfer 98 (2018) 31–40

Fig. 10. Variation of relative EC as a function of nanoparticles mass loading at different temperatures.

(~14%) compared with the data of Tokuda et al. [44].
4.3. Surface tension
Surface tension of the ionanofluids was determined experimentally
as a function of temperature and nanoparticle mass loading. As can be
observed in Fig. 12, the surface tension of ionanofluids decreases
slightly with temperature enhancement. Moreover, the surface tension
of ionanofluids reduces as nanoparticles weight fraction rises. It is ea-
sily comprehended that surface tension of the ionanofluid is strongly
affected by nanoparticles loading compared to temperature. Fig. 12 also
represents experimental data for surface tension of pure BMIM-PF6
reported in some previous works [46–48]. Comparing the experimental
data for pure IL, it is obviously seen that the results from the current
study are in a better consistency with the data reported by Pereiro et al.
[48] than others.
Fig. 13 illustrates variation of relative surface tension as a function
of nanoparticles mass loading at different temperatures. According to
Fig. 13, for each weight fraction, the maximum and minimum reduction
in surface tension of the ionanofluid is recorded at the highest and the
lowest temperature, respectively. For instance, at 3% wt., the maximum
and the minimum decrement in ST is specified around 29.8 and 22.9%,

Fig. 11. Comparison between the experimental results for electrical conductivity of pure IL and those reported by Tokuda et al. [44] and Yu et al. [45].

37
J. Alizadeh, M. Keshavarz Moraveji International Communications in Heat and Mass Transfer 98 (2018) 31–40

Fig. 12. Comparison between surface tension of the graphene-based ionanofluid at different weight fractions.

respectively. Regarding the conflicting deductions presented so far, it is
not obvious whether the surface tension enhances or diminishes
through adding and suspending nanoparticles and also what mechan-
isms could be certainly responsible for such behavior [49]. However,
the current decrements in surface tension of pure IL through adding
nanoparticles at various fractions may be corresponded to the hydro-
phobic character of graphene nanoplatelets which causes them to be
adsorbed at the liquid–air interface [50].
To get assured of the present experimental results, surface tensions
of the pure BMIM-PF6 were compared with those obtained from Refs.
[47, 48]. Fig. 14 clearly demonstrates that the measured surface
tensions of the pure IL match well with those previously reported by
Pereiro et al. [48]. Accordingly, the maximum deflection between the
results from Pereiro et al. [48] and this study does not exceed 2.5%.
5. Conclusions
Conducting the present experimental study on viscosity, electrical
conductivity and surface tension of BMIM-PF6 with functionalized
graphene nanoplatelets inclusion at weight fractions ranging from 1 to
3%, the following results are reported:

Fig. 13. Variation of relative surface tension as a function of nanoparticles mass loading at various temperatures.

38
J. Alizadeh, M. Keshavarz Moraveji
Fig. 14. Comparison between the experimental data for surface tension of pure IL and those reported by Freire et al. [47] and Pereiro et al. [48].
- In agreement with some previous works [42,43], viscosity of base
liquid reduced with addition and suspension of graphene nanopla-
telets which can be attributed to the self-lubricating nature of car-
bonous materials.
- Measuring electrical conductivity of the ionanofluid as a function of
temperature for various mass loadings of nanoparticles, it can be
concluded that the electric conduction capability of ionanofluid
improves as temperature rises and at a particular temperature, the
electrical conductivity of ionanofluid augments with increment of
nanoparticles fraction. Also it was observed that using the GNPs as
electrical conductivity enhancer in the IL (BMIM-PF6) are certainly
more effective within lower temperature ranges. The augmentations
in electrical conductivity of the ionanofluids at higher mass fractions
could be corresponded to the EDL interactions which are formed
around each nanoparticle.
- With regard to the results, surface tension of ionanofluids decreased
slightly with raising temperature. It was also seen that the surface
tension of ionanofluids reduced as nanoparticles weight loading
rose.
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