Energy Conversion and Management 196 (2019) 1222–1256

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Energy Conversion and Management

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

Graphene family nanofluids: A critical review and future research directions T

⁎
Mehdi Bahiraei , Saeed Heshmatian
Department of Mechanical Engineering, Kermanshah University of Technology, Kermanshah, Iran

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

Keywords: Graphene family nanomaterials including single-layer graphene, multi-layer graphene, graphene quantum dots,
Graphene family nanofluids graphene nanoplatelets, graphene oxide, and so forth demonstrate many excellent characteristics along with
Preparation techniques great thermal conductivity. Consequently, they are appropriate candidates for utilization in nanofluids and have
Convective heat transfer recently received major attention in this area. Although many studies have been performed on graphene-based
Hydrodynamic attributes
nanofluids, there is no thorough review article in which effective mechanisms on revealing enhancements and
Applications
Future directions
failures of graphene nanofluids are surveyed. Concerning various progress and problems existing in the field of
graphene nanofluids, performing a complete review in this context is highly required, and there are still a lot of
challenges that should be evaluated. In this review paper, the capabilities of graphene-based nanofluids are
examined, and new developments on preparation techniques, stability improvement, and types of surfactants
utilized are reviewed. Thermophysical properties, convective heat transfer, boiling, hydrodynamic attributes,
and second law characteristics of graphene-family nanofluids are also investigated. Moreover, approaches such
as molecular dynamics and artificial intelligence used in this field are reported and discussed. In addition,
applications including use of graphene-based nanofluids in car radiators, heat exchangers, solar thermal, heat
pipes, electronics cooling, and energy storage are presented. This in-depth review also identifies available
challenges and recommends several directions for future research in this field. Finally, it is concluded that
graphene family materials can improve the characteristics of base fluids considerably.

1. Introduction
Nanofluids have been introduced as a new fascinating kind of heat
transfer fluids, which are prepared with dispersing solid nanoparticles
in conventional liquids. In comparison with ordinary fluids, they have
superior thermal attributes for utilization in different heat transfer
applications. As a result, these suspensions have been investigated by
many scholars [1–8]. An overview of the relevant literature shows that
the number of papers published in this area has significantly increased
from a few articles before the year 2000 to many hundreds in the recent
decade.
Due to the unique characteristics of nanofluids, several review ar-
ticles have been written on the studies carried out in this field. These
review articles include various topics related to nanofluids such as heat
exchangers [9], thermophysical properties [10], modeling and simu-
lation [11], electronics cooling [12], artificial intelligence [13], particle
migration [14], mixed convection [15], phase change materials [16],
solar thermal [17], and so forth. In these review papers, nanofluids
have been proposed as excellent candidates in diverse thermal appli-
cations.
Thermal conductivities of carbon materials have a wide range,
which spans from ∼0.2 W/mK for diamond-like carbons to ∼5000 W/
mK for graphene. Accordingly, carbon materials can be employed as
both heat insulators (like some of the diamond-like carbons and
amorphous carbons) and the heat superconductors such as graphene.
Since discovering graphene by Novoselov et al. in 2004 [18], this ma-
terial – that consists of a single layer of carbon in a 2D lattice – has
found many interesting applications. Graphene has many excellent
chemical, physical, and mechanical features. In recent years, there has
been an increasing number of papers presenting the research progress
on graphene and graphene-based materials where the benefits of these
materials are employed in different situations. Particularly, the number
of research studies related to graphene has increased quickly in the past
five years, and it is expected that such statistics will increase in the
upcoming years as well. Consequently, many scholars have recently
reviewed the topic of graphene materials from various aspects such as
water treatment [19], energy storage [20], anti-corrosive coatings [21],
solar photovoltaic applications [22], rechargeable batteries [23], high-
voltage supercapacitors [24], fuel cells [25], and printing techniques
[26].
The publications such as the review articles above give appropriate
insights into the research on graphene materials, challenges prevailing

⁎
Corresponding author.
E-mail address: bahira@iust.ac.ir (M. Bahiraei).

https://doi.org/10.1016/j.enconman.2019.06.076
Received 9 March 2019; Received in revised form 26 June 2019; Accepted 27 June 2019
Available online 02 July 2019
0196-8904/ © 2019 Elsevier Ltd. All rights reserved.
M. Bahiraei and S. Heshmatian
on the research and the requirement of more elaborate experimental
and numerical studies to understand the science behind the observed
phenomena. However, although many studies have been carried out on
liquids containing graphene nanomaterials (i.e., graphene-based na-
nofluids), there is not any thorough review article in which effective
mechanisms on revealing enhancements and failures of graphene na-
nofluids are surveyed.
Concerning various progress and problems existing in the field of
graphene nanofluids, performing a complete review in this context is
highly required. Stability of these nanofluids is an important challenge
in determining their applicability. Scholars have made significant ef-
forts to reach stable graphene nanofluids, while there are still several
problems in this regard, which will be discussed in the present article.
Indeed, the stability issue is one of the causes for the noticeable in-
crement in the number of research investigations to functionalize gra-
phene including reactions of graphene materials with organic or in-
organic molecules, chemical modifying the surface of graphene, and
different analyses of covalent and non-covalent interactions with gra-
phene. Additionally, many contradictions, which are seen in the pub-
lished papers on graphene nanofluids, make this review survey irre-
vocable. Regarding the fact that the nature of graphene nanomaterials
is different from other nanoparticles, it is necessary to understand the
reasons resulting in thermal behaviors and hydrodynamic features of
graphene-family nanofluids. In addition, the existence of structural
defects, restacking, and multilayer thickness can influence the features
and great surface area of graphene materials, which should be dis-
cussed. A graphene sheet is also prone to get folded, coiled, and cor-
rugated at the surface and edges, and although these factors can pro-
foundly affect energy transmit mechanisms, little attention has been
paid to this subject in the literature. Moreover, it is known that dec-
orating metal or metal oxide nanoparticles on graphene sheets avoids
graphene agglomeration and eliminates the requirement of surfactants
for stabilizing graphene nanomaterials in base liquids, while the ben-
efits and challenges of such an important issue should be regarded in an
effective review study, however, the relevant literature lacks such
survey.
It should be noted that the graphene-family is not limited to single-
layer graphene, and has various types and derivatives. Different types of
graphene-based materials have been employed for preparing nano-
fluids, and have demonstrated superb attributes in this field. Therefore,
graphene family nanofluids can be promising options for next-genera-
tion heat transfer liquids.
This article attempts to review the studies performed on graphene-
based nanofluids from the atomic level to macroscopic view. The paper
starts by firstly discussing the different types of graphene materials used
in this area. The synthesis techniques are subsequently discussed, fol-
lowed by stability, wettability, thermophysical properties, convective
heat transfer, boiling, hydrodynamic features, molecular dynamics si-
mulation, and second law analysis. Finally, the uses of artificial in-
telligence in this area as well as applications of graphene-based nano-
fluids in different industrial sectors are introduced. Furthermore,
challenges and problems of this field are explored and discussed
throughout the paper, and several directions and opportunities are in-
troduced for future studies.
2. Different graphene-based materials used in nanofluids
The unique features of graphene emanate from the 2p orbitals that
develop the π-bonds. The π-bonds are then hybridized together to
create the π–π bands that are delocalized over the platelet of carbon
and form graphene. Accordingly, graphene possesses a superb stiffness
with high thermal conductivity, zero effective mass, great mobility of
charge carriers, impermeable to gases, and optically transparent.
Graphene-based materials have received noticeable attentions due to
their excellent properties such as small weight, appropriate mechanical
strength as well as unique conductivity of electricity and heat.
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Energy Conversion and Management 196 (2019) 1222–1256
Numerous experiments on thin films have shown that below a specific
thickness, typically of dozens of atomic layers, the films become ther-
modynamically unstable unless they constitute an inherent part of a 3D
system (such as being grown on top of a bulk crystal with a matching
lattice) [27,28]. However, a comprehensive analysis of 2D crystal
problem beyond harmonic approximation leads to the finding [29,30]
that the interaction between bending and stretching long-wavelength
phonons stabilizes atomically thin membranes through their deforma-
tion in the third dimension [30]. It has been shown that freely sus-
pended graphene crystals can appear without a substrate, and indicate
random elastic deformations involving all three dimensions [31].
Although there are several types of graphene-based materials, many
authors use the word “graphene” for the definition of their considered
material. Materials are termed as “graphene” by many authors even
when these materials possess hundreds of layers. Indeed, some of the
names employed by scholars for graphene-based materials are irra-
tional and, even contradictory. In the relevant literature, the single-
word name “graphene” is now being utilized for many various graphene
materials, and this unplanned over employment can lead to the pro-
blems for the readers, such that they may miss significant scientific
differences. Owing to the significant impotence of this issue, the in-
ternational editorial team of the Carbon journal [32] made an initial
effort for recommending rational names for different graphene mate-
rials. Homogenization of the names in the literature significantly helps
the readers and researchers in the simple understanding of material
kinds as well as the faster development of science in this area. As a
result, before performing a detailed review of different graphene-based
materials used in nanofluids, we introduce the correct names employed
in the literature for the graphene family materials along with their
accurate definitions:
Graphene – a single-atom-thick sheet of hexagonally arranged sp2-
bonded carbon atoms. It should be noted that graphene is freely sus-
pended or attached on another substrate, and is not an integral part of a
carbon material. The transverse sizes of graphene can be from several
nanometers to the macroscale. It is noteworthy that other members of
graphene-family cannot be termed “graphene,” and must be called with
the aid of a dedicated multi-word name for distinguishing them from
the monolayer 2D carbon (i.e., graphene).
Multi-layer graphene (MLG) – a 2D carbon material including a low
number (between 2 and about 10) of countable, well-defined, stacked
graphene layers of extended transverse size.
Graphene quantum dots (GQD) – few-layer graphene nanosheets that
are employed chiefly in situations in which photoluminescence is the
desired feature. In general, GQDs possess very small transverse sizes
(smaller than 10 nm).
Graphene nanoplatelets (GNP) – 2D honey comb lattice graphene
with 10–30 graphene layers [33]. The transverse sizes of this graphene
material can be from several nanometers to macroscale.
Graphene oxide (GO) – chemically modified graphene that is syn-
thesized through exfoliation and oxidation along with extensive oxi-
dative modification of the basal plane. Graphene oxide demonstrates a
monolayer material having a great oxygen content.
Reduced graphene oxide (rGO) – graphene oxide that is processed via
thermal, chemical, microwave, photo-thermal, photo-chemical, or mi-
crobial/bacterial approaches for reducing its oxygen content.
Fig. 1 shows the main kinds of graphene materials that have been
utilized to produce nanofluids for diverse applications. According to the
figure, the structure of pristine graphene is regarded as a 2D array in
which sp2-hybridization of carbon atoms are arranged in a hexagonal
lattice via covalent bonds. Furthermore, the functionalized graphene
sheets are synthesized by preparation; the carbon core structure can be
oxidized deriving GO, the reduced structure having vacancy defects is
rGO, and structures with sizes of a few nanometers having quantum
phenomena are GQDs [34].
In the following, different graphene materials used in preparing
nanofluids are reviewed. It can be mentioned that the classification of
M. Bahiraei and S. Heshmatian Energy Conversion and Management 196 (2019) 1222–1256

Fig. 1. Structure of graphene-based materials: (a) pristine graphene having sp2-hybridized carbon atoms, and the chemically modified graphene including (b)
graphene oxide, (c) reduced graphene oxide, and (d) graphene quantum dot [35].

graphene materials can also be performed based on important features low synthesis cost. GQDs demonstrate important benefits like proper
such as carbon/oxygen ratio and the number of graphene layers. In the surface grafting features, minor cytotoxicity, unique solubility [44],
graphene materials, the number of layers has noticeable influences on tunable band gap, great surface area, good chemical inertness, quantum
the characteristics of these materials. Graphene sheets are characterized confinement and edge impacts [45]. Hence, graphene quantum dots
by different analytical techniques. Transmission electron microscopy have widely been employed in various areas. For example, Li et al. [46]
(TEM), scanning electron microscopy (SEM), atomic force microscopy reviewed the new developments in GQD-based optoelectronics and
(AFM), and ultraviolet visible absorption spectroscopy are beneficial to energy equipment and indicated the excellent potential of GQDs for the
identify the number of layers while these methods are time-consuming progress of energy functional systems and communication components.
and need specific sample preparation. In addition, after the year 2006, Also, Zhang et al. [47] considered the successes achieved in energy and
Raman spectroscopy is also regarded to be an easy and powerful charge transfer devices like light-emitting diodes and fuel cells utilizing
technique to determine the number of graphene layers [36]. GQDs. Zhu et al. [48] adopted GQDs as low toxicity and biocompatible
material for use in bioimaging. Moreover, Chen et al. [49] examined the
promising potential of GQDs in sensors.
2.1. Graphene quantum dots
In addition to the above applications, GQDs have also been im-
plemented as an additive for preparing nanofluids to improve attributes
As mentioned, graphene quantum dots are few-layer graphene na-
of these suspensions. Ettefaghi et al. [50] utilized the biocompatible
nosheets having very small transverse sizes (smaller than 10 nm). The
GODs to produce nanofluids. They prepared GQDs through a “bottom-
GQDs can be made up of a single atom of graphite layer or graphene cut
up” approach, such that the graphene quantum dots were synthesized
into tiny fragments. The disk property of GQDs is very small, similar to
using a hydrothermal technique with the aid of urea and citric acid.
a dot [37]. After stimulus via electrical energy or UV light, the excitons
5.2% and 17% improvements were obtained respectively for the
would be confined to the quantized energy levels and release photo-
thermal conductivity and convective heat transfer coefficient at
luminescent light under a limited band. It should be noted that the main
100 ppm concentration in comparison with the base fluid.
precursors are not only the infinite graphene plate and the functiona-
Goharshadi et al. [51] measured the viscosity, electrical con-
lized graphene, but some organic materials are also usable.
ductivity, and thermal conductivity of the nanofluids containing GQDs
Different approaches have been adopted to produce GQDs, which
in glycerol and pure water. The GQDs were synthesized by one-step
can be categorized into two chief classes, namely “top-down” and
green pyrolysis of citric acid. A 49.97% reduction in the glycerol visc-
“bottom-up” techniques. In the “top-down” approach, graphene dots
osity was observed by adding 2% GQDs at a shear rate of 0.66 s−1 and
are prepared by cutting carbonaceous materials through electro-
temperature of 20 °C. Moreover, the thermal conductivity of the water
chemical or chemical oxidation, hydrothermal treatment, microwave
enhanced almost 9% as the GQDs were added at a temperature of 298 K
process, and electron beam [38]. For instance, Lin and Zhang [39]
and a concentration of 2%. Besides, the electrical conductivity of the
employed an efficient technique on the basis of intercalation and ex-
water increased with the addition of the GQDs.
foliation of graphite and carbon nanotubes to synthesize GQDs through
Amiri et al. [52] investigated the thermophysical properties and
“top-down” method. Besides, Shinde and Pillai [40] produced GQDs
colloidal stability of water-based GQD nanofluids. Amine-treated GQDs
from multiwall carbon nanotubes using electrochemical approach.
(A-GQDs) were prepared through a new technique. No sedimentation
However, very low reaction yields and rather expensive starting ma-
was perceived during 30 days. It was also revealed that the ascending
terials are the most important limitations of the “top-down” approach
rate of the viscosity and density is not significant with adding the A-
[41]. On the other hand, graphene quantum dots are produced from
GODs to the water.
organic compounds in the “bottom-up” approach [42]. In large scales,
In another study, Amiri et al. [53] synthesized graphene quantum
the “bottom-up” approaches are appropriate routes to synthesize
dots with the aid of a cost-effective exfoliation method for dispersing in
fluorescent quantum dots [38]. It can be mentioned that for the top-
transformer oil. The transformer oil-based nanofluid demonstrated
down approaches, the hydrothermal cutting prepares many nano-sized
considerably greater positive voltage breakdown, convective heat
platelets, whereas the bottom-up techniques employ direct pyrolysis
transfer, thermal conductivity as well as higher flash point levels in
and carbonization of the organic precursors.
comparison with the pure transformer oil.
Various kinds of GQDs have attracted interest owing to their unique
optical properties in the presence of photoluminescence involving the
specific binding ability to a varied domain of biomolecules. Moreover, 2.2. Graphene nanoplatelets
they have presently found growing attention in an extensive range of
biological applications [43] owing to their excellent characteristics and Graphene nanoplatelets are multi-layer particles including 10–30

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M. Bahiraei and S. Heshmatian
graphene sheets with much retention of graphene (i.e., monolayer
sheet) properties [54,55]. Employing GNPs is desired because they are
cheaper, and their synthesis is easier compared with graphene or
carbon nanotubes (CNT) [56]. One of the important problems in syn-
thesizing composites and suspensions is the uniform dispersion and
effective utilization of the secondary phase. Dispersion of graphene
nanoplatelets is easier than both graphene and carbon nanotubes be-
cause during dispersion, single layer graphene (i.e., graphene) may be
curled, and CNTs may be entangled. GNPs possess a rather lower sur-
face area in comparison with graphene; however, their surface area is
still much greater than that of CNTs. It can be mentioned that the
thermal conductivity of GNPs decreases by increasing the number of
layers [57].
Due to the unique characteristics of GNPs, several researchers have
utilized them for preparing nanofluids. Hussien et al. [58] evaluated
thermophysical properties, pressure drop, and heat transfer coefficient
of a hybrid nanofluid containing GNPs and multi-walled carbon nano-
tubes (MWCNTs) through a circular pipe. Heat transfer coefficient in-
creased considerably with employing this hybrid nanofluid. Moreover,
an 11% increment in pressure loss was seen in the case of applying the
nanofluid.
Sharma et al. [59] studied the influence of alumina–GNP hybrid
nanoparticles on tribological features of a lubricant as cutting fluid. The
wear and friction coefficient reduced with increasing the nanoparticle
concentration. Meanwhile, this prepared hybrid nano-lubricant con-
siderably decreased the nodal temperature and tool flank wear by
5.79% and 12.29%, respectively, in comparison with alumina-based
lubricant.
Amiri et al. [60] dispersed GNPs in aqueous media through covalent
and non-covalent functionalization. It was observed that the thermo-
physical and rheological properties of the treated samples were no-
ticeably higher than those of the pure water. Besides, the results in-
dicated that the thermal conductivity changes considerably depending
on the functionalization method.
Safaei et al. [61] assessed the heat transfer rate, pressure drop,
friction loss, and pumping power for utilizing a water-based nanofluid
containing GNPs–silver nanoparticles within a rectangular conduit. It
was shown that the heat transfer attributes enhance by increasing the
concentration and Reynolds number. However, an increment of the
pumping power was also observed in the case of using the nanofluid.
Yarmand et al. [33] prepared a GNP–Ag/water nanofluid and stu-
died its thermophysical properties, heat transfer performance, and
friction coefficient for flow within a circular pipe. The GNP–Ag nano-
composite was synthesized via a facile chemical process, which in-
cluded acid treatment to functionalize the GNPs. The experimental data
showed that the thermal conductivity and heat transfer rate of the
nanofluid enhance compared with the base fluid.
Yarmand et al. [62] investigated the attributes of GNP–Pt/water
nanofluids. The prepared nanofluids were stable, and any noticeable
sedimentation was not seen during a long period (22 days). Thermal
conductivity of the nanofluid demonstrated a 17.77% enhancement at a
temperature of 40 °C and a concentration of 0.1%.
2.3. Graphene oxide
Because synthetizing graphene is expensive and rather intricate,
many efforts have been made to reach appropriate cost-effective
methods to develop and utilize graphene derivatives and other asso-
ciated materials. Graphene oxide, which is a single-atomic layered
carbon-based material and is obtained through exfoliating graphite
oxide into layered plates via sonicating or mechanical stirring, is one of
these materials. Graphene oxide, as a 2D material, demonstrates an
oxidized form of graphene including carbon/oxygen atomic ratio of
2:0–2:9. GO has a greater and more disordered chemical structure layer
in comparison with graphene with the domain of 0:6–1:1 nm, which is
dependent on its synthesis approach. It is known that graphene is
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Energy Conversion and Management 196 (2019) 1222–1256
hydrophobic, while the existence of O functional groups makes GO
hydrophilic for dispersion in aqueous media. It should be noted that in
typical graphene oxide, the number of carbon atoms bonded to oxygen
atoms is more than the number of intact sp2–hybridized carbon atoms,
which modifies properties of GO from pristine graphene.
Graphene oxide is easy to process because it is dispersible in water,
and can even be employed for reaching graphene. The exfoliated GO
plates can be simply suspended in an aqueous solvent without using
amphiphilic stabilizers. It should also be noted that graphene oxide
demonstrates a heterogeneous chemical structure, and the coverage of
oxygen groups alters with respect to the degree of oxidation in synthesis
processes. In recent years, GO has attracted growing interests owing to
its excellent attributes such as mechanical stability, great surface area
as well as controllable optical and electrical features. In the field of
nanoparticle suspensions, several researchers have also used GO for
preparing nanofluids. Vincely and Natarajan [63] performed the ex-
periments on a solar flat plate collector using graphene oxide nanofluid
as the working fluid. The nanofluid was synthesized via ultrasonication
of the GO in the pure water. The enhancement of the collector efficacy
was 7.3% at a flow rate of 0.0167 kg/s and concentration of 0.02 re-
lative to the pure water.
Azimi et al. [64] evaluated the heat transfer of unsteady flow of
nanofluid containing GO between two moving parallel plates by
homotopy asymptotic approach. Comparing their solution with a valid
method, they proved cogency of the approach. It was also revealed that
the heat transfer rate increases with altering the nanoparticle con-
centration at invariant Eckert number.
Fu et al. [65] synthesized graphene oxide sheets, and gold nano-
particles for generating solar steam. The color and morphology of the
GO–gold nanofluids changed with the time under sunlight, and it was
concluded that the graphene oxide sheets were reduced to graphene
plates. This process of photo thermal deoxygenation of GO presents an
efficient approach to prepare graphene sheets with no reductions. The
process of gold nanoparticles improved solar steam production em-
ployed in this study is illustrated in Fig. 2.
Hussanan et al. [66] examined the natural convection of nanofluids
on a vertical surface. They used five kinds of oxide nanoparticles in-
cluding alumina, titania, copper oxide, iron oxide, and graphene oxide
dispersed in three different base fluids. The results showed that the
temperature of the graphene oxide nanofluid was greater than that of
the other nanofluids.
Ranjbarzadeh et al. [67] developed an isotherm heat transfer system
for studying the influence of water-graphene oxide nanofluid on friction
factor and heat transfer in a circular pipe. Employing the nanofluid
resulted in a 40.3% increment in the convective heat transfer coeffi-
cient. A small increase also occurred for the friction factor in the case of
using the nanofluid.
Fig. 2. Schematic of gold nanoparticles improved solar steam production: (1)
Irradiation, (2) absorption, (3) phase transition, (4) coalescence of nanobubbles
[65]. Reprinted with permission from Elsevier.
M. Bahiraei and S. Heshmatian
Fig. 3. The production process of controlled reduced graphene oxide (CRGO) [75]. Reprinted with permission from Elsevier.
Rose et al. [68] introduced a numerical wave optics model for si-
mulating the absorption of nanoparticles dispersed in a base liquid for
solar radiation. The optical features of the nanofluids containing GO
were determined. An optimal concentration of 0.012% was observed,
causing the lowest reflectance and maximum absorbance over the
visible spectral range.
Yu et al. [69] produced a stable nanofluid containing ethylene
glycol (EG) and graphene oxide sheets. The results indicated that the
thermal conductivity of the nanofluid is significantly greater than that
of the ethylene glycol. In addition, the thermal conductivity remained
invariant for seven days showing appropriate stability.
Yu et al. [70] measured thermal conductivity of the nanofluids
prepared by graphene oxide sheets and base fluids of the water, liquid
paraffin, and propyl glycol. At a concentration of 5%, the enhancements
of thermal conductivity were 30.2%, 62.3% and 76.8% as the base li-
quids were the water, propyl glycol and liquid paraffin, respectively.
Yudong et al. [71] studied nucleation rate and supercooling degree
of GO-water nanofluids using classical nucleation theory. It was re-
vealed that two types of nucleation in the GO nanofluids could differ by
23.08 orders of magnitude at 241.65 K. Furthermore, the super-cooling
degrees decreased by higher than 74% with the nanoparticle con-
centration increment.
In spite of the interesting characteristics, there are still some pro-
blems with graphene oxide for efficient utilization in nanofluids. The
existence of structural defects, rather poor stability, restacking, and
multilayer thickness can influence the features and great surface area of
graphene oxide. The insulating property of conventional graphene
oxide also restricts its use in energy-related applications with the aid of
nanofluids. Opportunely, the oxygenated groups can strongly enhance
the structural and chemical variety of GO through chemical functio-
nalization or modifications, which suggest an efficient route to assign
the different physical and chemical attributes of GO. Consequently, GO
nanofluids can have noticeable potentials in the applications of energy
conversion, energy storage as well as thermal engineering. The physical
and chemical attributes based on the pH-dependent amphiphilicity of
graphene oxide have also introduced vital insights about the specific
properties of GO such as mass transport and permeation, wetting as
well as self-assembly at interfaces, which should be considered in the
studies related to GO nanofluids. Finally, because of the extensive
structural variety and enhanced characteristics, graphene oxide nano-
fluids possess promising applications in energy fields including photo-
catalyst for water splitting, hydrogen storage materials, water pur-
ification, removal of air pollutants, and so forth.
It is noteworthy that a comprehensive history for the creation of
graphene oxide with various reagents including concentrated sulphuric
acid, nitric acid, and potassium chlorate with HCrO4, KMnO4, gaseous
CIO2, Mn2O7 can be found in Ref. [72].
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Energy Conversion and Management 196 (2019) 1222–1256
2.4. Reduced graphene oxide
Generally, graphene oxide possesses proper dispersion in water
because of the hydrophilic groups on the surface, while enhancement of
thermal conductivity in suspensions containing GO is minor in com-
parison with base fluids. In contrast, graphene enhances the thermal
conductivity of base fluids considerably, whereas it shows poor stabi-
lity. As a result, utilizing reduced graphene oxide as an additive in base
fluids can be a very good item to enhance both thermal conductivity
and stability. Reduced graphene oxide exists in different forms in-
cluding one-atom-thick, flexible construction, and honeycomb struc-
ture. Owing to excellent thermal stability, charge transportation, elec-
tron mobility, electrical conductivity, thermal conductivity, mechanical
strength and optical properties, rGO can be employed for developing
various types of advanced materials in different situations such as solar
energy conversion storage, nanofiltration, chemical batteries, nano-
scale electrodes, and so on. Meanwhile, rGO has been utilized for pre-
paring nanofluids in recent years.
Lin et al. [73] developed a novel nanosurfactant as a 2D charged
zirconium phosphate (CZ) nanoplatelet and then, used it for dispersing
rGO in a base liquid. The results indicated that the rGO nanofluids vary
from non-homogeneous non-Newtonian nanofluids to homogeneous
Newtonian ones after being exfoliated with the aid of CZ nanoplatelets.
Zubir et al. [74] employed an rGO nanofluid for enhancing thermal
efficiency a closed duct structure. They prepared rGO by reduction
process of chemically exfoliated GO via Tannic acid. The convective
heat transfer enhancement of the nanofluid was greater than the
thermal conductivity increment, which is due to the significant effects
of both particles and turbulent induced flow attributes.
Zhang et al. [75] synthetized water-based nanofluids containing
controlled rGO at various concentrations through ultrasonication. Fig. 3
shows the production process of controlled reduced graphene oxide
(CRGO). The prepared nanofluids had proper stability with an incre-
ment of the concentration and temperature. Moreover, all nanofluids
demonstrated Newtonian behavior at high shear rates.
It should be noted that the excellent properties of rGO are related to
monolayer or few-layered structures. However, similar to carbon na-
notubes, neighboring rGO sheets causes aggregating them into macro-
scale carbon allotropism due to the strong π-π interaction between the
exposed sp2 electrons on the surface of rGO sheets. Therefore, the
quality of nanoparticle dispersion is very important in preparing na-
nofluids containing rGO. Schlierf et al. [76] used pyrene derivatives for
stabilizing rGO suspensions because of the repulsive forces and the π-π
interaction between functionalized pyrene derivatives and π systems of
rGO. Polymers having a great amount of aromatic rings can forcefully
connect on rGO monolayers by π-π interactions, and uniformly sus-
pended rGO can enhance thermal, electrical and mechanical char-
acteristics. Biomolecules including peroxidase, heparin, hexahistidine,
M. Bahiraei and S. Heshmatian
glucose oxidase, and peptide have also been successfully attached on
rGO monolayers with the aid of repulsive forces, aromatic π-π inter-
actions, and hydrophobic interactions.
Considering the chemical reduction of graphene oxide, the benefits
of this approach are as below:
- The method is a simple and cost-effective procedure with the use of
inexpensive chemical solutions;
- The technique results in a great yield of graphene dispersion scal-
able for industrial situations;
- The chemically-derived graphene causes highly stable suspensions;
- Great-size graphene layers can be prepared, which facilitates mac-
roscopic production.
2.5. Nitrogen-doped graphene
A method for reaching more efficient properties of graphene sheets
is doping heteroatoms such as nitrogen, sulfur, boron, and fluorine into
graphene sheets. Among different dopants, nitrogen as a well-known
item can be doped by various techniques including nitrogen plasma
process, chemical vapor deposition, and thermal treatments.
Applications of nitrogen-doped graphene have been regarded fre-
quently for water treatment units and electrochemistry. Because doping
graphene materials with the aid of nitrogen atoms enhances electrical
conductivity, investigation of thermo-electrical features of nanofluids
containing N-doped hybrid of graphene is very important from the
applied viewpoint. In the field of nanofluids, some scholars have eval-
uated nanofluids containing nitrogen-doped graphene nanomaterials
under different conditions.
Mehrali et al. [77] synthesized nitrogen-doped graphene (NDG)
nanofluids through the two-step approach inside a solution of Triton X-
100 as the dispersant. The nanofluid electrical conductivity indicated a
linear dependence on the concentration and enhanced up to 1814.96%
for a concentration of 0.06 wt%.
Seyed Shirazi et al. [78] prepared a nitrogen doped activated hybrid
material including carbon obtained from empty fruit bunch pulp as a
waste material, and GO using KOH and urea by one step thermal
treatment. The related images have been shown in Fig. 4. The results
Fig. 4. (a) FESEM images of nitrogen doped activated carbon/graphene, (b) pure activated carbon, (c) TEM image and (d) Elemental mapping of nitrogen doped
activated carbon/graphene [78]. Reprinted with permission from Elsevier.
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Energy Conversion and Management 196 (2019) 1222–1256
revealed an appropriate connection of GO to the carbon matrix having a
spongy-like configuration with the great nitrogen content and surface
area. In addition, a noticeable increment in thermal conductivity and
electrical conductivity of the base fluid proved its potential for utili-
zation in nanofluids.
Mehrali et al. [79] studied the heat transfer performance of a
grooved heat pipe with employing NDG nanofluids. A 58.6% reduction
in the thermal resistance and a 99% increment in the evaporator heat
transfer coefficient were obtained for the nanofluid at a concentration
of 0.06 wt%, heating power of 120 W and inclination angle of 90°
compared with the base fluid.
Shende and Sundara [80] examined the utilization of a nanofluid
containing N-(rGO-MWNTs) (nitrogen-doped hybrid structure of rGO
and multi-walled carbon nanotubes) in a direct absorption solar col-
lector. A 17.7% increase in thermal conductivity at 0.02% concentra-
tion with the water and a 15.1% enhancement at 0.03% concentration
with the ethylene glycol were observed. Moreover, the nanofluid had
proper stability because of the percolation network developed by in-
tercalation of the MWNTs between the rGO layers.
2.6. Nanofluids containing graphene sheets functionalized via ecofriendly
methods
It is known that graphene-based materials are hydrophobic, and
accordingly, it is not possible to disperse them in polar fluids like water.
Therefore, several techniques are implemented to enhance the stability
of graphene sheets in organic and aqueous liquids via physical and
chemical methods, including covalent or non-covalent functionaliza-
tion. Graphene sheets are functionalized by acid treatment and become
hydrophilic for stable dispersion in polar liquids. Functionalization
leads to the introduction of functional groups like hydroxyl and car-
boxyl on the surface of graphene sheets. It is noteworthy that functio-
nalization approaches may lead to defects on graphene plates and also
cause hazardous and toxic materials. Besides, used organic solvents in
addition to strong acids cause environmental pollution, health dangers
as well as corrosion. As a result, developing ecofriendly and green ap-
proaches to functionalize graphene plates is essential. In this regard,
some investigators have adopted ecofriendly methods for
M. Bahiraei and S. Heshmatian
Fig. 5. TEM images of (a) graphene oxide and (b) wine reduced graphene oxide [82]. Reprinted with permission from Elsevier.
functionalization of graphene plates in preparing stable nanofluids.
Shazali et al. [81] offered an ecofriendly cost-effective technique for
the synthesis of tetrahydrofurfuryl polyethylene glycol-functionalized
graphene nanoplatelets (TFPEG-treated GNPs) with proper stability in
water. The authors employed zirconium (IV) oxychloride octahydrate
as the catalyst for covalently functionalizing the GNPs with TFPEG. The
nanofluids having these nanosheets showed appropriate stability.
Mehrali et al. [82] suggested a novel ecofriendly method to produce
a graphene-based nanofluid and employed a new mode of GO reduction
via functionalization with polyphenol extracted from red wine. Fig. 5
illustrates the TEM images of GO and wine reduced graphene oxide. It
was observed that the deoxygenation level of the reduced graphene
oxide is rather similar to that reported by common techniques.
Sadri et al. [83] implemented a green approach to synthesize a new
nanofluid containing highly dispersed functionalized GNPs. The gra-
phene nanoplatelets were functionalized covalently with Gallic Acid
(GA) in a one-pot free radical grafting technique (see Fig. 6). Gallic acid
is a natural polyphenol antioxidant that can be extracted from berries,
green tea, grapes, and wine. The resultant nanofluids indicated a con-
siderable increment in the convective heat transfer coefficient.
Sadri et al. [84] used a green covalent functionalization technique
to prepare highly stable graphene nanoplatelets in aqueous media (see
Fig. 6. Process of functionalization approach for the graphene nanoplatelets [83]. Reprinted with permission from Elsevier.
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Energy Conversion and Management 196 (2019) 1222–1256
Fig. 7). This method involved free radical grafting of biological Gallic
acid onto the surface of GNPs instead of corrosive inorganic acids. The
solubility of the nanosheets in the aqueous media was verified, and the
obtained nanofluid also demonstrated great enhancements in thermo-
physical properties.
3. Preparation methods of nanofluids containing graphene-based
materials
Before explaining the preparation methods of nanofluids, a brief
description is presented on synthesis methods of graphene-based na-
nomaterials.
Graphene family materials can be produced in single-layer form or
multi-layer form. Single-layer graphene is usually synthesized from
highly ordered pyrolytic graphite via micromechanical cleavage. In the
following, four main methods of preparing graphene are introduced. A
monocrystalline graphitic film including a single one-atom-thick carbon
layer can be synthesized via peeling it from a tiny platelet of highly
oriented pyrolytic graphite under a mechanical exfoliation method
through a scotch tape. Mechanical exfoliation demonstrates a technique
in which transverse or longitudinal stress is applied on the surface to
prevail the van der Waals binding energy [18].
M. Bahiraei and S. Heshmatian
Fig. 7. Green covalent functionalization technique for GNPs [84]. Reprinted with permission from Elsevier.
Another method to reach graphene is Chemical Vapor Deposition
(CVD) [85] of graphene on metals and metal oxides. The CVD is a
method for dissolving gaseous reactants such as propane, methane or
ethane into warmed substrates like Ni or Cu, in which the reaction leads
to graphene film growth on top of the substrate from the nucleation
sites in the cooling course. A great-scale area of single-layer to few-layer
graphene films is generally grown on different metal substrates like Pt,
Cu, Ir, Ni, Co, and Ru. To reach superior control of the growth of
monolayer or bilayer graphene, Cu and Ni are frequently employed
rather than the other metals which have greater prices. The transmitted
substrate can be either a metal or polymer [86] where the transfer
procedure might lead to damages such as tearing and wrinkles forma-
tion. It can be mentioned that the CVD method results in multi-layer
graphene, and also, it is difficult to be taken out from metal surfaces. It
is noteworthy that no chemical method has been introduced so far to
produce graphene with given numbers of layers.
As another approach, liquid exfoliation is a low-cost top-down
procedure to fabricate graphene in solutions applying an ultrasonic
energy source for generating micro-cavitations and blasting the raw
bulk graphite into smaller pieces and finer layers of graphene. Several
hours are required for extracting the graphite into separate layers. The
technique of the liquid exfoliation is performed in organic solvents such
as N,N-dimethylacetamide (DMA), N-methylpyrrolidone (NMP), γ-bu-
tyrolactone (GBL) and 1,3-dimethyl-2-imidazolidinone (DMEU). This
approach is very general thanks to the easy intercalation, cavitation,
and exfoliation process. The exfoliated graphite layers demonstrate
great throughput during the production course. A lengthy ultrasonica-
tion stage, however, may damage the exfoliated graphene platelets
causing tiny size and nano-impurities. The thickness of the exfoliated
graphite layers is in the range of 10 nm to 100 nm where they miss the
unique graphene electronic features. For enhancing the characteristics,
microwave radiation and annealing are employed for the removal of the
air bubbles and trapped solvent and decreasing the nano-scrolling im-
pact.
The epitaxial growth on SiC is another approach that starts with
silicon carbide (SiC) heated up to 1250–1450 °C in ultrahigh vacuum.
After that, the silicon ions sublimate, leaving behind the carbon atoms
on the surface of SiC. After cooling under optimal states, the carbon
atoms self-organize into a honeycomb configuration. The epitaxial
graphene on SiC can then be transmitted onto a specific substrate as
free-standing graphene. For instance, epitaxial graphene reaches the
transfer by applying a thin gold layer and polyimide to peel-off from SiC
to a SiO2/Si wafer. But, the resultant graphene layer shows great
amounts of defects with small mobility of 100 cm2/Vs [87]. This tech-
nique has some problems in control of the number of layers as well as
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Energy Conversion and Management 196 (2019) 1222–1256
the existence of disorder or defects in the hexagonal configuration.
Graphene oxide materials can be achieved through a simplified
Hummers technique that is indicated elsewhere [88,89]. Hummers
method is oxidization of graphite plates via treatment with different
solutions of NaNO3, KMnO4, H2O2, and concentrated H2SO4, and after
that washing with the aid of water and HCl [77]. In 1958, this method
was introduced for synthesizing GO as a safe, quick, and effective ap-
proach. Before introducing the Hummers method, production of GO
was dangerous and sluggish because of using sulfuric acid and con-
centrated nitric.
The Hofmann, Staudenmaier, and Hummers techniques introduced
adding potassium chlorate [90]. This approaches, however, had the
dangers and prepare one gram of GO to ten grams of potassium chlo-
rate. Hummers and Offeman [91] presented an approach as an alter-
native to the abovementioned techniques regarding hazardous wastes.
Their method was to add graphite powder to a solution of concentrated
acid. While, it was simplified to just graphite, sulfuric acid, potassium
nitrate, and concentrated sodium nitrate.
Graphene family based nanofluids can be prepared through the one-
step approach or two-step approach. In the one-step approach, nano-
fluids are produced directly via chemical techniques. In the two-step
approach, graphene sheets are firstly produced in nanopowder form
through chemical or physical techniques such as laser ablation,
grinding and sol-*gel processing methods and after that, are suspended
in a base liquid. Yu et al. [92] introduced a chemical approach to
synthesize GO sheets. The graphene oxide sheets were produced with
exfoliating graphite oxide in anhydrous ethanol. The resultant product
of nanoparticles was a loose brown powder, which was suspended in
ethylene glycol without any dispersants for preparing the nanofluid
under a two-step method.
Hajjar et al. [93] synthesized GO from graphite powder through the
modified Hummers method. The hydrophilic surfaces resulted in proper
compatibility between the water and graphene oxide sheets. Hence,
graphene oxide sheets were appropriately suspended in the base fluid
only with employing ultrasonication without any dispersants.
Sadri et al. [94] prepared covalently functionalized GNPs disper-
sions that were greatly stable and environmentally friendly. The GNPs
were functionalized by clove buds through the one-pot method. After
that, the clove-treated GNPs were added to the base fluid for preparing
the nanofluid through a two-step method. The hydrophilic functiona-
lized groups were certified through the UV–vis absorption spectra,
which resulted in good stability even about two months after synthesis.
Fig. 8 displays the method employed for preparing the clove extract.
Martin-Gallego et al. [95] prepared the rapid thermal expansion of
GO at a temperature of 1000 °C under the inert atmospheric state. They
M. Bahiraei and S. Heshmatian
Fig. 8. The technique employed for preparing the clove extract [94]. Reprinted with permission from Elsevier.
synthesized the carbon material having great surface area including
graphene layers with residual hydroxyl, carbonyl, and epoxy groups.
The authors indicated that phonon coupling of the vibrational modes of
the graphene and the polymeric matrix has a significant effect on the
thermal conductivity.
Wang et al. [96] reported preparing a highly stable graphene-based
nanofluid with ionic liquid without any additives. It should be noted
that nanofluids with ionic liquids, as base fluid, are termed ionano-
fluids. Optical photos were supplied with locating a drop of the fluid on
a cleaned glass, and the nanoparticle dispersion in the base fluid was
detected. The even distribution of graphene sheets in the liquid was
evident in these images.
Baby and Sundara [97] presented a technique for preparing nano-
fluids containing graphene sheets decorated with metal oxide nano-
particles. At first, the authors added hydroxyl and carboxyl functional
groups on the surface of graphene sheets under acidic treatment and
ultrasonication. After that, the functionalized graphene sheets were
employed for decorating the copper oxide nanoparticles.
Ahammed et al. [98] produced a graphene-water nanofluid by use
of the two-step approach. Just a low value of sodiumdodecyl benzene
sulfonate was employed to stabilize the graphene sheets. The surfactant
was first added to the water and after that, the graphene sheets were
added, while the suspension was sonicated by an ultrasonic vibrator.
Great zeta potential was noticed showing suitable stability.
Kole and Dey [99] and Baby and Ramaprabhu [100] utilized dried
graphene oxide for synthesizing the hydrogen exfoliated graphene
(HEG) in hydrogen atmosphere. Functionalizing the HEG was carried
out via treating with acid and ultrasonication. Kole and Dey [99] pre-
pared nanofluids containing the functionalized HEG sheets at con-
centrations between 0.041 and 0.395 vol% with no surfactant. It was
found that the conventional models cannot predict the dependency of
the viscosity of these nanofluids on the concentration. Also, Baby and
Ramaprabhu [100] dispersed the HEG nanosheets in the deionized
water and ethylene glycol. The water-based nanofluid demonstrated
increments in thermal conductivity by almost 16% at 25 °C and 75% at
50 °C for a concentration of 0.05%.
Dhar et al. [101] prepared graphene based nanofluids in which the
graphene sheets were produced by a two-step procedure. Oxidation of
the graphite powder to the GO sheets was carried out through the
modified Hummers method, followed with the GO reduction to the
rGO. The observations proved that the graphene sheets achieved are
two- or three-layered.
Ghozatloo et al. [102] and Park et al. [103] produced graphene
nanoflakes. The CVD method was employed to make the graphene
sheets on Cu foil through catalytic decomposition in a quarts tube
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Energy Conversion and Management 196 (2019) 1222–1256
furnace device. After that, functionalization of graphene sheets was
performed using a reflux system and potassium per sulfate. Finally, the
nanofluid was papered with adding the graphene nanoflakes to the
water.
Fan et al. [104] oxidized graphite flakes using an improved Hum-
mers method. A mixture of H3PO4 and H2SO4 was added to a mixture of
the graphite flakes and KMnO4, and after that the solution was stirred.
After stirring, the mixture was cooled for reaching the room tempera-
ture. As the mixture became yellow color after the addition of H2O2, the
deposit was centrifuged, and the remaining material was washed. The
graphene oxide nanosheets were produced after drying at room tem-
perature. The relevant preparation procedure is shown in Fig. 9a. GO
can be chemically reduced to graphene with different reducing agents.
In this research, 100 mg GO was dispersed in 100 mL water. After ad-
dition of 50 mL hydrazine monohydrate to the mixture, it rapidly be-
came black. The solution was warmed for refluxing and then, was
cooled to room temperature. The product was washed in ethanol and
water and then, was filtered. The graphene powder was achieved
through vacuum-drying the obtained deposition on the filter, according
to Fig. 9b. The authors also produced the Sn@SiO2 nanoparticles for
preparing a hybrid graphene nanofluid as per Fig. 9c. Moreover, the
interaction of the nanofluid and sunlight related to this work is pre-
sented in Fig. 10.
Lee et al. [105] synthesized graphene oxide–water nanofluids with
suspending GO sheets into the water. The authors prepared the GO
sheets through the CVD method. The zeta potential and pH of the na-
nofluid were −31.5 mV and 3.58, respectively. The authors indicated
that these magnitudes demonstrate reasonable stability.
Sun et al. [106] added graphite to a polymer solution for preparing
the graphene suspensions. A sonicator bath was utilized to remove
graphite aggregates. Then, the top two-thirds of the suspension was
gradually removed via pipetting after centrifugation. The suspensions
were stable for 24 h irrespective of heating (70 °C) or freezing (−26 °C).
Legrand et al. [107] synthesized the graphene sheets by homo-
geneous nucleation following the plasma decomposition of a carbon
material inside an inductively coupled thermal plasma reactor. After
synthesis, the graphene sheets were functionalized with adding oxygen
to the main plasma stream. Tunable oxygen functionalization was
achieved, and amounts up to 14.2 atomic percent were obtained on the
surface. Although the non-functionalized graphene sheets were hydro-
phobic, the oxygen functionalized ones demonstrated perfect stability.
Li et al. [108] presented an approach for preparing the solvent-free
graphene nanofluid. The authors prepared the graphene oxide through
the modified Hummers method, and after that, the khaki precipitate
was made by ammonia solution in the presence of ionic surface
M. Bahiraei and S. Heshmatian
Fig. 9. Preparation mechanism of (a) GO, (b) graphene, and (c) Sn@SiO2 nanoparticle [104]. Reprinted with permission from Elsevier.
Fig. 10. Interaction of nanofluid and sunlight [104]. Reprinted with permission
from Elsevier.
modifier and sonication. In the next step, they washed the precipitate
for removing the excess of the ionic surface modifier and dried it. The
graphene nanofluid was then produced with treating graphene chlorine
salt by potassium sulfonate salt in methanol, and the product was
dialyzed, dissolved and centrifuged. Lastly, the resultant particles were
extracted, and the supernatant liquid was collected and dried for
achieving the solvent-free graphene nanofluid.
Mehrali et al. [88] produced nitrogen-doped graphene from the
original GO via hydrothermal treatment with the assistance of am-
monia. The authors dispersed the obtained nitrogen-doped graphene
nanosheets in a base liquid by the two-step approach. The electrical
conductivity of the nanofluid increased considerably because of adding
NDG nanosheets to the base liquid.
Ma et al. [109] presented an approach for preparing stable
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Energy Conversion and Management 196 (2019) 1222–1256
nanofluids, including functionalized graphene sheets. The functiona-
lized graphene sheets were prepared via a two-step technique with 3-
glycidoxypropyltrimethoxysilane as the functionalization modifier. The
nanofluids were produced with adding the graphene sheets to the base
liquid.
Table 1 lists some of the studies carried out on graphene-based
nanofluids regarding the preparation methods.
Production of monosized graphene platelets is still a challenging
topic. It is noteworthy that graphene family materials are frequently
produced with rather poor quality in some of the extensively utilized
techniques. Indeed, some of the chief causes restricting the adoption of
technologies on the basis of graphene materials are the present re-
strictions in producing these materials. The CVD approach synthesizes
small amounts of graphene nanosheets restricting the variety of appli-
cations. Moreover, the poor crystallinity, noticeable disorder, and the
low purity of rGO lead to great limitations for reduced graphene oxide
sheets. Furthermore, the graphene exfoliation can only be adopted in
limited systems, has some problems like rather small concentrations,
and requires significant sonication.
Nucleophilic substituting an amine-terminated organic modifier in
the presence of covalent modification is regarded as the simplest ap-
proach for producing functionalized graphene sheets. Some studies,
however, show the quality reduction for graphene sheets obtained from
this method because of sonication and chemical oxidation. Also, elec-
trical conductivity and thermal conductivity of these functionalized
graphene sheets reduce noticeably.
Based on the relevant literature, single-layer graphene possesses
superior thermal conductivity than multi-layer graphene sheets. The
interlayer linkages can cause a significant reduction in thermal con-
ductivity of multi-layer graphene sheets concerning location, kind and
concentration of interlayer linkages. In addition, thermal conductivity
 Table 1
Some of the studies carried out on graphene-based nanofluids regarding the preparation methods.
M. Bahiraei and S. Heshmatian

Authors Year Material Base liquid Preparation method Concentration

Li et al. [108] 2014 Graphene Water Modified Hummers method and then synthesis of the 10 mg/ml
material
Fan et al. [104] 2017 GO nanosheets Water Modified Hummers method 0.05–0.3 g/L
Park and Kim [110] 2014 Graphene sheets and GO Water Prepared by the manufacturer and after that oxidation by 0.001–0.01 vol%
acid
Irani et al. [111] 2019 GO nanosheets Diethanolamine modified Hammer method 0.1 and 0.2 wt%
Baby and Ramaprabhu [112] 2011 Graphene decorated with silver nanoparticles Water Modified Hummers method to synthesize the GO 0.005–0.056 vol%
Mehrali et al. [113] 2014 GNPs Water Prepared by manufacturer 0.025–0.1 wt%
Dhar et al. [114] 2013 Polydispersed graphene Water Modified Hummers method and after that synthesis of the 0.05–0.2 vol%
material
Shende and Sundara [80] 2015 Nitrogen-doped graphene Ethylene glycol water GO was produced via Hummers method 0.005–0.03 vol%
0.005–0.02 vol%
Ghozatloo et al. [102] 2013 Ag nanoparticles decorated multiwalled carbon nanotubes- Water Modified Hummers method and after that synthesis of the 0.005–0.04 vol%
graphene material
Yu et al. [92] 2010 GO nanosheets Ethylene glycol Modified Hummers method 1–5 vol%
Baby and Ramaprabhu [100] 2011 HEG Ethylene glycol water Exfoliation of GO 0.005–0.05 vol%
0.05–0.08 vol%
Hernaiz et al. [115] 2019 GO nanosheets Water Modified Hummers method 0.1 g/L

1232
Lee et al. [105] 2013 GO nanosheets Water CVD 0.01 vol%
Yu et al. [69] 2010 GO nanosheets Ethylene glycol Modified Hummers method 0.01–11.03 wt%
Mahmudul Haque et al. [116] 2015 MWCNTs and graphene nanopowder Water Synthesized by manufacturer Mass ratios were 1/3, 3/1, 1/1, 1/2 and 2/1
Moghaddam et al. [117] 2013 Few-layer graphene nanosheets Glycerol Burning magnesium metal in dry ice Mass fractions (0.0025–0.0200)
Park et al. [118] 2010 Graphene and GO nanosheets Water Modified Hummers method 0.001 vol%
Campos et al. [119] 2019 Graphene oxide Water Hummers and Offeman method 0.2 g/L
Yu et al. [70] 2010 GO nanosheets Ethylene glycol Modified Hummers method 0.01–0.05 vol%
Esmaeili Faraj et al. [120] 2014 Exfoliated GO Water Modified Hummers method and after that synthesis of the 0.005–0.025 wt%
material
Liu et al. [121] 2014 Graphene sheets Water Modified Hummers method and reducing GO Mass fractions (0.03–0.06)
Mehrali et al. [88] 2014 Nitrogen-doped graphene Water Modified Hummers method and after that synthesis of the 0.01–0.06 wt%
material
Park and Bang [122] 2013 GO Water Modified Hummers method 0.0001 vol%
Liu et al. [123] 2014 Functionalized graphene–metal nanoparticles Water Modified Hummers method and after that synthesis of the 1–3 G (generation)
material
Baby and Ramaprabhu [124] 2010 Graphene nanosheets Ethylene glycol + water Modified Hummers method 0.005–0.056 vol%
Akhavan-Zanjani et al. [125] 2014 Graphene nanosheets Water Modified Hummers method and reducing GO 0.005–0.02 vol%
Park et al. [126] 2012 GO Water Modified Hummers method 0.0001 vol%
Dhar et al. [101] 2013 Polydispersed graphene sheets Water Modified Hummers method and after that synthesis of the 0.5 wt%
material
Yu et al. [127] 2011 Graphene nanosheets Ethylene glycol Modified Hummers method 0.01–11.03 wt%
Baby and Sundara [97] 2011 Graphene sheets decorated with copper oxide nanoparticles Ethylene glycol + water Hydrogen-induced exfoliation/reduction of graphite oxide 0.005–0.056 vol%
Energy Conversion and Management 196 (2019) 1222–1256
M. Bahiraei and S. Heshmatian
may be considerably decreased due to the existence of vacancies in
linkages. Although the mentioned aspects of graphene production
methods are important, they have been mainly ignored whereas can
clarify the reasons for changes in different features of graphene-based
nanofluids. Besides, controlled graphene production and precise char-
acterization can aid to understand the essential causes which influence
different attributes of the graphene family based nanofluids.
4. Stability of graphene-based nanofluids
The stability mechanism of nanofluids is demonstrated as the rate of
aggregation of nanoparticles suspended in base liquid, which is com-
monly evaluated via the frequency of collisions as well as the prob-
ability of cohesion due to collisions. Nanoparticles may adhere together
and form aggregates at grater scales, which causes sedimentation and
agglomeration. As per the theory of Derjaguin, Landau, Verway, and
Overbeek (DLVO) [128], which is on the basis of suspensions stability,
the stability of each particle in solutions is found by the sum of Van der
Waals attractive forces and the electrical double layer repulsive forces
occurring between the nanoparticles when they approach each other
because of the Brownian motion. In the case that the Van der Waals
attractive forces are greater than the repulsive forces, the particles will
aggregate and settle, which causes a non-stable colloid. On the con-
trary, in the case that the net electrical repulsive force between the
particles is large, the colloid will be stable, and agglomeration will not
happen. Based on the type of repulsion forces, the dispersed nano-
particles can be stabilized by steric repulsive and electrostatic (charge)
or electro-steric repulsive forces, as illustrated in Fig. 11 [129].
In steric stabilization, polymers are directly added to the colloid
system and absorbed on the surface of particles, which results in an
additional steric repulsive force. In electrostatic stabilization, the
charges on the surface of nanoparticles are developed through the
below mechanisms:
- Preferential adsorption of ions
- Dissociation of the surface changed species
- Isomorphic substituting ions
- Depletion or accumulation of electrons at the surface
- Physical adsorption of charged species onto the surface
One of the most important problems in preparing nanofluids con-
taining graphene-based materials is to disperse the nanosheets in base
fluids and improve their stability. In reality, graphene is hydrophobic
and cannot be dispersed in most of liquids for a long time, and shows a
significant tendency to agglomerate. Many efforts have been made to
enhance the stability of graphene materials in a variety of liquids in-
cluding covalent and non-covalent techniques.
In covalent functionalization methods, permanent bonding between
carbon atoms and other organic molecules is created, while it needs the
opening of the aromatic conjugated structure of the material.
Fig. 11. Types of suspensions stabilization [129].
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Energy Conversion and Management 196 (2019) 1222–1256
Consequently, electrical and thermal characteristics of nanofluids may
be degraded thanks to the disturbance in electron transports and bal-
listic phonon.
Covalent functionalization includes chemical reactions between
graphene platelets in the main structures and other functional groups,
which produce functionalized materials with various features. Acid
treatment demonstrates one of the methods for covalently functiona-
lizing graphene sheets, and is often adopted by scholars to enhance the
stability of graphene sheets in different liquids. Although acid treat-
ment changes the original structure of the material, it is proved to be an
efficient approach to produce stable suspensions of graphene-based
nanomaterials. However, a high grade of functionalization is needed in
this technique for reaching graphene sheets with proper dispersibility.
This causes a great level of generation of sp3-hybridized carbons in the
main backbone. Therefore, the selection of functional groups with long-
chain branches and high hydrophilicity has been recommended for
reducing the sp3-hybridized carbons generation in the main backbone.
Generally, the organic covalent functionalization reactions of gra-
phene comprise two overall ways: (a) formation of covalent bonds be-
tween C]C bonds of graphene sheets and free radicals or dienophiles,
and (b) formation of covalent bonds between the oxygen groups of
graphene oxide and organic functional groups. One instance of covalent
modifications is the chemical reaction of amine-terminated ionic liquid-
modified graphene oxide [130], which results in appropriate stability in
water.
Another approach that is used for improving stability of graphene
materials in liquids is the non-covalent method which frequently em-
ploys polymers or surfactants to isolate particles. The non-covalent
methods are based on the repulsive nature of surfactant or polymer
molecules in addition to short-range hydrophobic physisorption be-
tween graphene sheets and relevant stabilizing materials. Several sta-
bilizers have been evaluated for improving the stability of graphene
sheets and other carbon materials in a variety of liquids [131,132].
Surfactants can increase the surface charge density on graphene sheets
and can develop significant electrostatic repulsive forces, such that
reunion of graphene sheets is decreased and thus, the stability is im-
proved.
Employing suitable non-covalent functionalization approaches can
considerably improve the stability of graphene sheets in base liquids in
which graphene sheets are wrapped with long-chain stabilizers. The
main mechanism behind this approach is π-π stacking interactions be-
tween the surface of graphene sheets and functional groups, which
decrease the influence on the surface and prevent disturbance in elec-
tron conjugation.
The most important techniques for evaluating the stability of na-
nofluids are as follows:
- Zeta potential measurements
- Sedimentation photograph capturing
- UV–Vis spectrophotometer
- 3ω method
- Transmission Electron Microscopy (TEM)
- Dispersion analyzer centrifuge
- Scanning Electron Microscopy (SEM)
- Thermal conductivity measurement
- Sedimentation balance method
Based on the relevant literature, several studies have been carried
out to improve the stability of graphene-based materials in different
base liquids for preparing stable nanofluids. In these studies, different
approaches, including covalent and non-covalent functionalization
methods, have been employed.
Ghozatloo et al. [102] employed the alkaline method for functio-
nalizing graphene sheets in order to improve their stability in water.
The graphene sheets became hydrophilic through treating with this
approach. The authors reported a simple and efficient method for
M. Bahiraei and S. Heshmatian
synthesizing the water-graphene nanofluid using the potassium car-
boxylate in a mild oxidation process with employing potassium per-
sulfate.
Sarsam et al. [133] investigated the impact of employing four dif-
ferent surfactants including sodium dodecyl sulfate (SDS), sodium do-
decyl benzene sulfonate (SDBS), gum Arabic (GA) and cetyl trimethy-
lammonium bromide (CTAB) on the stability of water-GNPs nanofluids.
The greatest stability was achieved at ultrasonication time of 60 min.
The water–pristine GNPs nanofluids did not show good stability, while
the stability was enhanced by adding the surfactants. The existence of
SDBS, SDS, and CTAB surfactants caused some foam. Among all the
nanofluids, the SDBS–GNPs sample demonstrated the best stability.
Sun et al. [106] used polymerization for enhancing the stability of
nanofluids containing few-layer graphene sheets. The monomers of
allyl methacrylate, polyethylene glycol methacrylate, butyl acrylate, 2-
(dimethylamino) ethyl methacrylate, and methacrylic acid were used to
synthesize the polymer. The resultant polymer resulted in better dis-
persing capability for the graphene sheets in comparison with the
conventional dispersants.
Radnia et al. [134] developed a new nanofluid based on sulfonated
graphene (G-DS-Su) for enhanced oil recovery. The nano porous gra-
phene produced through the CVD technique was sulfonated using 4-
sulfobenzenediazonium salt. After that, more sulfonated groups were
introduced to the functionalized graphene, and the last product was
termed as G-DS-Su. The zeta potential was about −30 mV showing the
stable nanofluids. Fig. 12 shows the amphiphilic nature of G-DS-Su at
the water–oil interface.
Irani et al. [135] assessed a new method via adding amine-modified
reduced graphene oxide to amine solutions for enhancing the CO2 ab-
sorption capacity. Amine functionalized rGO/methyl diethanolamine
(MDEA) nanofluid was synthesized to absorb acid gases. The graphene
oxide was functionalized by the solvothermal approach, and the NH2-
rGO suspended in MDEA indicated very good stability.
Paul et al. [136] examined the tribological features of nano-lu-
bricants prepared by dispersing dodecylamine functionalized graphene
sheets in engine oil. About 500 mg of graphite oxide was taken in a flask
containing water and was mixed. After that, the suspension was cen-
trifuged for removing unexfoliated graphite oxide. Dodecylamine was
dissolved in ethanol and was then added to the graphene oxide sus-
pension. At the next step, the dispersion was refluxed for almost 24 h.
The suspension turned into black together with some black aggregates
which demonstrated mild reduction and also functionalizing the GO
sheets. The authors reported very good stability for the nanofluids.
It should be noted that the existence of surfactant additives can
affect thermal attributes and can decrease the thermal conductivity of
nanofluids thanks to the poor thermal conductivity of surfactants.
Therefore, to enhance the solubility of graphene materials in base fluids
without reduction of the thermal conductivity of nanofluids, an
Fig. 12. Amphiphilic nature of G-DS-Su at the water-oil interface [134]. Reprinted with permission from Elsevier.
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Energy Conversion and Management 196 (2019) 1222–1256
inorganic layer can be decorated on graphene platelets rather than the
use of surfactants. Method of coating nanomaterials via an inorganic
layer has been an efficient technique to enhance nanomaterial features
such as colloidal stability, chemical stability as well as biocompatibility.
Use of this approach in graphene-based nanofluids can enhance the
wettability of graphene nanosheets and can keep them at a certain
distance, which reduces the reunion of graphene sheets. Therefore, the
modifying the surface of graphene nanosheets through inorganic na-
nomaterials helps to overcome aggregation of graphene nanosheets and
so, can enhance the stability.
Indeed, with decorating the nanoparticles on carbon materials, a
type of composite is achieved. Composite materials obtained via dec-
orating metallic or metal oxide nanoparticles on carbon nanotubes have
been widely employed so far in fuel cells, catalytic or optoelectronic
applications, batteries, supercapacitors, and so on. In the recent decade,
because of the increased interest in graphene materials, coating gra-
phene nanosheets with the aid of metallic nanoparticles or other na-
noparticles has also become a key research subject. A graphene platelet
can be an excellent medium for decorating nanoparticles owing to its
great active surface area per mass unit compared with graphite or
carbon nanotubes that have a smaller active surface area in which only
their outside surface is active.
In reality, graphene can be two-dimensional support for growth,
assembly, and nucleation of metal or metal oxide nanoparticles, and
integrating influences of these nanoparticles with graphene sig-
nificantly improves the performance of these composite materials.
Hence, graphene-based metal or metal oxide composites having en-
capsulated, anchored, wrapped, layered, and mixed structures possess a
vast potential for several technological applications.
Existence of metallic or metal oxide nanoparticles prevents stacking
of graphene platelets, extends the total surface area and thus results in
stability enhancement of nanofluids along with heat transfer increment.
Decorating these nanoparticles on graphene sheets with functional
groups avoids graphene agglomeration and eliminates the requirement
of surfactants for stabilizing graphene nanomaterials in base liquids.
Besides, the utilization of graphene/metal oxide hybrid can improve
heat transfer features of base fluids considerably. This is due to the fact
that both graphene and metal oxides can enhance thermal attributes
separately and therefore, a higher increment can be perceived as these
structures are employed concurrently.
Usual approaches for decorating metal nanoparticles on graphene
sheets include covalent functionalizing graphene sheets to induce an-
choring sites for metal precursor and resulting connection of the re-
duced nanoparticles to the surface. This method leads to interruption of
sp2 bonded carbon atoms in the basal plane, which results in decreased
transport features of graphene due to further scattering sites. Another
extensively implemented method is nanoparticle growth on non-cova-
lently functionalized graphene sheets, which preserves the pristine
M. Bahiraei and S. Heshmatian
Fig. 13. Chemical exfoliation schematic of multi-layer graphene sheets [140]. Reprinted with permission from Elsevier.
characteristics of graphene platelets owing to minor chemical pertur-
bation of basal planes. Other approaches for decorating metal nano-
particles on graphene materials are evaporation, electrodeposition, and
solventless bulk preparation. Although these techniques demonstrate
some benefits in comparison with solution-phase methods, they are
rather expensive and energy intensive.
SiO2 nanoparticles are usually employed as coating nanomaterials
since SiO2 possesses several excellent features including chemical in-
ertness, hydrophilicity, ultraviolet resistance as well as biocompat-
ibility. The mentioned attributes guarantee that the physical and che-
mical characteristics of wrapped materials are retained when they are
coated. So far, very few graphene-based nanocomposites have been
utilized for preparing nanofluids. In the case of using SiO2 nano-
particles, SiO2-coated layers are anchored onto graphene sheets
through SieOeC bonds. Therefore, decorating SiO2 nanoparticles re-
places some of C]C and CeO stretching vibrations with SieO bonds on
graphene sheets. This method can decrease aggregation of graphene
sheets and result in lower sedimentation since SieO bond is more hy-
drophilic than C]C one, and also, SiO2 nanoparticles decorated on
graphene sheets can develop steric hindrance impact.
In some of the studies, decoration of nanoparticles on graphene
sheets has been performed for stability improvement in nanofluids.
Moreover, some of the investigators have examined hydrothermal
characteristics of nanofluids containing graphene platelets decorated
with nanoparticles in different thermal applications.
Li et al. [137] made a comparison between two methods of im-
proving the stability of graphene sheets in nanofluids, namely decora-
tion of nanoparticles on graphene sheets, and the use of surfactant.
SiO2-coated graphene sheets were synthesized through the chemical
liquid deposition technique. The authors also prepared another type of
water–graphene nanofluid with the use of the functionalized nanoma-
terial. The results revealed that the SiO2-coated modification enhances
the hydrophilicity and stability of the graphene sheets significantly. It
was also argued that the SiO2-coating enhances the thermal con-
ductivity better than surfactants.
Baby and Sundara [97] employed a new chemical reduction with
calcination for synthesizing graphene sheets decorated with copper
oxide nanoparticles. They functionalized the graphene sheets in an acid
medium for decorating the nanoparticles. The nanocomposite powder
obtained was properly dispersed in the pure water and ethylene glycol
without using any surfactant.
Baby and Ramaprabhu [112] introduced a new preparation method
for silver decorated functionalized hydrogen induced exfoliated gra-
phene (Ag/HEG) and then, synthesized nanofluids utilizing this mate-
rial. The authors applied a simple chemical reduction technique for
synthesizing uniformly coated Ag/HEG. The nanofluid obtained was
stable for more than three months.
Yarmand et al. [138] investigated thermal performance and friction
features of a graphene nanoplatelet-Platinum nanofluid in a stainless-
steel square duct. The results showed that the nanofluid has a greater
heat transfer rate in comparison with the base fluid. Moreover, the
Nusselt number was dependent on the particle concentration and
Reynolds number.
Bahiraei et al. [139] assessed the flow and heat transfer character-
istics of a nanofluid having GNPs decorated with platinum
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Energy Conversion and Management 196 (2019) 1222–1256
nanoparticles in tubes enhanced with different twisted tapes. The
configurations under investigation were single twisted tape (ST), twin
co-twisted tapes (CoTs) and twin counter twisted tapes (CTs). The heat
transfer amount in the tube equipped with CTs was significantly greater
than that in the other geometries.
Ramon-Raygoza et al. [140] introduced new formulations of nano-
lubricants by adding multi-layer graphene sheets, multi-layer graphene
sheets decorated with copper as well as multi-layer graphene sheets
coated via polyaniline to engine oil. For the nanofluid having the
copper decorated graphene sheets, the friction factor and wear reduced
by 43% and 63%, respectively. All three nanofluids did not demonstrate
any sedimentation for a long time. The chemical exfoliation of multi-
layer graphene sheets carried out in this study is illustrated in Fig. 13.
One of the novel strategies for improving characteristics of gra-
phene-based materials is to decorate magnetic nanoparticles on gra-
phene or graphene oxide sheets. By this approach, in addition to the
abovementioned attributes, the nanofluid possesses magnetic char-
acteristics, and therefore, it can be controlled with employing the ex-
ternal magnetic fields.
Syam Sundar et al. [141] synthesized graphene oxide sheets deco-
rated with Co3O4 nanoparticles by chemical co-precipitation method.
The hybrid nanofluid was also produced with suspending the resultant
GO/Co3O4 powder in different base fluids. The thermal conductivity of
the water-based nanofluid enhanced 19.14%, and that of the ethylene
glycol-based nanofluid enhanced 11.85% at particle loading of 0.2% in
comparison with their base liquids.
Askari et al. [142] prepared Fe3O4 decorated graphene sheets
through a new synthesis technique with the aid of oleic acid (see
Fig. 14) and then, produced the kerosene-based nanofluid by these
nanoparticles. The nanofluid remained stable for five months without
any sedimentation. Moreover, a 66% heat transfer enhancement was
obtained at a particle loading of 0.3 wt% and Reynolds number of 4553.
The interactions between graphene sheets and metal or metal oxide
nanoparticles in nanocomposite powders have opened the routes to
design and develop novel applications ranging from the energy issues to
the medical sector. In addition to improving the characteristics of
Fig. 14. Preparation of graphene-Fe3O4 coated with oleic acid [142]. Reprinted
with permission from Elsevier.
M. Bahiraei and S. Heshmatian
graphene sheets, metal and metal oxide nanoparticles work as stabi-
lizers against aggregating single graphene sheets, which is due to robust
van der Waals interactions among graphene layers. Hence, performing
more studies and introducing newer procedures for the synthesis of
graphene-based nanocomposite powders are crucial.
In spite of the noticeable progress in synthesizing graphene-based
nanocomposites, there are challenges for utilization in industrial scales.
Indeed, advanced applications of graphene sheets decorated with metal
or metal oxide nanoparticles need noticeable research studies to re-
cognize the interactions between graphene surface and nanoparticles,
which directly affect the properties of these nanocomposite powders.
It should be noted that functional groups result in a reduction in the
theoretical surface area of graphene sheets, which diminishes their
excellent features. As a consequent, applying nanoparticles as a guest
material on graphene sheets can be efficient and suitable in thermal
conductivity increment of functionalized graphene platelets.
In comparison with covalent techniques, non-covalent methods are
specifically promising since the achieved products are more simply
handled, and the modification can be performed such that the original
properties of graphene sheets are preserved, whereas the stability is
enhanced. However, the process capability and manipulation of gra-
phene platelets may not be satisfied because of the robust Van der
Waals forces.
Main problems on the utilization of surfactants in non-covalent
functionalization are usually related to the production of undesirable
foam, small temperature degradation, and severe surfactant con-
centration requirement that intensifies insulation of particles. These
factors diminish the thermal and electrical attributes in addition to
increase of nanofluid viscosity, particularly in the case of using high
molecular weight polymers. Due to the formation of foam related to the
utilization of surfactants, covalently functionalization is suggested to
prepare nanofluids for meeting the needs of foam-free coolants.
The methods utilized for improving the stability make a graphene-
based nanofluid stable for only some days or months. Hence, applying
superior changes on the surface of graphene sheets based on advanced
research in the future can be effective to reach more stable nanofluids
with longer stability time.
Thermal conductivity of functionalized graphene nanoplatelets is
lower than that of pristine graphene ones. This is because the functional
groups decrease thermal conductivity, which is attributed to structural
disturbance and mass impact. Furthermore, acid chemical functionali-
zation can damage graphene sheets structure and even rupture them.
Also, based on the new studies, the carboxylic group is one of the chief
causes of corrosion in engineering devices. These important factors
should be considered in future studies with more attention.
5. Different surfactants used in graphene-based nanofluids
As stated before, graphene is hydrophobic and thus cannot be sus-
pended in polar liquids. It simply settles and agglomerates when is
added to fluids like water. Using surfactants (i.e., surface active agents)
for surface functionalization to improve the chemical compatibility of
graphene sheets with base fluids can enhance their wetting or adhesion
features and decrease the tendency to agglomerate. Stabilization with
the use of surfactants can be performed through the two mechanisms:
electrostatic stabilization by employing ionic surfactants as well as
steric stabilization via nonionic ones. Each graphene nanosheet coated
with surfactants resists against aggregation owing to the existence of
repulsion between neighbor surfactant-coated sheets.
According to head composition, surfactants can be categorized into
three groups including nonionic surfactants without charge groups in
the head, anionic surfactants having negatively charged head groups,
and cationic ones having positively charged head groups. It should be
noted that stabilization of suspensions through ionic surfactants is
achieved from electrostatic repulsion among ionic hydrophilic heads
which exist on neighbor graphene platelets. Indeed, the formation of
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Energy Conversion and Management 196 (2019) 1222–1256
electrical double layers including surfactant molecules adsorbed onto
graphene platelets, and a diffuse layer of counter ions causes electro-
static repulsions, which are adequately robust to overcome van der
Waals attractions among graphene sheets.
In this regard, as mentioned, surfactants can be utilized for non-
covalent functionalization of graphene sheets. Different surfactants
have been employed for this purpose to reach stable nanofluids.
Mahmudul Haque et al. [116] carried out experimental work on
preparing the graphene and MWCNT based nanofluids with the aid of
SDBS and SDS surfactants. The nanofluids prepared with both surfac-
tants showed proper stability. It was also revealed that the SDBS is an
appropriate surfactant for MWCNTs, while the SDS is suitable for gra-
phene sheets.
Ahammed et al. [143] evaluated the influence of temperature and
volume fraction on the surface tension of a water–graphene nanofluid
in which the SDBS was employed as the surfactant. The surface tension
reduced by the increase of either temperature or volume fraction. The
authors claimed that this reduction at greater volume fractions is be-
cause of the adsorption of nanoparticles at the gas-liquid interface,
while at greater temperatures, it is because of the weakening of mole-
cular attractions between the nanoparticles and fluid molecules.
Shazali et al. [144] assessed the stability of GNPs inside a nanofluid
in the case of using Pluronic P-123 as the surfactant in comparison with
other conventional surfactants including SDS, CTAB and Triton X-100
(TX). The Pluronic P-123, as a novel surfactant, demonstrated the best
stability. Additionally, the CTAB, SDS, and TX surfactants led to the
formation of excessive foam, whereas Pluronic P-123 did not cause any
foam formation.
Selvam et al. [145] reported the thermal conductivity of water and
ethylene glycol containing GNPs. Sodium deoxycholate was employed
as the surfactant. The results revealed that despite the great thermal
conductivity of graphene sheets, interfacial thermal resistance between
the graphene sheets and base liquid restricts the thermal conductivity
increment considerably.
Jia et al. [146] synthesized graphene–water nanofluids with and
without carboxyl methyl cellulose (CMC) surfactant. The surfactant
varied the zeta potential and therefore, resulted in the stable nano-
fluids. The prepared nanofluid then froze with and without an external
electromagnetic field and melted at room temperature. Mechanisms
related to the electromagnetic field, surfactant adsorption, and possible
gas evolution were suggested for explaining the behavior of graphene
sheets in front of the water–ice interface.
To evaluate the influence of ionic and non-ionic surfactants on the
stability of graphene-based nanofluids, Uddin et al. [147] utilized
SDBS, SDS, and Triton X-100 surfactants in preparing the nanofluids.
The stability of SDBS functionalized graphene sheets was best in the
water at 1.5 mg ml−1. The results also showed that the surfactants do
not prevent GO reduction. The thickness of functionalized graphene
sheets varied considerably with the change of the surfactant type.
Jia et al. [148] employed SDS and CMC as the surfactants to syn-
thesize the water–graphene nanofluids. The results indicated that the
dispersion of the nanofluid without surfactant was significantly de-
graded, whereas the nanofluids with surfactant showed rather appro-
priate dispersion.
In general, surfactants are utilized to improve the stability of na-
noparticles in suspensions, while their poor thermal conductivities
make a restriction for utilization in nanofluids. This issue should be
assessed carefully in future studies. Moreover, employing a specific
ratio of surfactants in preparing nanofluids can be very crucial to reach
optimal dispersion of graphene sheets. In addition, the process of dis-
persing graphene sheets in liquids with the use of surfactants followed
by centrifugation for isolating well-suspended components can be ap-
propriate only for small scales. Indeed, it may not be proper for large
scales since such techniques cause wastage of significant amounts of
graphene sheets. Meanwhile, surfactants may not be appropriate for
lubricants because they would not meet viscosity criteria. In reality,
M. Bahiraei and S. Heshmatian Energy Conversion and Management 196 (2019) 1222–1256

although mineral oils are usually non-polar, graphene sheets are not
adequately hydrophobic to create uniform suspensions.
Additionally, although gum Arabic surfactant can result in a more
appropriate state for dispersing graphene sheets compared to Triton X-
100 and SDBS surfactants, it considerably intensifies viscosity of sus-
pensions, which can lead to issues such as increment of pumping power
in heat transfer devices.
In the future, simulations based on molecular dynamics can disclose
molecular mechanisms of adsorption morphology of dispersants, and
determine the interaction energy between graphene sheets modified via
surfactants.
6. Wettability and contact angle
The capability of fluid to hold its contact with a solid surface is
termed wettability. The surface forces, including the adhesive and co-
hesive forces, control the wettability level on various solid surfaces.
Wettability is one significant factor, particularly in evaluating hydro-
thermal characteristics of multiphase flows in practical situations. The
adhesive force leads to spreading fluid droplets on the surface. On the
contrary, liquid droplets resist against contact with solid surface thanks
to cohesive force. To determine the wettability, the contact angle is
calculated, which indicates the wetting grade of liquids. Thereby,
contact angles with values of greater than 90° mean lower wetting
while those with values of less than 90° show higher wetting of liquids.
It is noteworthy that wettability plays a key role in applications such as
boiling heat transfer, and the presence of the nanoparticles can affect
this characteristic. As a result, some of the researchers have in-
vestigated the wettability and contact angle for nanofluids containing
graphene-based nanomaterials.
Askari et al. [149] prepared the graphene-Fe3O4 hybrid nanofluids
and investigated their wettability. Fig. 15 displays the preparation
method of the hybrid graphene-Fe3O4 nanoparticles. The contact angle
decreased with the increase of the concentration. Thereby, on the
copper surface, the contact angle for the base fluid was 99.3° whereas,
for the nanofluid, it reduced to 93.6°, 92.1° and 90.4° at concentrations
of 0.1, 0.3 and 0.5 wt%, respectively.
Kamatchi et al. [150] synthesized a water-based rGO nanofluid and
showed that the surface tension of the nanofluid is dependent on the
temperature and concentration. Investigation of the wettability also
revealed an increase of the contact angle by the concentration incre-
ment.
Park et al. [118] used the graphene and graphene oxide sheets in
preparing the nanofluids. The results indicated that the contact angle
for the graphene nanofluid and GO nanofluid is greater than that for the
pure water. Finally, the authors mentioned that unlike common nano-
fluids, it is very difficult to interpret the increased critical heat flux
(CHF) of graphene and GO nanofluids through the capillarity and sur-
face wettability.
Lee et al. [105] examined the flow boiling CHF for a GO-water
nanofluid. It was shown that the CHF of the nanofluid is greater than
that of the water. Increment in the CHF was because of the increased
wettability of the liquid film on the heating surface due to the deposi-
tion of the graphene oxide nanosheets. It is noteworthy that the en-
hanced wetting and surface deposition structures in this study had not
consistency with results of their previous paper [118] on pool boiling
CHF with the graphene oxide nanofluids. The enhanced wettability in
[105] can be because of the fact that the graphene oxide sheets may not
be chemically converted into rGO during the process whereas the de-
creased wettability in the previous research [118] can be certified by
the fact that the graphene oxide sheets may be chemically converted
into rGO during the nucleate boiling.
Sarsam et al. [151] prepared a nanofluid containing triethanola-
mine-treated graphene nanoplatelets and measured the contact angle
on a glass surface. A reduction in the contact angle was seen from 50.7°
for the pure water to almost 47.1°–47.9° for the nanofluids. The contact
angle reduction means an increment of the surface wettability, which
can cause heat transfer enhancement. In some studies [152], it is
mentioned that greater viscosity is related to lower contact angle. Ac-
cordingly, the viscosity of the nanofluids in this work [151] was higher
than that of the water.
Singh et al. [153] synthesized a hybrid nanofluid through com-
bining the Al2O3 based nanofluid with the GNPs. The hybrid nanofluid
demonstrated a superior wettability in comparison with either Al2O3

Fig. 15. Preparation of hybrid graphene-Fe3O4 [149]. Reprinted with permission from Elsevier.

1237
M. Bahiraei and S. Heshmatian
based nanofluid or base fluid. Moreover, the Al2O3–GNP nanofluid in-
dicated a smaller contact angle compared with the Al2O3 nanofluid and
base fluid.
The abovementioned studies show some contradictions between the
reported results about the wettability and contact angle of graphene-
based nanofluids. For instance, Askari et al. [149] stated that the con-
tact angle reduces with the increase of the concentration, whereas
Kamatchi et al. [150] reported a contact angle increment with in-
creasing the concentration. As a consequence, new studies in this field
need to be further performed to establish an accepted trend about
changes of the contact angle in nanofluids including graphene sheets.
7. Thermophysical properties of graphene-based nanofluids
Due to the noticeable importance of thermophysical properties in
hydraulic and thermal applications of graphene-based nanofluids, the
studies carried out in this area are reviewed and discussed in this sec-
tion. In fact, these properties are needed in either numerical evaluations
or experimental studies. It should be noted that in nanofluids, graphene
sheets––because of their great surface area-can result in different
thermophysical properties in comparison with other nanoparticle types.
For example, a graphene sheet has higher contact area with base fluid
and hence, the contact resistance at graphene sheet–liquid interface will
be decreased considerably. Moreover, graphene appears to be a strictly
2D material, which demonstrates a high crystal quality in which elec-
trons can move submicron lengths without scattering.
Balandin et al. [154] measured the thermal conductivity of a sus-
pended single-layer graphene. They employed a new method for the
noncontact measurement of the thermal conductivity of graphene with
use of the confocal micro-Raman spectroscopy. Based on the depen-
dence of the Raman G peak frequency on the excitation laser power and
independently measured G peak temperature coefficient, the thermal
conductivity was obtained up to 5300 W/mK. The authors stated that
graphene sheets have a higher thermal conductivity than carbon na-
notubes. Superior thermal conductivity of graphene can be because of
the lower Gruneisen parameter for the pertinent phonon modes as es-
timated from the first-principle evaluations [155].
Yarmand et al. [156] synthesized the functionalized GNP nanofluids
through a simple method. The results indicated the significant incre-
ment in the thermal conductivity of the nanofluids compared with the
base fluid. The increment percentage was dependent on the tempera-
ture and concentration. Moreover, the viscosity and density were
greater than those of the water. In addition, the specific heat reduced by
increasing the concentration.
Yarmand et al. [157] prepared a mixture of empty fruit bunch fiber
as the matrix material and GO sheets as the additive which was acti-
vated through KOH. Thereafter, the as-synthesized hybrid containing
activate carbon/graphene (ACG) was suspended in EG. The thermal
conductivity of the ACG–EG nanofluid demonstrated an increment of
6.47% at weight concentration of 0.06%. Additionally, the electrical
conductivity of the nanofluid showed a substantial increase.
Chen et al. [158] assessed the thermophysical properties, optical
absorption feature as well as the photo-thermal conversion performance
of the water–GO nanofluids. A significant increase in the optical ab-
sorption property and thermal conductivity was perceived for the na-
nofluid compared with the water. Besides, the photo-thermal conver-
sion performance of the nanofluids was greater than that of the base
fluid.
Yu et al. [127] introduced a facile method for preparing EG-based
nanofluids including graphene and GO sheets. The thermal conductivity
of the EG increased considerably up to 86% with dispersing the na-
nosheets. The thermal conductivity of the GO nanofluid and graphene
nanofluid were approximately 4.9 W/mK and 6.8 W/mK, respectively.
Lee and Rhee [159] produced EG-based nanofluids containing
GNPs. The nanoplatelets demonstrated an invariant magnitude of the
thermal conductivity increment at concentration of 2% and the
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Energy Conversion and Management 196 (2019) 1222–1256
temperature range of 10–90 °C. Also, the thermal conductivity of the
nanofluids was much greater than the theoretical values based on the
Hamilton-Crosser model, which can be because of greater surface area
and 2D structure of the graphene nanoplatelets.
Yudong et al. [160] synthesized the GO nanofluids with suspending
graphene oxide sheets into the water, and the nucleation tests were
performed with the levitated deionized water and GO nanofluid drops.
The outcomes revealed that the supercooling degree of the nanofluid
drop is considerably lower than that of the water drop. In addition, the
nucleation of the levitated water drops was frequently surface-domi-
nated, while that of the levitated nanofluid drops was both surface-
dominated and volume-dominated.
Akhavan-Zanjani et al. [125] measured the thermal conductivity
and viscosity of a water–graphene sheet nanofluid. The findings re-
vealed significant increment in the thermal conductivity and moderate
increase in the viscosity by adding small amounts of the graphene na-
nosheets. The highest enhancements were 4.95% and 10.30% for the
viscosity and thermal conductivity, respectively.
Eswaraiah et al. [161] synthesized very thin graphene sheets
through exfoliating graphite oxide on the basis of concentrated solar
radiation. They prepared the graphene sheets–engine oil nanofluids,
and determined their antiwear (AW), frictional characteristics (FC) as
well as extreme pressure (EP) features. The enhancements in FC, AW,
and EP of the nanofluid were almost 80, 33, and 40% in comparison
with the base fluid.
Iranmanesh et al. [162] evaluated the effects of temperature and
concentration on the thermal conductivity and viscosity of the gra-
phene nanoplatelets nanofluids. The outcomes indicated that the con-
centration directly affects the thermal conductivity and viscosity. It was
also shown that the temperature has the more important effect on the
viscosity in comparison with the other factors.
Liu et al. [121] studied the specific heat, thermal conductivity,
viscosity and density of the graphene sheets nanofluids based on an
ionic liquid. Compared with the base fluid, the thermal conductivity of
the nanofluid at concentration of 0.06 wt% enhanced by 15.2%–22.9%
when the temperature was changed from 25 to 200 °C. The nanofluid
viscosity significantly reduced with the temperature increment. More-
over, the density and specific heat of the nanofluid reduced slightly in
comparison with those of the base fluid.
Moghaddam et al. [117] synthesized high quality few-layer gra-
phene sheets via burning magnesium metal in dry ice. The authors
measured the viscosity of the nanofluids containing these graphene
sheets, and reported increase of the viscosity with increasing the mass
fraction and decrease of the viscosity with the temperature increment.
Zhang et al. [163] utilized three different nanoparticles including
graphene sheets, graphite nanoparticles and single-wall carbon nano-
tubes to synthesize the ionic liquid-based nanofluids. All the nanofluids
demonstrated greater thermal conductivity and lower viscosity in
comparison with the base fluid. The nanofluid having graphene sheets
had the greatest thermal conductivity increment compared with the
two other nanofluids. Additionally, the graphene-based nanofluid
showed the smallest transmittance, maximum extinction factor and
greatest photo-thermal conversion efficiency.
Park and Kim [110] experimentally studied the changes of the
viscosity and thermal conductivity of three types of water-based gra-
phene sheets nanofluids including those with the oxidized graphene
sheets and graphene sheets at two different sizes. The increment rate of
the thermal conductivity for the nanofluid containing the oxidized
graphene sheets was highest among the three nanofluids, while that of
the viscosity was maximum for the nanofluid containing the graphene
sheets with the larger size.
In addition to the above reviewed studies, some of scholars have
considered graphene-based nanofluids as non-Newtonian fluids, and
have examined their rheological attributes. Tesfai et al. [164] evaluated
the rheological features and intrinsic viscosity of the suspensions
having GO sheets. The dilute suspension showed a shear thinning
M. Bahiraei and S. Heshmatian
Fig. 16. Optical microscopic images of nanoporous graphene nanohybrid Pickering emulsions [165]. Reprinted with permission from Elsevier.
behavior at small shear rates followed by a shear-independent region.
The shear thinning behavior became more noticeable by increasing the
concentration. The nanofluid also had a great intrinsic viscosity because
of the high aspect ratio of the GO sheets.
AfzaliTabar et al. [165] assessed the influence of the nanoporous
graphene–silica nanohybrid particles on the rheological features of
xanthan gum (XG) suspension. It was found that these suspensions are
shear thinning fluids. The viscosity reduction in the case of nanoporous
graphene–SiO2 nanohybrid/XG suspension was lower than that in the
case of XG suspension. The results also indicated that the nanoporous
graphene-SiO2 nanohybrid enhances the rheological characteristics of
the XG suspension. Fig. 16 shows the optical microscopic images of
nanoporous graphene nanohybrid.
Chai et al. [166] researched the rheological attributes of a graphene
sheets–hydrogenated oil nanofluid to be utilized as drilling fluid. With
increment of the concentration up to the maximum value, the shear
stress and viscosity increased up to 33% at temperature of 30 °C. It was
also shown that the Bingham model is fitted well with the rheological
data achieved in this work.
Rabbani Esfahani et al. [167] produced the water-based GO nano-
fluids, and showed that they have the non-Newtonian behavior (shear
thinning) at lower shear rates. The results revealed that the viscosity
increases linearly with the concentration increment from 0.01 to 0.1 wt
%, while a sharp increment was noticed with increase of the con-
centration to 0.5 wt%.
Ho et al. [168] experimentally studied the rheological character-
istics of the hydrogenated drilling fluid–graphene sheets nanofluids. It
was found that the graphene/oil-based drilling fluid has higher visc-
osity than the base fluid at the shear rates between 0 and 140 s−1, and it
behaves similar to Bingham fluids. The thickening behavior of the na-
nofluid was attributed to the agglomerating the graphene sheets.
In an experimental work, Ijam et al. [169] investigated the viscosity
of a GO sheets–water/EG nanofluid. The nanofluid demonstrated a
shear thinning attribute at small shear rates, and a Newtonian behavior
at great shear rates. The viscosity of the nanofluid intensifies by 35% in
comparison with the base fluid at a weight concentration of 0.1% and a
temperature of 20 °C.
In most of the studies conducted on nanofluids, the transient hot-
wire method, parallel plate method, and 3ω method have frequently
been employed for measuring thermal conductivity. However, the
transient hot-wire method has been considerably utilized for graphene-
based nanofluids due to its reliability in the measurement of thermal
conductivity.
The Klemens theory [170] indicated that the thermal conductivity
in graphene has logarithmic divergence with the layer or grain size,
which is presented as follows:
υ4 ⎞ ⎛ fm ⎞
k = (2πγ 2)−1ρm ⎜⎛ ⎟ ln ⎜ ⎟
⎝ fm T ⎠ ⎝ fB ⎠ (1)
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1/2
Mυ3fm ⎞
fB = ⎜⎛ 2
⎟
⎝ 4πγ kB TL ⎠ (2)
in which fm represents the upper limit of the phonon frequencies in-
troduced through the phonon dispersion, M indicates the mass of an
atom, υ is the mean phonon group velocity, γ represents the Gruneisen
parameter, and fB denotes the size-dependent low-bound cut-off fre-
quency for acoustic phonons, defined by limiting the phonon mean-free
path with the graphene layer size L.
Based on the review carried out in this part, it is found that nano-
fluids containing graphene nanomaterials frequently have higher
thermal conductivity and viscosity compared with those including
other nanoparticles. In fact, in addition to unique properties of gra-
phene-family materials, the plate shape of these materials is also a very
effective cause. It is noteworthy that a graphene sheet is prone to get-
ting folded, coiled, and corrugated at the surface and edges. This can
affect energy transmit mechanisms and so, thermal conductivity models
developed for a specific shape may not be capable of predicting the
actual mechanisms in other nanoparticle shapes. In fact, most of the
models have been derived for elongated or spherical shape nano-
particles and therefore, novel models should be developed for pre-
dicting thermophysical properties of graphene-based nanofluids.
Indeed, there is not any comprehensive and effective outcome about
thermophysical properties of these nanofluids. For instance, in gra-
phene and GO nanofluids, most of the studies have reported that
thermal conductivity is temperature dependent, whereas Sun et al.
[106] and Yu et al. [127] indicated the inconsistent results. Such a
temperature independency has also been reported for other nano-
particle types such as CNT [171] and Al2O3 [172]. Moreover, although
it is expected that increment rate of thermal conductivity for graphene
nanofluids is higher than that for GO nanofluids, Park and Kim [110]
stated that the thermal conductivity enhancement rate is greater for GO
nanofluids compared to graphene nanofluids. As a result, more theo-
retical and experimental studies should be carried out in the future to
accurately uncover governing mechanisms.
In addition, the defects in graphene sheets can influence the ther-
mophysical properties of nanofluids. The impacts of defects on nano-
fluid properties are not obviously known. The characterization methods
can be efficient for disclosing unknown details about graphene defect
influences on the nanofluid thermophysical properties.
Generally, size of graphene sheets is not uniform and planar shape
of sheets does not remain invariant after dispersing them in base fluids.
These specific factors have been frequently ignored while they can
explain the effective mechanisms. Besides, when graphene sheets are
exposed to shear forces, they experience rippling, buckling, exfoliation,
puckering, and even rupture. Therefore, combination of multiple me-
chanisms can be able to clarify the improved thermophysical properties
in graphene-based nanofluids. Characterizing graphene sheets after
dispersing them into base fluids is also pivotal because it can indicate
scrolling and corrugation of graphene plates, which are inevitable for
M. Bahiraei and S. Heshmatian Energy Conversion and Management 196 (2019) 1222–1256

Fig. 17. AFM and TEM photos of graphene plates: (a) bar 0.5 μm; (b) bar 200 nm, graphene wave in the middle; (c) bar 100 nm, graphene coiled at the edge; (d)
HRTEM photo of the graphene; (e) a tapping mode AFM photo of graphene plates, (f) the height profiles in chosen place [173]. Reprinted with permission from
Elsevier.

the 2D materials. As per Fig. 17, graphene gets corrugated, folded, and
coiled at both the edges and middle of its plates [173]. It should be
noted that the defects not only influence the thermal conductivity of
graphene but also several other characteristics.
In reality, presence of some contradictions between reported results
on thermophysical properties of graphene-based nanofluids is rather
reasonable, because a more thorough understanding is required for
relationship among the nanofluid properties and parameters such as
particle size, concentration, rheological behavior, stability, aspect ratio
of graphene sheets, PH, temperature, and so on. Meanwhile, the
synthesis technique of the graphene family sheets is a very important
factor. In the future, all the mentioned parameters should be taken into
account to reach exact predictor models.
As a crucial point, in case of using surfactants, the trace of surfactant
molecules absorbed on the surface of graphene sheets might con-
siderably promote phonon scattering, and it negatively affects the
thermal conductivity of graphene materials.
Most of the experimental studies have been conducted in room
temperature, while concerning the diverse applications of graphene-
based nanofluids, evaluating thermophysical properties of these

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M. Bahiraei and S. Heshmatian
Fig. 18. Preparation method of graphene ferromagnetic nanofluid [180]. Reprinted with permission from Elsevier.
nanofluids at temperatures above and below ambient conditions is also
very critical.
Finally, it can be mentioned that studies on the electrical con-
ductivity of nanofluids containing graphene nanomaterials is very
sparse, whereas electrical features play key roles in many of applica-
tions of graphene-based nanofluids. Indeed, carbon atoms have highly-
mobile electrons, which are termed π electrons and are located above
and below graphene plates. In graphene materials, the π orbitals
overlap and aid to augment the carbon-carbon bonds. Essentially, the
electronic features of graphene are established by the bonding and anti-
bonding of these π orbitals [59]. Besides, the superb high room tem-
perature carrier mobility, possibilities of induction of a band gap by the
lateral quantum confinement, conductance quantization, and feasibility
for epitaxial growth make graphene a potential material for future
electronic circuits. Furthermore, a more significant attention should be
paid to optical properties of these nanofluids to be utilized in solar
thermal applications.
8. Convective heat transfer
In addition to thermophysical properties, the nanofluid character-
istics under flow conditions are also essential. In fact, in most of im-
portant applications of graphene-based nanofluids, fluids move in re-
levant geometries and hence, their features in such states should be
examined thoroughly. In this regard, natural and forced convection
heat transfer problems of these nanofluids have been investigated by
several scholars.
Joshi and Pattamatta [174] carried out an experimental research to
study the natural convection heat transfer in a cavity by various kinds
of nanofluids including the Al2O3–water, MWCNT–water and graphe-
ne–water. An increment in natural convection heat transfer was
achieved by the MWCNT–water and graphene–water nanofluids at
concentration of 0.1%, while a decrement was perceived at the greater
volume fractions. The Nusselt number enhanced almost 19% and 5%
for the graphene–water nanofluid at concentrations of 0.1% and 0.3%
in comparison with the water, respectively.
Mehrali et al. [175] experimentally evaluated the convective heat
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Energy Conversion and Management 196 (2019) 1222–1256
transfer coefficient of the GNPs nanofluid flow within a horizontal pipe.
The convective heat transfer coefficient of the nanofluid was greater
than that of the base fluid by about 83–200%. Moreover, the heat
transfer coefficient enhanced by increasing either the flow rate or
specific surface area.
Akhavan-Zanjani et al. [176] studied the convection heat transfer of
a water–graphene nanofluid in a circular tube. The results revealed that
adding small amount of the graphene nanosheets to the base fluid en-
hances the convection heat transfer coefficient noticeably. The highest
increment in the convection heat transfer coefficient was 14.2%, which
occurred at Reynolds number of 1850 and concentration of 0.02%.
Bahiraei and Mazaheri [177] researched the thermohydraulic fea-
tures of a hybrid nanofluid containing GNPs coated with platinum na-
noparticles inside a chaotic minichannel. The pumping power and
convective heat transfer intensified with increase of either Dean
number or concentration. Figure of merit, which is ratio of increment in
convective hear transfer to increment in pumping power in the condi-
tion of using the chaotic channel, was larger than 1.5.
Naghash et al. [178] examined the convection heat transfer coeffi-
cient of nanofluids synthesized from nanoporous graphene sheets. The
nanofluid thermal conductivity at 0.1% concentration remained rather
invariant, with only 3.8% increment, whereas the convection heat
transfer coefficient enhanced profoundly, with 34% increment.
Bahiraei et al. [179] studied hydrothermal characteristics of a green
graphene-based nanofluid inside a spiral heat exchanger. By increase of
the Reynolds number or concentration, the overall heat transfer coef-
ficient and heat transfer rate enhanced. Moreover, the pressure loss
increased by increasing the Reynolds number, and the nanofluid
showed a higher pressure loss compared with the water particularly at
greater Reynolds numbers.
Sadeghinezhad et al. [180] experimentally researched the influence
of a permanent magnetic field on the convective heat transfer of a
graphene–magnetite hybrid nanofluid. The preparation method of
graphene ferromagnetic nanofluid is shown in Fig. 18. The convection
heat transfer considerably enhanced under the effect of the magnetic
field. However, the heat transfer increase of the nanofluid compared
with the base liquid was minor when the magnetic field was not
M. Bahiraei and S. Heshmatian
Fig. 19. Temperature contours at various pumping power values and concentrations [181]. Reprinted with permission from Elsevier.
applied.
Bahiraei and Heshmatian [181] evaluated the hydrothermal attri-
butes and second law features of a hybrid nanofluid having graphe-
ne–Ag nanoparticles in two microchannel liquid blocks. With increase
in concentration or velocity, the surface temperature decreased and
uniformity of the cooling enhanced. The findings also indicated that the
friction has a lower contribution in the entropy generation in compar-
ison with the heat transfer. Fig. 19 illustrates the temperature contours
obtained in this research at various pumping power values and con-
centrations.
It can be mentioned that the majority of the studies carried out on
convective heat transfer of graphene-based nanofluids have focused on
forced convection, and very few investigations have been conducted on
natural convection in this area. Natural convection heat transfer of
graphene-family nanofluids can have many applications in different
industrial sectors such as microelectronics and MEMS, solar collectors,
nuclear reactors, and so on. Accordingly, much more efforts should be
made in this field in future investigations.
Some researchers have stated that enhancement of convective heat
transfer in graphene-based nanofluids is greater than thermal con-
ductivity increment. For instance, Baby and Ramaprabhu [100] men-
tioned that increment of the Nusselt number is higher than that of the
thermal conductivity. Moreover, Naghash et al. [178] presented a much
higher enhancement in convective heat transfer coefficient compared
with thermal conductivity increment. This certifies that in addition to
thermal conductivity enhancement, more mechanisms affect convec-
tion heat transfer of graphene-based nanofluids, which should be un-
derstood in the future research. For example, local order of base fluid
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Energy Conversion and Management 196 (2019) 1222–1256
molecules in vicinity of graphene sheets, parallel structure as well as
the potential π–π stacking can be effective mechanisms to clarify the
reasons of great heat transfer enhancement in graphene family nano-
fluids.
According to the performed evaluations, identification of a re-
cognized theory to exactly predict the convection heat transfer attri-
butes of nanofluids containing graphene materials is complex. In the
numerical studies, most of the papers have employed the single-phase
simulation that assumes nanofluids as homogenous fluids. More atten-
tion should be given to two-phase approaches to numerically simulate
graphene-based nanofluids because graphene sheets can possess a
macroscale transverse size that may cause significant errors in the case
of using homogenous methods. Indeed, with utilizing two-phase ap-
proaches, interactions between base fluids and graphene sheets are
considered, which may have profound effects on convection heat
transfer of these nanofluids.
Nanofluids with graphene sheets frequently possess superior con-
vective heat transfer compared with those containing GO sheets. In fact,
graphene oxide sheets include sp2-hybridized carbon atoms and sp3-
hybridized carbons bearing epoxide and hydroxyl groups. The existence
of oxygen atoms as well as saturated sp3 bonds in GO sheets reduces
thermal conductivity, promotes phonon scattering, and weakens con-
vection heat transfer of nanofluids in comparison with graphene sheets.
Generally, using graphene-family nanomaterials in nanofluids can
enhance thermal attributes and energy performance of heat transfer
equipment and therefore, size of devices such as heat exchangers de-
creases, which results in enhanced reliability, less pollution as well as
higher efficiency.
M. Bahiraei and S. Heshmatian
9. Boiling heat transfer
Boiling and its improvement have always been topics of interest in
the thermal engineering. In the recent two decades, a novel item has
been added to this conventional field due to growth of nanotechnology.
Employing different nanofluids, as new suspensions for boiling im-
provement, has attracted significant attention. Many experimental in-
vestigations on this subject have shown that modification of surface
properties owing to deposition of nanoparticles is the main reason of
pool boiling increment by nanofluids. Consequently, this fact can be
taken into account as a passive technique to reach boiling heat transfer
enhancement. Because of the passive nature of this method, the mod-
ification of surface properties including roughness and wettability can
be dependent on the shape, material, size, and loading of nanoparticles
as well as initial features of surfaces. Due to major effects of nanofluids
on boiling heat transfer, some studies have been carried out on nano-
fluids containing graphene-family nanomaterials to evaluate their
boiling characteristics.
Fan et al. [182] investigated transient pool boiling through
quenching of stainless steel spheres in GO nanofluids. The quenching
was augmented with increase in the concentration, which was attrib-
uted to the altered surface features such as the wettability, morphology
as well as roughness. In contrast to the outcomes reported in most of the
other relevant papers that imply surface wettability modification, the
main reason of CHF increment in this study was the surface roughness
intensification, which facilitated fluid–solid interactions.
Hu et al. [183] studied pool boiling features including the CHF and
boiling heat transfer coefficient (HTC) for a graphene sheets–EG/water
nanofluid. It was found that at small concentrations, the boiling per-
formance enhances with the concentration increment, which is due to
the surface wettability increment because of nanoparticles deposition.
However, more increase in the concentration decreased the HTC thanks
to the graphene sheets sedimentation as well as consequent blockage of
the nucleation sites. In addition, at the graphene loadings lower than
0.02%, the CHF quickly enhanced by the increment of the concentra-
tion.
Zhang et al. [184] experimentally assessed quenching with copper
spheres to determine the transient pool boiling of a GO nanofluid. The
trend of the CHF changes in terms of the concentration was ascending
and changed non-uniformly. Such a non-uniform trend was consistent
with the variations of the surface wettability caused by deposition of
the graphene oxide sheets after the quenching. The significant effect of
the dispersed GO sheets was also obvious at greater loadings.
Zhang et al. [185] employed the GO–water nanofluid for performing
the flow boiling experiments in microchannels. The heat transfer per-
formance decreased with the increase of the concentration. The surface
deposition was seen after the experimental tests. The authors argued
that the deposition process is augmented by increasing each of the
parameters of flow rate, temperature, and concentration.
As seen, different scholars have reported different results about the
changes of boiling heat transfer in nanofluids containing graphene
materials. In some of the studies, it is stated that the boiling heat
transfer is augmented with the concentration increment, while in some
other papers, a reduction in billing heat transfer by an increase of the
concentration is noticed. Moreover, some researchers have observed the
optimal points for boiling performance, namely at first, boiling heat
transfer enhances with the concentration increase and then, decreases
with more increment in the concentration. Such observations are de-
pendent on the concentration range under study. It means that at rather
small concentrations, the nanoparticles can enhance the wettability and
can also create a porous-like structure of deposition on heating surfaces.
This improves nucleation sites and consequently boiling performance at
these graphene loadings. However, at rather high concentrations, the
film-like shape of graphene sheets develops a nonporous structure of
deposition on surfaces, which can degrade nucleation sites and there-
fore diminish boiling performance.
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Energy Conversion and Management 196 (2019) 1222–1256
In addition, a critical need is felt to derive new correlations or im-
prove the common models for prediction of boiling attributes such as
CHF and boiling heat transfer coefficient as a function of effective
parameters for graphene-based nanofluids. For instance, Park et al.
[118] proved that increment in the CHF of GO and graphene sheets
nanofluids could not be predicted via the enhanced wettability and
capillarity of nanoparticles deposition film.
Generally speaking, the precise impacts of graphene-based nano-
fluids on boiling characteristics are not evident. Hence, it is suggested
to perform more studies for evaluating the parameters related to boiling
in these nanofluids under different states. Additionally, majority of the
papers in this area are about pool boiling in static systems, while flow
boiling is also very important in applications related to nanofluids.
10. Hydrodynamic characteristics
In addition to the thermal attributes, hydrodynamic characteristics
such as pressure drop and pumping power are also important in devices
in which a fluid flows for purpose of heat transfer. Indeed, a suitable
thermal system must possess low pumping power along with high heat
transfer rate. This fact becomes especially important for nanofluids in
which in addition to heat transfer enhancement, viscosity of base fluids
also intensifies by adding nanoparticles, which can increase pumping
power. As a consequence, several studies have concentrated on the
hydrodynamic features of graphene-based nanofluids.
Sadeghinezhad et al. [186] evaluated the pressure drop and
pumping power of the GNPs nanofluids inside a horizontal pipe. The
results revealed that the pressure loss intensifies 0.4% to 14.6% com-
pared with the base fluid. The authors also mentioned that this nano-
fluid has a small pumping power penalty.
Amiri et al. [187] employed single-layer graphene (Fig. 20) to
prepare the nanofluids, and examined their thermal and hydraulic at-
tributes over a backward facing step. The pressure drop increased by
increasing either Reynolds number or concentration, while the nano-
fluid pressure drop was very close to the base fluid. In addition, the
pressure loss became smaller than heat transfer increment at weight
concentrations higher than 0.005%.
Bahiraei et al. [188] investigated the pressure drop, pumping power
and thermal characteristics of a GNP/silver–water hybrid nanofluid
within a microchannel heat sink fitted with the secondary channels and
ribs. The secondary channels resulted in the flow area increase, which
decreased the pressure loss. It was found that combining the three
methods, i.e. use of the nanofluid, secondary channels and ribs, en-
hances the heat sink efficiency considerably. Furthermore, the flow
demonstrated a higher pumping power and pressure drop for greater
concentrations and Reynolds numbers (see Fig. 21).
Amiri et al. [189] carried out an experimental research on the
friction coefficient and thermal features of a GNP–EG nanofluid over a
backward facing step. The friction coefficient was not dependent on the
weight fraction. Meanwhile, with considering both pressure loss and
Nusselt number increment, the maximum performance index occurred
at weight concentration of 0.05%.
Azizi et al. [190] assessed the influence of a water–graphene na-
nofluid on the thermal efficiency and pressure drop of a Two-Phase
Closed Thermosyphon (TPCT). The vacuum pressure data indicated that
increase of the concentration intensifies the vacuum pressure loss. The
results also showed that when the concentration increases, the thermal
performance and overall heat transfer coefficient enhance.
Selvam et al. [191] studied the pressure drop and convection heat
transfer of a water/EG–GNP nanofluid in a double-pipe heat exchanger.
The pressure drop increase was predominant in the laminar region,
while it was moderate in the turbulent region. Besides, the convection
heat transfer enhanced by increasing each of the parameters of con-
centration, Reynolds number as well as inlet temperature.
Solangi et al. [192] investigated the hydrodynamic and thermal
features of the GNP–water nanofluid in a cooper tube. Both friction
M. Bahiraei and S. Heshmatian
Fig. 20. (a−d) TEM images, (e−h) FESEM images of single layer graphene [187]. Reprinted with permission from Elsevier.
factor and Nusselt number increased with increment in the Reynolds
number and volume fraction. The friction factor of the nanofluid in-
tensified by 4%–14% in comparison with the water. Moreover, a minor
increment in the pumping power occurred in terms of the concentra-
tion.
Most of the research studies carried out on hydrodynamic char-
acteristics of graphene-based nanofluids are experimental, and few of
them have modeled these nanofluids numerically. According to the fact
that the non-Newtonian behavior of graphene-based nanofluids can
have significant effects on friction and pressure drop, it is vital to
evaluate these nanofluids with considering dependency of viscosity on
the shear rate in future numerical studies specifically for high con-
centrations. Furthermore, more comprehensive investigations with
employing TEM, DLS, XPS, SEM, and AFM are recommended to better
understand the interactions between contact surfaces and graphene
sheets, which influence frictional attributes of nanofluids. Besides, es-
sential issues such as the number of layers of graphene, twisting,
puckering, exfoliation, and bending should be regarded concurrently
Fig. 21. Contours of pressure at: (a) Re = 300 and φ = 0, (b) Re = 300 and φ = 0.1%, (c) Re = 500 and φ = 0 and (d) Re = 500 and φ = 0.1% [188]. Reprinted
with permission from Elsevier.
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Energy Conversion and Management 196 (2019) 1222–1256
because of the poly-dispersed feature of graphene-family nanofluids.
11. Molecular dynamics simulation
One of the most efficient techniques in atomistic modeling is the
Molecular Dynamics (MD) simulation. This approach is adopted to si-
mulate atomic or molecular interactions where, on the one hand,
methods based on continuum assumption are not usable, and on the
other hand, quantum mechanical approaches are not needed. The MD
simulation method can be an efficient tool to examine microscopic
mechanisms for predicting thermohydraulic attributes in the field of
nanofluids.
The MD simulation works based on the principle in which atomic or
molecular Newton motion equations are solved regarding interactions
among atoms or molecules. With the aid of this method, simulation of
the time-evolving microscopic process is carried out, and transport
features as well as equilibrium parameters are statistically evaluated.
Effectiveness of this approach has been certified in instances including
M. Bahiraei and S. Heshmatian
molecular liquids, polymers as well as ionic solutions.
Zhu and Ertekin [193] examined phonon conduction on 2D gra-
phene/boron nitride superlattices with changing interface structures
and periods. They utilized non-equilibrium molecular dynamics and
lattice dynamics. Their results showed that when the period of super-
lattice reaches a critical value near 5 nm, the lattice thermal con-
ductivity reduces severely to a minimum value, and then, it smoothly
rises with the period increment. It was revealed that the minimum in
the thermal conductivity emanates from a competition between lattice
dispersion and anharmonic impacts like interface scattering. The first
decrease in the thermal conductivity can partially be explained through
the harmonic wave impacts induced by interfacial modulation, such as
the opening of phononic band gaps and decrease of group velocity.
Beyond the minimum, decreased inelastic interface scattering is the
reason for the observed trend. A universal scaling of the thermal con-
ductivity with total superlattice length indicated that the critical period
is independent of total length, and long-wavelength phonons are
leading carriers. The authors also showed the ultrasensitivity of thermal
conductivity to superlattice periodicity disorder and interfacial defects.
Such a study reveals that the thermal conductivity of low-dimensional
systems might diverge when the total length rises. Although the reasons
for such a divergence are still unclear in the literature [194], it may be
due to the lower contribution of anharmonic scattering compared with
the heat conduction by long-wavelength, low-frequency phonons that
are activated as the system size becomes larger. It can also be due to
contributions from the high (diverging) density of states of the long-
wavelength z-acoustic phonon modes that activate as the sample size
enlarges [193,195].
In another study, Zhu and Ertekin [196] investigated the effects of
structural disorder on vibrational energy transport in low-dimensional
disordered materials. With employing amorphous graphene and glassy
diamond nanothreads as the samples, the MD simulation and the modal
localization analysis showed that the thermal transport properties have
both differences and similarities from disordered 3D materials. Similar
to 3D, the low-D disordered systems showed both propagating and
diffusive vibrational modes. In contrast to 3D, however, the diffusion
contribution to thermal transport in these low-D systems was insignif-
icant, which can be due to inherent differences in the nature of random
walks for lower dimensions. In spite of the lack of diffusions, the re-
duction of thermal conductivity because of disorder in low-D systems
was low or comparable to 3D. The authors mentioned that such a small
reduction in the thermal conductivity emanates from the existence of
low-frequency vibrational modes that keep a well-defined polarization
and preserve the thermal conductivity in the presence of disorder.
Although many papers have been published on the basis of MD si-
mulation in different liquids, the studies carried out through this
method for graphene-based nanofluids are very sparse. Cha and Kyoung
[197] conducted an MD simulation for the nanofluid having a single
graphene nanosheet with different functional groups (Fig. 22) for
evaluating the effects of affinity and particle dimension on the graphene
nanosheet behavior. With the aid of nanoparticle velocity concept, the
authors examined the dependence of behavior on affinity to explore the
influence of functional groups and interactions on the stability of the
nanofluid. The results showed that the larger particles lead to better
stability of the nanofluid.
Moghaddam et al. [198] evaluated the viscosity of a glycerol–-
graphene sheet nanofluid using the MD simulation. It was revealed that
the dispersion factor of pure graphene with five layers was 37.37 MPa1/
2
which was close to that of the pure glycerol. Therefore, the authors
argued that the graphene can develop a stable suspension in the gly-
cerol. In addition, the diffusion factor of the nanofluid reduced by in-
crement of the graphene layers.
Rodriguez-Laguna et al. [199] employed the MD simulation to as-
sess interactions between the graphene sheets and base fluid, and to
evaluate a potential order induced by the graphene sheets in the base
fluid. Parallel orientation of dimethylformamide (DMF) towards the
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Energy Conversion and Management 196 (2019) 1222–1256
Fig. 22. MD simulation of nanofluid having graphene sheet with functional
groups [197]. Reprinted with permission from Elsevier.
graphene sheet was observed, which augmented the π–π stacking. Be-
sides, a local order of the DMF molecules around the graphene sheet
was achieved, which this specific type of interaction as well as the in-
duced local order can contribute to the improvement of the heat
transfer characteristics of the graphene-based nanofluid.
Although MD simulation can provide efficient information about the
behavior of nanoparticles in liquids, it has some restrictions such as
computational time and the number of nanoparticles. Indeed, it is not
an optimum work to apply full MD simulation to assess flows at micro-
or nano-scales since simulation time, and computations amount in-
tensify profoundly. It is known that inaccuracy of the continuum as-
sumption is often limited to specific regions like solid–fluid or fluid–-
fluid interfaces. Consequently, using the MD technique in the whole
domain is not needed, and a hybrid approach can be utilized that
combines MD simulation with continuum fluid dynamics. Hence, more
attentions should be paid to hybrid methods for studying nanofluids
containing graphene sheets in future investigations.
In addition, MD simulation needs considerable computations, while
it is known that nanoparticles have greater sizes compared with mo-
lecules of liquids and accordingly, their motion is much slower. On the
other hand, the nanosheets motion length scales are much larger than
length scale of base liquid molecules. Greater time steps cannot be used
since they lead to overlap of fluid particles, which causes significant
errors in final outcomes. Meanwhile, smaller time steps will require a
very long computational execution to take into account thorough evo-
lution of more sluggish mode. In these situations, it is recommended to
use Brownian dynamic simulation in which liquid molecules are re-
moved from the simulation and hence, calculation of short-time-scale
motions is not required. In reality, the impact of hydraulic interactions
caused by the base liquid is regarded via a spatial friction tensor. Thus,
calculations volume will be reduced considerably with the aid of this
technique compared to conventional MD method.
12. Second law of thermodynamics
In order to evaluate the behavior of graphene-based nanofluids,
most of the researchers have employed the first law of thermodynamics,
which cannot completely explain the overall efficiency of equipment
operated with these nanofluids. All in all, entropy parameter increases
in hydrothermal processes. This means that unlike energy amount that
follows a conservation rule, energy quality degrades when energy
M. Bahiraei and S. Heshmatian
converts to another form with lower capability of generating power.
Quality of energy can be examined by the second law of thermo-
dynamics, which is essential to reach optimal designs of industrial
components. As a result, evaluating nanofluids containing graphene-
family nanomaterials with the aid of the second law of thermodynamics
is of many importance. Very few studies have been performed in this
regard on graphene-based nanofluids, most of which have investigated
entropy generation rates.
Tharayil et al. [200] modeled a mini loop heat pipe and evaluated
heat transfer efficiency and entropy generation for the nanofluid flow
having the graphene sheets. It was shown that using the nanofluid re-
duces the entropy generation and enhances the second law efficiency.
The decrease in the overall entropy generation in the case of utilizing
the nanofluid was 34.6% and 23.9% at volume concentrations of 0.006
and 0.003%, respectively.
Mehrali et al. [201] studied entropy generation of a nitrogen-doped
graphene nanofluid flowing inside a circular pipe. With the con-
centration increment, the thermal entropy generation decreased while
the frictional entropy generation intensified. In addition, the total en-
tropy generation was affected by the concentration with higher in-
tensity at the greater velocities.
Mehrali et al. [202] investigated entropy generation for the flow of
a nanofluid containing GNPs with a specific surface area of 750 m2/g
inside a circular pipe. The results showed that with the increase of the
volume fraction, frictional entropy generation intensified, whereas
thermal entropy generation reduced.
Bahiraei et al. [203] evaluated the second law features such as en-
tropy generation, second law efficiency, and exergy destruction for flow
a nanofluid containing GNPs coated by Ag nanoparticles within a micro
heat exchanger. The thermal and frictional exergy destruction rates
increased with the increment of the concentration or Reynolds number.
Moreover, the second law efficiency reduced with increase in the con-
centration or Reynolds number.
Mehrali et al. [204] examined the entropy generation of a hybrid
GO–magnetite nanofluid under forced convection in the presence of the
permanent magnetic field. The results indicated that the entropy gen-
eration decreases by 41% in comparison with the pure water. Moreover,
the convective heat transfer was enhanced profoundly under the mag-
netic field.
Sadeghinezhad et al. [205] experimentally studied the entropy
generation of a GNP nanofluid within a horizontal pipe. Based on the
obtained results, the entropy generation of the nanofluid reduced with
an increment of the wall heat flux.
Bahiraei and Mazaheri [206] studied the entropy production and
second law features of a nanofluid with GNPs coated by platinum na-
noparticles inside a chaotic twisted geometry. Thermal entropy gen-
eration decreased by increasing the distance from the inlet of each
bend. Additionally, with an increment of the Dean number and con-
centration, thermal entropy generation, and Bejan number reduced
whereas frictional entropy generation increased. Fig. 23 displays the
velocity vectors and contours of thermal entropy generation rate at
different cross sections for Dean number of 300 and a concentration of
0.1%.
As can be seen, the focus of the research studies in this area has been
on values of entropy generation, while low attention has been paid to
exergy destroyed. Evaluation of exergy destruction due to heat transfer
and friction can provide more efficient information in these systems to
illustrate potential work destroyed. Moreover, many of the papers are
related to basic geometries such as circular tubes, whereas investigating
the second law characteristics of graphene-based nanofluids in im-
portant equipment including heat exchangers, heat sinks and solar
collectors can result in significant guidelines to optimum utilization of
these components under various conditions. Such studies can be fol-
lowed by researchers in future research in this area.
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Energy Conversion and Management 196 (2019) 1222–1256
Fig. 23. Velocity vectors and contours of thermal entropy generation rate at
different cross sections for Dean number of 300 and concentration of 0.1%
[206]. Reprinted with permission from Elsevier.
13. Artificial intelligence
Artificial Intelligence (AI) methods are appropriate tools as sub-
stitute approaches to common techniques. They are employed to solve
complex practical problems in diverse areas, and today, these methods
are becoming growingly popular. AI methods can be trained through
patterns, and are capable of handling noisy data, and can also manage
non-linear problems. Also, an AI technique can conduct estimation and
generalization with excellent speed.
Due to the unique features of AI algorithms, some investigators have
used these methods for prediction and optimization in the field of na-
nofluids. Neural networks and genetic algorithm have been most uti-
lized AI approaches in the area of graphene-family based nanofluids.
Khosrojerdi et al. [207] developed a model for predicting the
thermal conductivity of a graphene sheets nanofluid through multilayer
perceptron artificial neural network (ANN). To collect data required for
training the ANN, the authors experimentally measured the nanofluid
thermal conductivity at temperatures of 25 °C–50 °C and concentrations
of 0.00025–0.005. The obtained model was able to predict the thermal
conductivity accurately, such that determination factor (R2) and mean
absolute percentage error were obtained 0.99 and 0.26%, respectively.
Vakili et al. [208] used an ANN combined with a genetic algorithm
to predict the viscosity of a GNP nanofluid in terms of the temperature
and concentration. The experimental data were utilized for training the
ANN, and the genetic algorithm improved the training technique. In
this study, the results proved the suitable accuracy of the ANN model in
predicting the viscosity.
Tahani et al. [209] developed a mathematical model using the ANN
for predicting the thermal conductivity of a GO sheets-water nanofluid
as a function of the concentration and temperature. Optimal config-
uration of the ANN had two hidden layers with four and eight neurons
in these layers, respectively. The obtained model accurately estimated
the nanofluid thermal conductivity.
Bahiraei et al. [210] optimized heat transfer and hydrodynamic
features of a biological graphene sheets nanofluid in a pin fin liquid
block. The cylindrical fins with various heights and diameters were
considered. The pumping power and surface temperature were re-
garded as the objective functions, and optimum magnitudes of the fin
diameter, fin height and concentration were determined to minimize
these objective functions. The compromise programming method, along
with the genetic algorithm, was utilized to consider standpoints of a
decision maker. The fin height had a quite similar influence on the two
objective functions, while the concentration and fin diameter change
M. Bahiraei and S. Heshmatian
Fig. 24. a) Micro liquid block under study, b) configuration of used neural
network [212]. Reprinted with permission from Elsevier.
the surface temperature more intense than the pumping power.
Azimi and Mozaffari [211] investigated the heat transfer of a
GO–water nanofluid flowing between two moving parallel plates via an
intelligent black-box identifier. The proposed intelligent tool was
termed as evolvable evolutionary fuzzy inference system that was on
the basis of integrating low-level fuzzy programming and hyper-level
evolutionary computing concepts. The authors provided a nonlinear
map between the inputs including the volume concentration, moving
parameter and Eckert number, and the output namely the Nusselt
number. The suggested model showed a proper capability of predicting
the Nusselt number.
Bahiraei et al. [212] carried out the optimization of hydrothermal
characteristics of an ecofriendly graphene nanofluid in a heat sink for
various importance grades of objective functions. The authors obtained
optimum cases to reach minimum surface temperature and pumping
power. Use of the nanofluid with the highest concentration was sug-
gested for all cases except the conditions in which importance grades of
surface temperature and pumping power are very low and very high,
respectively. Fig. 24 displays the micro liquid block under study as well
as the configuration used for the neural network.
The above literature survey indicates that in most of the studies in
this arena, AI methods (specifically ANNs) have been utilized for pre-
diction of thermophysical properties of nanofluids such as thermal
conductivity and viscosity. However, these techniques can have a
proper ability for performing prediction in problems related to heat
convection as well. Furthermore, data obtained from experimental
studies have frequently been used to train ANNs for modeling.
Indeed, according to the fact that experimental measurements are
intricate and expensive, specifically for graphene based nanofluids,
using AI algorithms is strongly recommended for performing prediction
in this field. It should be noted that employing these approaches can
considerably decrease the number of required experiments, and hence,
the costs needed are reduced.
In addition, CFD simulations usually have the limitations of CPU
time and large computations. Hence, use of AI methods in combination
with CFD solutions can significantly reduce the computational volume
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Energy Conversion and Management 196 (2019) 1222–1256
in problems related to graphene family nanofluids. Accordingly, more
utilization of these techniques is expected in the future research on this
topic.
14. Applications of graphene-based nanofluids
Owing to the excellent characteristics of nanofluids containing
graphene sheets, they have found several interesting applications in
diverse industrial sectors, some of which are introduced in this section.
14.1. Car radiator
Selvam et al. [213] used a GNPs nanofluid as the working fluid in a
car radiator. Water–EG mixture was utilized as the base liquid, and the
experiments were conducted at different mass flow rates. The con-
vective heat transfer coefficient enhanced by increasing the con-
centration, inlet temperature, and flow rate. The highest increment was
104%, which occurred at a temperature of 35 °C.
Selvam et al. [214] measured the pressure loss and convective heat
transfer coefficient of a GNPs nanofluid within a car radiator. The
convective heat transfer coefficient enhanced with increase in each of
the parameters of the concentration, inlet temperature, and flow rate.
The increment of the convective heat transfer coefficient for the max-
imum values of concentration and flow rate was 20% and 51% at
temperatures of 35 °C and 45 °C, respectively. Moreover, the pressure
loss intensified by increasing the concentration.
14.2. Electronics cooling
Bahiraei and Heshmatian [215] investigated the thermal perfor-
mance and entropy generation of a nanofluid having GNPs decorated
with Ag nanoparticles for CPU cooling. A new distributor heat sink was
assessed in comparison with two common heat sinks. It was shown that
the new heat sink has a better performance based on both heat transfer
rate and irreversibility features. Fig. 25 presents the temperature con-
tours reported for different conditions.
Ali and Arshad [216] experimentally studied the angle effect of a
pin fin heat sink with employing water–GNPs nanofluid. Three heat
sinks with the channel angles of 22.5°, 45°, and 90° were examined.
According to the results, the heat sink with a channel angle of 22.5°
demonstrated superior heat transfer efficiency in comparison with the
other heat sinks.
Arshad and Ali [217] utilized a GNPs nanofluid in an integral fin
heat sink to evaluate its hydrothermal characteristics. For the nano-
fluid, the smallest base temperature and highest heat transfer increment
were obtained, which respectively were 36.81 °C and 23.91% for heat
flux of 47,960 W/m2. Additionally, greater pumping power was ob-
served for the nanofluid in comparison with the base fluid.
14.3. Energy storage
Fan et al. [218] investigated GNPs and CNTs based nanofluids on
assessing their super cooling degree and latent heat of crystallization as
well as the crystallization kinetics. The results revealed that the dilute
nanofluids decrease the super cooling degree because of the nucleating
influence. The planarly-shaped graphene nanoplatelets with great
contact area act better than the CNTs to facilitate heterogeneous nu-
cleation. These materials can be used as phase change materials for low-
temperature thermal energy storage.
Li et al. [219] benefitted the great specific surface area of graphene
sheets to decrease the subcooling of freezing for a phase change ma-
terial. The findings showed the ability of graphene sheets in energy
storage by the phase transition latent heat. The requirement for sub-
cooling to freeze water was deleted by suspending the graphene sheets.
Moreover, in comparison with the TiO2 and SiO2 nanoparticles, the
graphene sheets resulted in freezing the water at a lower freezing time
M. Bahiraei and S. Heshmatian Energy Conversion and Management 196 (2019) 1222–1256

Fig. 25. Temperature contours for cases of using: (a) water in the distributor heat sink, (b) nanofluid in the distributor heat sink, and (c) nanofluid in parallel heat
sink [215]. Reprinted with permission from Elsevier.

and smaller subcooling degree.

Sathishkumar et al. [220] examined the solidification features of a
water–GNPs nanofluid during the solidification inside a spherical con-
tainer. Adding the GNPs led to a significant decrease in the subcooling
of the water from −7°C to −2.5 °C accompanied by a 25% decrease in
the solidification time because of the high specific surface area as well
as great thermal conductivity.

14.4. Heat exchangers

Khajeh Arzani et al. [221] employed a GNP–water nanofluid in an

annular heat exchanger to evaluate its thermohydraulic attributes. The
suspended nanosheets profoundly increased the thermal efficiency of
the water in the heat exchanger. In addition, the friction factor reduced
with increase in the Reynolds number, while intensified with the GNP
concentration increment.
Rabbani Esfahani and Mohseni Languri [222] investigated the ex-
ergy loss for a GO nanofluid flow inside a shell-tube heat exchanger. It
was indicated that employing the nanofluid causes lower exergy loss in
the heat exchanger. Thereby, in comparison with the nanofluid at
concentrations of 0.01 and 0.1 wt%, the pure water resulted in 22% and
109% increments in the exergy loss, respectively.
Ghozatloo et al. [223] studied the convective heat transfer of the
graphene sheets nanofluids within a shell-tube heat exchanger. It was
found that suspending the graphene sheets in the base liquid enhances
the thermal conductivity and convective heat transfer. For instance, the
convective heat transfer coefficient of the nanofluid with a concentra-
tion of 0.1 wt% was 35.6% higher than that of the water.
Bahiraei et al. [224] examined the thermohydraulic attributes of a
nanofluid including GNP–platinum composite powder inside a triple-
pipe heat exchanger fitted with inserted ribs. The effectiveness and
overall heat transfer coefficient increased with increment of the con-
centration and rib height, and with decrease of the rib pitch. Mean-
while, the pressure loss was more significant for higher rib heights and
smaller rib pitches. The velocity vectors obtained from this work are
illustrated in Fig. 26 at a concentration of 0% and rib pitch of 50 mm for
different rib heights.
Goodarzi et al. [225] employed the nitrogen-doped graphene na-
nofluids as the working fluid in a double-tube heat exchanger. In-
creasing the Reynolds number or concentration enhanced the heat
transfer rate. For example, use of the nanofluid with concentration of
0.06 wt% caused a 15.86% increment in the convective heat transfer
coefficient compared with the base fluid. Besides, the pumping power
intensification was minor.
Hung et al. [226] employed a hybrid nanofluid having GO sheets,
Fig. 26. Velocity vectors at concentration of 0% and rib pitch of 50 mm for rib
heights of a) 3 mm, and (b) 9 mm [224]. Reprinted with permission from
Elsevier.
amorphous carbon as well as graphite-2H as the coolant in an air-cooled
heat exchanger. The thermal performance and pumping power in-
creased by the concentration increment. For the nanofluid at weight
concentration of 0.02%, the highest increments of the thermal perfor-
mance and efficiency factor were almost 13.0% and 11.7%, respec-
tively, in comparison with the base fluid.
Ranjbarzadeh et al. [227] experimentally investigated the influence
of utilizing a GO–water nanofluid in an air-cooled heat exchanger. It
was shown that the Nusselt number and friction coefficient increase in
case of using the nanofluid rather than the base fluid. Due to the var-
iations in the friction coefficient and heat exchange rate, the heat
transfer performance factor enhanced up to 42.2%.
14.5. Heat pipe
Tharayil et al. [228] investigated the thermal efficiency of a min-
iature loop heat pipe (Fig. 27) using a water–graphene sheets nanofluid.
An optimal filling ratio of 30% of the entire volume of the heat pipe was
utilized. The nanofluid enhanced the heat transfer efficiency and re-
duced the evaporator interface temperature in comparison with the
base fluid. Optimal concentration was 0.006%, which provided the
highest enhancement in the heat transfer.

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M. Bahiraei and S. Heshmatian Energy Conversion and Management 196 (2019) 1222–1256

Fig. 27. Employed experimental setup [228]. Reprinted with permission from Elsevier.

Kim and Bang [229] evaluated heat transfer efficiency of a GO–-

water nanofluid in a heat pipe having screen mesh wick. For the walls,
the temperatures of the nanofluid-filled heat pipe were smaller than
those of the base fluid-filled heat pipe. In addition, the heat pipe op-
erated with the nanofluid demonstrated smaller thermal resistances in
the evaporator in comparison with that operated with the base fluid.
Sadeghinezhad et al. [230] experimentally investigated the heat
transfer efficiency of a sintered wick heat pipe working with a GNPs
nanofluid. In the case of using the nanofluid for tilt angle of 60°, the
highest enhancements in the effective thermal conductivity of the heat
pipe were 23.4, 29.8, 37.2 and 28.3% at heat input amounts of 20, 40,
60 and 80 W, respectively, in comparison with the horizontal condition.
Su et al. [231] assessed the thermal efficiency of an oscillating heat
pipe filled with a GO nanofluid. There was an optimal concentration in
which a greater heat transfer performance was achieved. An approach
was suggested on the basis of measuring the thermal physical properties
of the nanofluid, which determined the optimal concentration to reach
the highest thermal performance. Fig. 28. Configuration of evacuated tube solar collector [233]. Reprinted with
permission from Elsevier.

14.6. Solar energy

Chen et al. [232] synthesized a nanofluid containing reduced gra-

phene oxide sheets and employed it for utilization in a low-temperature
direct absorption solar collector. The proper stability, together with the
great thermal conductivity, optical absorption, and photo-thermal
conversion efficiency make this nanofluid a very good candidate for this
application. The photo-thermal conversion efficiency of the nanofluid
was 52% at 75 °C and 96.93% at 30 °C.
Iranmanesh et al. [233] evaluated the impact of employing a
GNP–water nanofluid on the efficiency of an evacuated tube solar
collector water heater (Fig. 28). The heat transfer efficiency increased
by 90.7% at a flow rate of 1.5 L/min in case of utilizing the nanofluid as
the absorption medium. Moreover, the thermal energy gain enhanced
with the increase of the nanoparticle concentration.
Khosrojerdi et al. [234] studied the thermo-optical features of a
nanofluid having GO sheets as the working fluid in a low temperature
direct absorption solar collector. The lowest thickness of the nanofluid Fig. 29. Schematic for the model of a volumetric solar receiver based on gra-
phene sheets nanofluid [235]. Reprinted with permission from Elsevier.
layer with the ability of full sun's energy was obtained for the nanofluid
with weight fraction of 0.045 and height of 3 cm. This nanofluid with
an excellent absorption band is a good candidate for utilization in direct
absorption solar collectors.

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M. Bahiraei and S. Heshmatian
Liu et al. [235] performed experimental and analytical investiga-
tions on a high temperature direct solar collector with employing a
graphene sheets–ionic liquid nanofluid as the absorber (see Fig. 29).
The results indicated that the efficiency enhances with increase of the
receiver height and solar concentration, while reduces by increasing the
nanoparticle concentration.
Liu et al. [236] employed an ionic liquid containing graphene sheets
as working liquid in moderate- and high-temperature direct absorption
solar collectors (DASCs). The DASC was optimized in terms of the na-
noparticle concentration, nanofluid height, exposure time as well as
solar concentration. The results showed that the photo-thermal con-
version performance was profoundly dependent on the nanofluid sta-
bility at high temperatures.
Vakili et al. [237] examined the stability and optical properties of a
nanofluid having GNPs for use in DASCs. This nanofluid had an ap-
propriate absorption band for direct absorption collectors. It was able to
completely absorb solar energy for a concentration of 0.005 occurred at
286 wavelength. Besides, the increment of the concentration enhanced
the absorption coefficient of the nanofluid.
Vakili et al. [238] used a water–GNPs nanofluid in a volumetric
solar collector for generating domestic hot water. The results showed
that the efficiency enhances with increase of the concentration, and the
highest efficiency was achieved at a flow rate of 0.015 kg/s. Moreover,
the zero-loss efficiencies for concentrations of 0, 0.0005, 0.001 and
0.005 were 70, 83.5, 89.7 and 93.2%, respectively.
Wang et al. [239] prepared an oil-based nanofluid containing gra-
phene sheets and used this nanofluid in a direct absorption solar col-
lector. The nanofluid demonstrated great absorption coefficient, low
scattering coefficient, as well as great extinction factor. Adding the
nanoparticles to the pure oil significantly increased the heat collection
efficiency.
14.7. Under magnetic fields
Lei et al. [240] studied solidification of a graphene sheets–paraffin
nanofluid in a rectangular cavity under an electromagnetic field. It was
revealed that in case of without the electromagnetic field, the graphene
sheets distribute in the upper region of the solid part, and cluster sig-
nificantly. In contrast, in the case of employing the electromagnetic
field, the graphene sheets distributed in the whole solid part and
showed a superior dispersion.
Sandeep and Malvandi [241] evaluated the hydrothermal attributes
of an electrically conducting liquid film flow of water–graphene sheets
nanofluid. They suggested a model for the flow of Jeffrey, Maxwell, and
Oldroyd-B nanofluids past a stretching surface under a magnetic field.
With increase of the magnetic field parameter, the temperature field
increased while the velocity field decreased.
Sandeep [242] studied the thermal features a nanofluid film flow on
a stretching surface in the presence of an aligned magnetic field. The
nanofluid contained graphene sheets with three different base fluids
including the pure water and water–EG combinations (i.e., 70%
water + 30%EG and 50%water + 50%EG). The concentration incre-
ment considerably enhanced the thermal conductivity of the nanofluid
with the water + 50%EG base fluid in comparison with the nanofluids
with the pure water and water + 30%EG base fluids.
Different applications of graphene-based nanofluids were reviewed
in this section. As seen, although these nanofluids usually have higher
processing costs in comparison with other nanofluids, their utilization is
rather extensive due to the excellent thermal characteristics. Great at-
tributes of graphene-family nanofluids improve heat exchange rates and
therefore, result in significant energy saving in engineering equipment.
Consequently, it is also expected to use them in other applications such
as nuclear system cooling, space and defense, magnetic sealing, and
heating buildings in the future investigations.
As a novel application, nanoparticles are also added to phase change
materials (PCMs) to enhance their thermal properties and form
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Energy Conversion and Management 196 (2019) 1222–1256
nanofluids in the molten state. The majority of the studies in the lit-
erature have concentrated on the addition of metal oxide nanoparticles
to PCMs, while a few investigations have been carried out on adding
graphene materials to PCMs. This can be an interesting research topic
for the scholars who work in this area. Moreover, generating graphene-
based nanofluids with polymer additives can introduce other applica-
tions as advanced thermal liquids to develop more functional nano-
materials because polymer molecules might lead to improved web-like
arrangements for nanoparticles within base liquids.
Refrigerants containing graphene sheets should be examined to
evaluate their potential in enhancing the thermal features of condensers
and evaporators employed for two-phase heat transfer applications,
including air-conditioning and refrigeration devices.
Graphene-based nanofluids can also be implemented for cooling of
high-temperature tubes when extracting energy from the crust of the
earth in geothermal applications. Moreover, these nanofluids can be
used to cool the devices and equipment operated in great friction and
high-temperature situations such as drilling.
In power generation technology, graphene family nanofluids can be
utilized for transformer cooling, which will reduce the weight and size
of transformers. They can also be employed to reach great temperature
gradients in thermoelectrics for better converting waste energy to
electricity.
15. Concluding remarks
In this survey, a comprehensive review was performed on graphene
family nanofluids. Different aspects including as material type, pre-
paration methods, stability, types of surfactants, convective heat
transfer, hydrodynamic characteristics as well as second law features
were considered. In addition, most important applications of graphene
based nanofluids were introduced. The studies carried out indicate that
these nanofluids possess very good capabilities for utilization in diverse
thermal applications. The most important findings from this review
paper along with the challenges and future directions are as follows:
15.1. Results
- Single-layer graphene possesses superior thermal conductivity than
multi-layer graphene sheets.
- Decorating metal or metal oxide nanoparticles on graphene sheets
avoids graphene agglomeration and eliminates requirement of sur-
factants for stabilizing graphene nanomaterials in base liquids.
- Functional groups result in reduction in the surface area of graphene
sheets and therefore, applying nanoparticles as a guest material on
graphene sheets can be suitable in thermal conductivity increment
of functionalized graphene sheets.
- In comparison with covalent techniques, non-covalent methods are
specifically promising since the achieved products are more simply
handled, and the modification can be performed such that the ori-
ginal properties of graphene sheets are preserved, whereas the sta-
bility is enhanced. However, the process capability and manipula-
tion of graphene platelets may not be satisfied because of the robust
Van der Waals forces.
- Thermal conductivity of functionalized graphene nanoplatelets is
lower than that of pristine graphene ones.
- Local order of base fluid molecules in vicinity of graphene sheets,
parallel structure as well as the potential π–π stacking can be ef-
fective mechanisms to clarify the reasons of great heat transfer en-
hancement in graphene family nanofluids.
- Nanofluids with graphene sheets frequently possess superior con-
vective heat transfer compared with those containing GO sheets.
- Using graphene family nanomaterials in nanofluids can enhance
thermal attributes and energy performance of heat transfer equip-
ment and therefore, size of devices such as heat exchangers de-
creases, which results in enhanced reliability, less pollution as well
M. Bahiraei and S. Heshmatian
as higher efficiency.
- At rather high concentrations, film-like shape of graphene sheets
develops a nonporous structure of deposition on surfaces, which can
degrade nucleation sites and therefore diminish boiling perfor-
mance.
- Due to unique properties of graphene materials, nanofluids con-
taining these materials can be prepared in small concentrations. This
results in contamination decrease and will reduce sedimentation
challenges and the costs of heat transfer liquids.
15.2. Challenges
- In spite of the interesting characteristics, there are still some pro-
blems of graphene oxide for efficient utilization in nanofluids. The
existence of structural defects, rather poor stability, restacking and
multilayer thickness can influence the features and great surface
area of graphene oxide.
- The excellent properties of rGO are related to monolayer or few-
layered structures. However, neighboring rGO sheets causes ag-
gregating them into macro scale carbon allotropism. Therefore,
quality of nanoparticle dispersion is very important in preparing
nanofluids containing rGO.
- Graphene exfoliation method can only be adopted in limited sys-
tems, has some problems like rather small concentrations, and re-
quires significant sonication.
- Although acid treatment changes the original structure of the ma-
terial, it is proved to be an efficient approach to produce stable
suspensions of graphene based nanomaterials. However, a high
grade of functionalization is needed in this technique.
- Surfactants may not be appropriate for lubricants because they
would not meet viscosity criteria. In reality, although mineral oils
are usually non-polar, graphene sheets are not adequately hydro-
phobic to create uniform suspensions.
- Although gum Arabic can result in more appropriate state for dis-
persing graphene sheets compared to triton X-100 and SDBS, it
considerably intensifies viscosity of suspensions.
- Different scholars have reported different results about the changes
of boiling heat transfer in nanofluids containing graphene materials.
In some of the studies, it is stated that boiling heat transfer is aug-
mented with concentration increment, while in the some other pa-
pers, a reduction in billing heat transfer is noticed. Such observa-
tions are dependent on the concentration range under study.
15.3. Future directions
- Existence of surfactant additives can decrease thermal conductivity
of nanofluids. Therefore, in order to enhance the solubility of gra-
phene materials in base fluids without reduction of the thermal
conductivity of nanofluids, an inorganic layer can be decorated on
graphene platelets rather than use of surfactants.
- Interactions between graphene sheets and metal or metal oxide
nanoparticles in nanocomposite powders have opened the routes to
design and develop novel applications ranging from the energy is-
sues to medical sector. Hence, performing more studies and in-
troducing newer procedures for synthesis of graphene-based nano-
composite powders are crucial.
- The methods utilized for improving the stability make a graphene
based nanofluid stable for only some days or months. Hence, ap-
plying superior changes on surface of graphene sheets based on
advanced research in the future can be effective to reach more stable
nanofluids with longer stability time.
- Acid chemical functionalization can damage graphene sheets
structure. Also, carboxylic group is one of the chief causes of cor-
rosion in engineering devices. These important factors should be
considered in the future studies with more attention.
- In the future, simulations based on molecular dynamics can disclose
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Energy Conversion and Management 196 (2019) 1222–1256
molecular mechanisms of adsorption morphology of dispersants,
and determine the interaction energy between graphene sheets
modified via surfactants.
- Some contradictions are seen among the reported results about the
wettability and contact angle of graphene based nanofluids. Hence,
new studies in this field need to be further performed to establish an
accepted trend about changes of the contact angle in nanofluids
including graphene sheets.
- A graphene sheet is prone to getting folded, coiled, and corrugated
at the surface and edges. This can affect energy transmit mechan-
isms and so, thermal conductivity models developed for a specific
shape may not be capable of predicting the actual mechanisms in
other nanoparticle shapes. Therefore, novel models should be de-
veloped for predicting thermophysical properties of graphene based
nanofluids.
- In graphene and GO nanofluids, most of the studies have reported
that thermal conductivity is temperature dependent, whereas some
studies have indicated the inconsistent results. As a result, more
studies should be carried out to accurately uncover governing me-
chanisms.
- Defects in graphene sheets can influence thermophysical properties
of nanofluids, while these effects are not obviously known. The
characterization methods can be efficient for disclosing unknown
details about graphene defect influences on nanofluid thermo-
physical properties.
- Most of the experimental studies have been conducted in room
temperature, while with respect to the diverse applications of gra-
phene based nanofluids, evaluating thermophysical properties of
these nanofluids at temperatures above and below ambient condi-
tions is also very critical.
- Studies on electrical conductivity of nanofluids containing graphene
nanomaterials is very sparse, whereas electrical features play key
roles in many of applications of these nanofluids.
- A more significant attention should be paid to optical properties of
graphene based nanofluids to be utilized in solar thermal applica-
tions.
- In the numerical studies, most of the papers have employed the
single-phase simulation, while more attention should be given to
two-phase approaches because graphene sheets can possess a mac-
roscale transverse size that may cause significant errors in the case
of using homogenous methods.
- According to the fact that the non-Newtonian behavior of graphene
based nanofluids can have significant effects on friction and pres-
sure drop, it is vital to evaluate these nanofluids with considering
dependency of viscosity on shear rate in future studies.
- More attentions should be paid to hybrid methods that combine MD
simulation with continuum fluid dynamics for studying nanofluids
containing graphene sheets in future investigations.
- In second law analysis, many of the papers are related to basic
geometries such as circular tubes, whereas investigating the second
law characteristics of graphene based nanofluids in important
equipment including heat exchangers, heat sinks and solar collectors
can result in significant guidelines to optimum utilization of these
components. Such studies can be followed by researchers in the
future research on this area.
- According to the fact that experimental measurements are intricate
and expensive specifically for graphene based nanofluids, using AI
algorithms is strongly recommended for performing prediction in
this field.
- The majority of the studies in the literature have concentrated on
addition of metal oxide nanoparticles to PCMs, while a few in-
vestigations have been carried out on adding graphene materials to
PCMs. This can be an interesting research topic for the scholars
which work in this area.
- Refrigerants containing graphene sheets should be examined to
evaluate their potential in enhancing the thermal features of
M. Bahiraei and S. Heshmatian
condensers and evaporators employed for two-phase heat transfer
applications including air-conditioning and refrigeration devices.
- Graphene based nanofluids can be implemented for cooling of high
temperature tubes when extracting energy from the crust of the
earth in geothermal applications.
- Graphene family nanofluids can be utilized for transformer cooling,
which will reduce weight and size of transformers. They can also be
employed to reach great temperature gradients in thermoelectrics
for better converting waste energy to electricity.
- Ionnanofluid is a new opportunity for utilization in thermal appli-
cations. Ionnanofluids containing graphene nanomaterials should be
studied with more attention in the future.
Declaration of Competing Interest
None.
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