International Journal of Thermal Sciences 191 (2023) 108349

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International Journal of Thermal Sciences

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

Nucleate boiling enhancement on bubble-induced assembly of graphene

oxide/carbon black hybrid networks
Nurettin Sezer *, Shoukat Alim Khan, Yusuf Biçer, Muammer Koç
Division of Sustainable Development, College of Science and Engineering, Hamad Bin Khalifa University, Qatar Foundation, Education City, Doha, Qatar

A R T I C L E I N F O A B S T R A C T

Keywords: The efficiency and capacity of nucleate boiling can be enhanced by the bubble-induced assembly of nano­
Nucleate boiling particles, which are dispersed in a boiling liquid. Recently, carbon nanomaterials have attracted appreciable
Graphene oxide research interest for boiling heat transfer enhancement. This study presents nucleate boiling performance on
Carbon black
interconnected graphene/carbon black hybrid films formed through the bubble-induced self-assembly of sus­
Hybrid dispersions
Self-assembly
pended particles. Aqueous graphene/carbon black hybrid solutions at varying concentration ratios (GO:CB; 1:0,
1:1, 1:5) were prepared via probe sonication. The solutions were then saturated and subjected to pool boiling
under atmospheric pressure on a custom-made boiling test apparatus with a flat copper heating surface. Ex­
periments were carried out at a stepwise increasing heat flux until the critical heat flux was reached. A heat
transfer coefficient and critical heat flux enhancement of 223.0% and 182.4%, respectively, were achieved at a
GO:CB concentration ratio of 1:5. The change in surface characteristics and, subsequently, the boiling perfor­
mance were elaborated by conducting a series of surface characterizations such as Field Emission Scanning
Electron Microscopy, Energy Dispersive X-Ray analysis, contact angle analysis, and surface profilometry.
Nucleate boiling enhancement was attributed to the contribution of multiple factors such as surface roughening,
increased effective surface area, decent interfacial contact within the assembly structure, improved capillarity,
and lateral heat conduction.

1. Introduction
Due to the continuous quest for size diminution, higher computa­
tional capability and multifunctionality, the transfer or dissipation of
high heat fluxes from electronic devices has become a crucial, yet
challenging task to sustain safe, efficient, and cost-effective operation.
Among various heat transfer modes, nucleate boiling provides passive
and highly efficient phase change heat transfer with eminent heat
transfer capacity. Moreover, nucleate boiling ensures a minimal tem­
perature difference between the heated surface and saturated liquid, as
well as uniform cooling across the heated surface. Despite nucleate
boiling offers such desirable merits, it still has much room for
improvement in efficiency and capacity, which are termed as the heat
transfer coefficient and critical heat flux, respectively.
Heating surface characteristics such as the availability of active
cavities for bubble nucleation, roughness, wettability, capillarity, and
lateral heat conduction have been reported to play a key role in the
surface hydrodynamics and bubble dynamics, and subsequently, the
heat transfer coefficient and critical heat flux [1–3]. Thus, different
surface structuring and coating strategies have been explored over time
to manipulate the heating surface characteristics in order to enhance
nucleate boiling. In this regard, laser texturing [4–6], electrospinning
[6], laser processing [7–10], chemical vapor deposition [11–13], elec­
trochemical deposition [14–17], dip coating [18–20], and spray coating
[21–23] are some of the methods that have been investigated for
enhanced nucleate boiling. However, these methods are generally
time-consuming, costly, and labor-intensive [24,25].
Recently, researchers proposed bubble-induced deposition of nano­
particles through self-assembly as a cost-effective and facile route for
nucleate boiling enhancement [3,26,27]. Highly-ordered foam-like
interconnected nanostructures were formed through bubble-induced
self-assembly of graphene on heating surfaces along the liquid–vapor
interface of vapor bubbles. Ahn et al. [25] prepared foam-like graphene
layers through bubble-induced self-assembly during saturated pool
boiling of aqueous dispersions of reduced graphene oxide nanosheets.
The morphology and thickness of the deposition layer were manipulated
by varying the applied heat flux and boiling time. At low heat fluxes,
laminate deposition layers were produced. However, foam-like

* Corresponding author.
E-mail address: sezernureddin@gmail.com (N. Sezer).

https://doi.org/10.1016/j.ijthermalsci.2023.108349
Received 5 April 2022; Received in revised form 4 April 2023; Accepted 11 April 2023
Available online 15 April 2023
1290-0729/© 2023 The Authors. Published by Elsevier Masson SAS. This is an open access article under the CC BY license
(http://creativecommons.org/licenses/by/4.0/).
N. Sezer et al.
structures were formed when sufficiently high heat fluxes were applied,
i.e., in a range of 700 – 1300 kW • m− 2 [28]. The pore size of the gra­
phene layers varied between 10 and 2 μm, which decreased with
increasing heat flux, conforming to the theory proposed by Hsu on the
size of active nucleation cavities [29]. Therefore, the inverse relation­
ship between the applied heat flux and pore size was attributed to the
size and generation frequency of vapor bubbles. Besides that, static
contact angle analysis was conducted to investigate the wettability of
the porous graphene surfaces. Surfaces at all heat fluxes exhibited a
hydrophobic character, and the contact angle increased with increasing
heat flux. Further, the contact angle hysteresis increased with increasing
heat flux and the surface exhibited both hydrophobic character and
adhesivity towards water. It was ascribed by the coexistence of hydro­
phobic reduced graphene oxide planes exposed to the surface and car­
boxylic functional groups such as C = O, C − OH, and O = C − OH,
embedded inside the porous layer.
Ahn et al. [30] used a self-assembly method to build porous graphene
film architectures through spraying graphene dispersions over a super­
heated surface using an automated spray coating device. At varying
colloid discharge rates (400–640 μL • s− 1 ) and superheat temperatures
(130–160 ◦ C), this approach effectively created self-assembled 3D
porous graphene layers over a 75 cm2 substrate area. The produced
film’s electrical conductivity was measured as ∼ 108 S • m− 1 , which rose
to ∼ 574 S • m− 1 after annealing at 400 ◦ C. Besides that, with a Young’s
Modulus of 1000 MPa, the self-assembled graphene layer was mechan­
ically resilient and durable. Due to the presence of chemical functional
groups inside the self-assembled graphene sheet, the film displayed dual
wettability with hydrophobic and hydrophilic characteristics, similar to
their prior studies.
Nucleate boiling enhancement on self-assembled graphene surfaces
was studied by various research groups. In a study by Zhou et al. [31],
self-assembled graphene oxide surface enhanced the heat transfer co­
efficient and critical heat flux by 73% and 104%, respectively. The
enhancement was attributed to the favorable characteristics of the
self-assembly surface such as roughness, thermal conductivity, and
wettability. Accordingly, bubble nucleation, lateral heat dissipation, and
liquid spreading over the heating surface were enhanced that enabled
cooling and rewetting of localized hot/dry spots and delayed the critical
heat flux. Ahn et al. [32] achieved a heat transfer coefficient and critical
heat flux enhancement of 65% and 70%, respectively over
self-assembled graphene surfaces. The graphene film provided increased
nucleation site density, decent capillary wicking, and heat conduction,
which together improved the heat transfer coefficient and delayed dry
spot expansion to higher heat fluxes.
Recently, the hybridization of graphene self-assembly layers with
different nanoparticles has been of research interest. For instance, Sezer
et al. [33,34] studied bubble-induced assembly of graphene oxide/silver
and graphene oxide/carbon nanotube-based aqueous hybrid disper­
sions, and the nucleate boiling enhancement on the hybrid self-assembly
surfaces. Spherical silver nanoparticles deposited in 3D porous graphene
structure and provided increased bubble nucleation site density thereby
improved the heat transfer coefficient. On the other hand, a decent
interfacial contact between graphene oxide nanosheets and functional­
ized carbon nanotubes facilitated dissipation of localized heat to prevent
hot/dry spot formation. Heat transfer coefficient and critical heat flux
were enhanced by 100% and 152.9% on graphene oxide/carbon nano­
tube hybrid surface, and by 109% and 123.5% on graphene oxide/silver
hybrid surface, respectively.
Though various research groups studied hybrids of graphene with
other nanoparticles such as copper [35], Fe3O4 [36], Al2O3 [37], and
SiO2 [38], none of them yielded a uniform porous deposition layer. Since
it is clear from the reviewed literature that self-assembled porous gra­
phene surfaces enhance nucleate boiling, and the hybridization allows
for further enhancement, self-assembly of hybrids of graphene with new
nanomaterials worth investigation. Carbon black nanoparticles possess
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International Journal of Thermal Sciences 191 (2023) 108349
favorable properties such as high conductivity and a large microporous
and nano-porous area for nucleate boiling enhancement, and some ar­
ticles have already reported nucleate boiling enhancement of carbon
black-only dispersions [39,40]. Herein, we aimed to investigate the
boiling heat transfer characteristics of graphene oxide/carbon black
hybrid dispersions for the first time. Specific aims of the study are as
follows.
- To study the properties of bubble-induced graphene oxide/carbon
black hybrid assembly at different GO:CB concentration ratios (1:0,
1:1, 1:5),
- To examine the improvement of the boiling heat transfer coefficient
and critical heat flux on the graphene oxide/carbon black hybrid
surface,
- To investigate the impact of several factors on nucleate boiling
performance, such as heat flux, wall superheat, and the GO:CB
concentration ratio.
- To gain insight into the nucleate boiling enhancement using surface
characterization techniques such as Field Emission Scanning Elec­
tron Microscopy, Energy Dispersive X-Ray Spectroscopy, surface
profilometry, and contact angle analysis.
2. Experimental
2.1. Materials
Copper substrates in the shape of squares of 20 mm × 20 mm were
made using 100 μm-thick, high quality (> 99.8%) copper sheets from
Sigma Aldrich in the United States. Prior to each boiling experiment,
copper substrates were cleaned with 5% hydrochloric acid and then
deionized water. Deionized water was used to make all the solutions and
colloidal dispersions.
The Sixth Element Inc. in China provided chemically oxidized
graphite. High purity (> 99.8%) carbon black nanoparticles (Black Pearl
2000) with a specific surface area of ∼ 1500 m2 • g− 1 were purchased
from Cabot Corporation in South Korea. Transmission Electron Micro­
scopy (Talos F200X) was used to collect micrographs of pure carbon
black nanoparticles and graphene oxide nanosheets. A volume of 20 μL
colloid dispersions were prepared by sonicating particles in ethanol. The
dispersion samples were dropped onto carbon-coated copper microgrids
with a mesh size of 300. The solvent was then given enough time to
evaporate at ambient conditions. The samples were micrographed at a
voltage of 200 kV (Fig. 1). Fig. 1a shows the shape of graphene oxide
nanosheets, which were free of contaminants and had numerous wrin­
kles and ripples. Furthermore, the carbon black nanoparticles were also
observed to be pure in micrographs taken at various magnifications, and
consisted of nearly spherical primary particles, which are fused together
in aggregates. The average size of the CB nanoparticles was ∼ 25 nm.
(Fig. 1b).
2.2. Preparation of hybrid dispersions
By sonicating chemically oxidized graphite and carbon black nano­
particles in deionized water, aqueous dispersions of graphene oxide and
carbon black (0.005wt%) were produced at different concentration ra­
tios; GO:CB = 1:0, 1:1, 1:5 by weight. To evaluate the sole influence of
colloids on nucleate boiling performance, no surfactants were used.
2.3. Experimental apparatus
A custom-built boiling test apparatus was used to conduct experi­
ments with colloidal dispersions (Fig. 2). The apparatus had boiling
pool, condensation, and heat supply units. The pool was arranged on top
of a heating surface, where heat was supplied to the pool of liquid. A
dimroth condenser was connected to a temperature-controlled chiller to
N. Sezer et al. International Journal of Thermal Sciences 191 (2023) 108349

Fig. 1. Transmission Electron Microscopy images of (a) graphene oxide nanosheets and (b) carbon black nanoparticles.

Fig. 2. Schematic of the experimental boiling setup.

condense the vapor leaving the boiling chamber and to sustain the initial
liquid level inside the saturated liquid pool. Heat input to the pool was
controlled by a variable power supply module, which provided required
power to cartridge heaters immersed into a copper heating block from its
bottom along its center-periphery. The block was isolated by a Teflon
case to support the pool, to prevent radial heat loss, and to facilitate one-
dimensional heat conduction on copper block from bottom to top. The
top surface of the heating block was made in square shape (200 mm ×
200 mm) that served as a heating surface. Before each boiling experi­
ment, the same size of a copper substrate with a thickness of 100 μm was
mounted on this surface to facilitate surface characterizations after
boiling. The mounting process for a copper substrate on a copper block
involves heating the copper block to 220 ◦ C and melting a soldering
material, typically a tin and lead alloy, onto it. The substrate is placed on
the melted material and gently pressed to ensure good contact. The
contact resulted in a very thin, negligibly small layer of solder material
and hence its contribution has been neglected in the calculation. The
firm contact is ensured by cooling the copper block. Two thermocouples
were inserted into the heating block underneath the heating surface and
plugged into a thermometer to calculate the temperature and heat flux
on the heating surface. An auxiliary heater was employed to maintain
the bulk water at a saturated temperature prior to the start of the
experiment. The auxiliary heater was used for the purpose of achieving a
stable saturated temperature in the bulk water, and was subsequently
removed before starting the measurements, and hence not shown in
(Fig. 2). More detailed explanation of the boiling test apparatus can be
found in our previous article [34].

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N. Sezer et al. International Journal of Thermal Sciences 191 (2023) 108349

2.4. Surface characterization

Field Emission Scanning Electron Microscope (Versa 3D, FEI) was

used to take micrographs of the graphene oxide/carbon black hybrid
films. Drop Shape Analyzer, KRÜSS, was used to do contact angle
evaluations. A profilometer (KLA Tencor P-17 Stylus Profiler) was used
to describe the surface profiles from a specimen surface area of 100 μm ×
100 μm.

2.5. Data reduction and uncertainty analysis

Experiments on nucleate boiling were carried out at atmospheric

pressure. 250 ml colloidal dispersions were exposed to saturated pool
boiling in the custom-built test equipment at a step size of ∼ 100 kW •
m− 2 until the boiling crisis occurred. Thermometer readings were taken
at each heat flux when the temperature fluctuation was less than 0.1 ◦ C Fig. 3. Comparison of the experimental result with Rohsenow correlation [43]
during a 3 − minute observation period. These temperature readings and Kandlikar CHF model [44] for Cu surface and DI water as working fluid.
enabled the calculation of heating surface temperature and the heat flux
on this surface using the Fourier law as described in Eq. (1) and Eq. (2), X-axis displays the difference between the substrate surface temperature
respectively [41]. and the saturation temperature of the working fluid, and the Y-axis
( ) shows the input thermal energy to the system. The details of these
T2 − T1
Twall = T1 − Δx1s (1) methods can be found in the previous publication of the authors
Δx12
[45–48].
where Twall is the temperature [K] of the heating surface, T1 is the
temperature [K] of the upper thermocouple, T2 is the temperature [K] of
3.1. Boiling curves
the lower thermocouple, Δx12 is the distance (m) between the upper
thermocouple and lower thermocouple, and Δx1s is the distance (m)
The boiling performance of graphene oxide dispersions and graphene
between the upper thermocouple and heating surface.
oxide/carbon black hybrid dispersions were studied by plotting boiling
The heat flux on the heating surface was obtained by the following
curves. The boiling enhancement of colloidal dispersions were observed
formula.
in comparison to water. The graphene oxide dispersed solution had a
T1 − Twall steeper boiling curve than water. Even steeper curves were obtained
q′′ = kCu (2)
Δx1s after boiling graphene oxide/carbon black hybrid dispersions. Steeper
curves indicated the efficiency enhancement of colloidal dispersions.
where q′′ is the heat flux (kW • m− 2 ) and kCu is the thermal conductivity Maximum heat transfer coefficient of graphene oxide dispersion was
(kW •m− 1 •K− 1 ) of the heating block. 59.7 kW • m− 2 • K− 1 , while it increased to 66.9 kW • m− 2 • K− 1 and
The heat transfer coefficient of nucleate boiling was finally calcu­
83.3 kW • m− 2 • K− 1 at graphene oxide/carbon black hybrid dispersions
lated by the following formula.
with GO:CB concentration ratio of 1:1 and 1:5, respectively. Besides
q′′ that, the capacity of nucleate boiling was also significantly enhanced by
h= (3)
Twall − Ts colloidal dispersions. The critical heat flux of water was
∼ 850 kW • m− 2 , which increased to ∼ 2000 kW • m− 2 after dispersing
where h is the heat transfer coefficient (kW • m− 2 • K− 1 ) and Ts is the graphene oxide nanosheets. In addition, the critical heat flux of gra­
liquid saturation temperature [K]. phene oxide/carbon black hybrid dispersions at GO:CB concentration
Uncertainties of the boiling parameters were calculated using the ratios of 1:1 and 1:5 was ∼ 2000 kW • m− 2 and ∼ 2400 kW • m− 2 ,
Kline and McClintock technique [42]. Eq. (4) was used to compute the respectively. Boiling studies on self-assembled surfaces with water
uncertainty of the boiling heat flux and Eq. (5) was used for heat transfer yielded comparable findings, indicating that the nucleate boiling
coefficient.
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
( )2 ( )2 ( )2
Δq′′ ΔkCu Δ(T1 − Twall ) Δ(Δx1s )
= + + (4)
q′′ kCu T1 − Twall Δx1s
√̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅̅
( ′′ )2 ( )2̅
Δh Δq Δ(Twall − Ts )
= + (5)
h q′′ Twall − Ts

The maximum uncertainties of the heat flux and heat transfer coef­
ficient were determined as ± 5.0% and ± 5.4%, respectively.

3. Results and discussion

It is crucial to verify the precision of the experimental setup before

conducting experiments. To evaluate the accuracy of the experimental
setup, the average results obtained from experiments with de-ionized
water (DI) and an untreated copper (Cu) surface were compared to the
Rohsenow correlation [43] and Kandlikar model [44], which are widely Fig. 4. Boiling curves of graphene oxide and carbon black dispersions
accepted in the field. This comparison is illustrated in Fig. 3, where the compared to water.

4
N. Sezer et al.
improvement was caused by bubble-induced self-assembly.
Fig. 4 shows the changes in heat transfer coefficient with applied
heat flux and wall superheat. In Fig. 5, the heat transfer coefficient
increased with the increase of heat flux and superheat at all concen­
tration ratios until reaching the critical heat flux. Table 1 compiles the
nucleate boiling enhancement of colloidal dispersions.
3.2. Morphology
Field Emission Scanning Electron Microscopy images were acquired
to investigate the morphological features of the heating surface after
boiling graphene oxide and carbon black dispersions. Top views of the
self-assembly films at various magnifications are compiled in Fig. 6. The
graphene-only film in Fig. 6a exhibited a uniform 3D porous structure. A
homogenous distribution of carbon black nanoparticles and graphene
oxide nanosheets was observed through the hybrid deposition layers. In
Fig. 6b, the hybrid film at 1:1 GO:CB concentration ratio also possessed a
foam-like morphology similar to that of graphene oxide deposition layer
(Fig. 6a). On the other hand, the hybrid film at 1:5 GO:CB concentration
ratio had completely different morphology with fewer porous structures
distributed through the heating surface (Fig. 6c). However, all deposi­
tion films featured plentiful microcavities for the nucleation of vapor
bubbles.
Tilted views of the surfaces in Fig. 7 confirmed the uniformity of the
deposition films. Though the surface structures appeared to be different
for each deposition film, all surfaces featured porous structure. The
presence of a porous structure is one of several factors that can
contribute to nucleate boiling enhancement, along with other reported
Fig. 5. Variation of the heat transfer coefficient of graphene oxide and carbon
black dispersions and water as a function of (a) heat flux and (b)
wall superheat.
5
International Journal of Thermal Sciences 191 (2023) 108349
Table 1
Enhancement of the heat transfer coefficient and critical heat flux on the self-
assembly surfaces.
GO:CB Heat Transfer Coefficient Critical Heat Flux
Concentration
Maximum Average Value Percent
Ratio
(kW • m− 2 • K− 1 ) Enhancement (kW • m− 2 ) delay
1:0 59.7 112.4% 2000 135.3%
1:1 66.9 137.3% 2000 135.3%
1:5 83.3 223.0% 2400 182.4%
factors such as surface roughness, wettability, morphology, etc. The
cross-sectional images in Fig. 8 also shows the unique porous structure
of each self-assembly film.
3.3. Contact angle
Static contact angle of sessile water droplets on self-assembly films
was measured to investigate their wettability. 2 μL droplets were
mounted on the top surface of the specimens at room temperature under
atmospheric pressure. The photographs of the droplets were taken 5 s
after the droplets were mounted on the surface of specimens. For each
specimen, measurements were conducted at minimum of 5 different
locations. The apparent contact angles were then analyzed by Drop
Shape Analyzer, KRÜSS (Germany). All deposition layers exhibited poor
wettability with contact angles > 90◦ (Fig. 9). Hydrophobicity of gra­
phene oxide assembly layer is in good agreement with previous findings
[28,30,33,34]. The addition of carbon black, on the other hand, did not
make any significant impact on the surface wettability as graphene oxide
film and graphene oxide/carbon black hybrid films exhibited similar
contact angle values.
3.4. Surface profilometry
Surface roughening plays a significant role in enhancing the surface
hydrodynamics and bubble dynamics, and subsequently on the perfor­
mance of pool boiling heat transfer. Therefore, the surface profiles of the
self-assembly films were investigated over a representative surface area
of 100 μm × 100 μm, using a profilometer; KLA Tencor P-17 Stylus
Profiler, Milpitas, CA, (USA). The surface profiles of the plain copper
substrate and coating films are shown in Fig. 10. After boiling colloidal
dispersions of graphene oxide nanosheets and carbon black nano­
particles, self-assembly layers formed on the heating surface that
featured micro and nanocavities, and subsequently yielded a higher
surface roughness. The surface roughness of the plain copper substrate
was 0.13 μm whereas the surface roughness of the bubble-induced self-
assembly layers ranged from 0.44 μm to 0.52 μm.
3.5. Physical mechanism of nucleate boiling enhancement
Physical characteristics of a heating surface, such as effective surface
area, roughness, morphology, wettability, and capillarity, have a sig­
nificant impact on surface hydrodynamics and bubble dynamics during
a boiling process [49]. Since surface hydrodynamics and bubble dy­
namics are essential drivers of nucleate boiling, this section expounds
the physical mechanism of nucleate boiling enhancement based on the
characteristics of the self-assembled films on the heating surface.
Bubble-induced deposition of graphene oxide nanosheets and carbon
black nanoparticles on the heating surface increased the surface
roughness by ∼ 4 times and provided abundant micro and nanocavities
for the nucleation of vapor bubbles. The increased nucleation site den­
sity improved the bubble generation rate, which enabled the dissipation
of higher heat fluxes at relatively low superheats. Therefore, the boiling
of graphene oxide dispersion yielded a significantly higher heat transfer
coefficient in comparison to that of water. The heat transfer coefficient
further increased with the graphene oxide/carbon black hybrid disper
N. Sezer et al. International Journal of Thermal Sciences 191 (2023) 108349

Fig. 6. Scanning Electron Microscopy images of bubble-induced self-assembly films at magnifications 1000 × , 5000 × , 25,000 × , and 100,000 × from left to
right: Top views of (a) graphene oxide film, and graphene oxide/carbon black hybrid film at GO:CB concentration ratios of (b) 1:1 and (c) 1:5.

Fig. 7. Scanning Electron Microscopy images of bubble-induced self-assembly films: Tilted views of (a) graphene oxide, and graphene oxide/carbon black hybrid film
at GO:CB concentration ratios of (b) 1:1 and (c) 1:5.

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N. Sezer et al. International Journal of Thermal Sciences 191 (2023) 108349

Fig. 8. Scanning Electron Microscopy images of bubble-induced self-assembly films: Cross-sectional views of (a) graphene oxide, and graphene oxide/carbon black
hybrid film at GO:CB concentration ratios of (b) 1:1 and (c) 1:5.

Fig. 9. Contact angle analysis of graphene oxide and carbon black deposition layers at different GO:CB concentration ratios: a) 0:1, b) 1:1, c) 5:1.

Fig. 10. Surface profiles of (a) the plain copper substrate, and graphene oxide/carbon black self-assembly films at various GO:CB concentration ratios: (b) 1:0, (c)
1:1, (d) 1:5.

7
N. Sezer et al.
sions. In addition, the heat transfer coefficient of both graphene oxide
and graphene oxide/carbon black dispersions improved with increasing
heat flux due to the reason that at low heat fluxes, only large surface
cavities served as active sites for bubble nucleation whereas smaller
cavities were activated at increased heat fluxes that improved the bubble
generation rate and subsequently the heat transfer coefficient. Thus, the
significant enhancement of heat transfer coefficient at high heat fluxes is
attributed to the activation of small surface cavities. Besides that, the
self-assembly of graphene oxide nanosheets and carbon black nano­
particles on the heating surface increased the roughness by ∼ 4 times,
which provided an increased effective surface area for achieving a
higher heat transfer coefficient.
The concentration ratio had a significant impact on the morphology
of the self-assembly films as graphene oxide, and graphene oxide/carbon
black hybrid (GO:CB 1:1) surfaces featured a similar microporous
structure, whereas graphene oxide/carbon black hybrid (GO:CB 1:5)
film featured a kind of wavy surface. All surfaces provided densely
populated surface cavities for bubble nucleation. Although 3D foam-like
structure of graphene oxide film possessed high contact angle, the
chemical functional groups including carboxylic acid (–COOH) and
hydroxyl (–OH) buried inside the micropores facilitated liquid pumping
through the capillary effect [28,30]. Besides that, as graphene nano­
sheets possess high thermal conductivity, the networks of graphene
oxide nanosheets effectively dissipate the localized heat on hot spots
[50]. Both decent liquid spreading, and lateral heat conduction pre­
vented the expansion of vapor films over the heating surface and
delayed critical heat flux. After the incorporation of carbon black, crit­
ical heat flux was further delayed. The delay in critical heat flux was
highest at the GO:CB concentration ratio of 1:5. The critical heat flux
enhanced by ∼ 35 % over hybrid film with GO:CB concentration ratio of
1:5 compared to graphene oxide-only surface. Thus, a good interfacial
contact in 1:5 graphene oxide/carbon black interconnected network,
subsequently a decent lateral heat conduction, and high capillarity are
considered as the key mechanisms for the highest critical heat flux
enhancement on this hybrid self-assembly surface.
4. Conclusions and outlook
Bubble-induced self-assembly of graphene oxide and graphene
oxide/carbon black dispersions, and its impact on nucleate boiling
performance is presented. Sonication was used to make colloidal dis­
persions of graphene oxide nanosheets and carbon black nanoparticles
at various concentration ratios (GO:CB = 0:1, 1:1, 1:5). Using a custom-
developed boiling test setup, the saturated pool boiling performance of
colloidal dispersions was compared to that of water at atmospheric
pressure. The simultaneous assembly of graphene oxide nanosheets and
carbon black nanoparticles on the heated surface during boiling resulted
in improved nucleate boiling. The augmentation of the heat transfer
coefficient increased with the concentration ratio, peaking at 223% at a
GO:CB concentration ratio of 1:5. Furthermore, for GO:CB concentration
ratios of 0:1, 1:1, and 1:5, colloidal dispersions delayed the critical heat
flow by 135.3%, 135.3%, and 182.4%, respectively.
Surface characterizations revealed that the boiling-induced assembly
of graphene oxide nanosheets and carbon black nanoparticles resulted in
homogeneous 3D porous hybrid coating layers. The new surfaces had
plentiful microcavities for the nucleation of vapor bubbles. The greater
critical heat flux over self-assembly surfaces was explained by a firm
interfacial contact between nanoparticles and nanosheets, lateral heat
conduction and enhanced capillary wicking. Coolant pumping through
the heating surface was aided by the porous deposition layer, which
increased liquid replenishment on hot/dry regions and microlayer
development. It also improved heat dispersion in lateral directions from
hot/dry zones. The vapor film expansion was delayed to higher heat
fluxes owing to a rapid cooling and rewetting of the local hot/dry areas.
This study investigated the boiling heat transfer enhancement of
graphene oxide and carbon black hybrid dispersions at 0.005 wt%
8
International Journal of Thermal Sciences 191 (2023) 108349
concentration. Nucleate boiling enhancement of graphene oxide/carbon
black hybrid dispersions at various concentrations should be investi­
gated in future research.
Nomenclature
All symbols, parameters, and formulas are explained through the
manuscript.
Declaration of competing interest
The authors declare that they have no known competing financial
interests or personal relationships that could have appeared to influence
the work reported in this paper.
Data availability
No data was used for the research described in the article.
Acknowledgments
The authors acknowledge the support provided by the Core Labo­
ratory of Qatar Environment and Energy Research Institute for the
materials characterization.Open access fund provided by Qatar National
Library.
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