HEAT TRANSFER ENGINEERING

, VOL. , NOS. -, –

http://dx.doi.org/./..

Pool Boiling Enhancement through Graphene and Graphene Oxide Coatings

Arvind Jaikumara , Satish G. Kandlikara,b , and Anju Guptac
a
Microsystems Engineering Department, Rochester Institute of Technology, Rochester, NY, USA; b Mechanical Engineering Department,
Rochester Institute of Technology, Rochester, NY, USA; c Chemical Engineering Department, Rochester Institute of Technology,
Rochester, NY, USA

ABSTRACT
Boiling has served as an effective means to dissipate large quantities of heat over small areas.
Graphene, a two-dimensional material, has garnered significant attention of researchers due to its
excellent thermal properties. In this study, copper test chips are dip coated with a solution consisting
1-4 of graphene oxide and graphene and its pool boiling performance with distilled water at atmospheric
4 notes: pressure was investigated. The surfaces were characterized using X-ray diffraction, Fourier transform
infrared spectroscopy, thermogravimetric analysis, and scanning electron microscopy which con-
5-6 firmed the presence of graphene and graphene oxide. The contact angles measured on the coated
2 notes: surfaces indicated hydrophobic wetting behavior. Four heat transfer surfaces were prepared with dip
coating durations of 120 s, 300 s, 600 s, and 1200 s, respectively. A Critical Heat Flux (CHF) of 182 W/cm2
and a heat transfer coefficient (HTC) of 96 kW/m2 °C was obtained with the shortest coating dura-
tion which translated to an enhancement of 42% in CHF and 47% in HTC when compared to a plain
7-8 uncoated surface under similar conditions. Contact angle changes were not seen to be responsible,
2 notes: although roughness was seen as an influencing factor contributing to the enhancement. Further stud-
ies are needed to explain the enhancement mechanism.

Introduction header configurations and moving parts and can be read-

ily employed to cool high heat flux devices. Critical Heat
The rapid developments in microelectronics and micro-
Flux (CHF) and Heat Transfer Coefficient (HTC) are two
electromechanical systems has resulted in cooling chal-
parameters that are often used to characterize the pool
lenges that are at the micro/nanoscale [1]. Every succes-
boiling performance. The CHF is the upper boiling heat
sive generation of electronic devices are characterized by
transfer limit while the HTC determines the effective-
their increased packaging density and power consump-
ness of the surface to dissipate heat. This study is directed
tion. Furthermore, the physical volume of these devices is
towards increasing both the CHF limit and HTC for
shrinking which places an increasing demand for efficient
the surfaces developed. A brief description of the pas-
cooling. While air cooling can cater to only low power
sive geometries developed by previous researchers is high-
density components, liquid cooling has shown promise
lighted before introducing the scope of the current work.
to meet the shortcomings of air cooling. However, single-
Separate liquid-vapor pathways is an enhancement
phase cooling techniques involve large fluid temperature
mechanism identified in recent works [5–8] in which the
differences and high pressure drops which impose severe
liquid re-wetting pathways are unobstructed by the bub-
design constraints for these systems [2]. Two-phase cool-
ble departure routes, which ensures continuous supply
9-10 ing systems are attractive alternatives that are capable
2 notes: of liquid to the nucleation sites delaying the CHF and
of removing large amounts of heat over a small foot-
increasing the HTC. Kandlikar [5] identified evapora-
print while keeping the temperature differences under
tion momentum force as a major influence to control the
the desired limit [3,4]. These techniques offer a plausi-
bubble trajectory on the heater surface to facilitate sep-
ble solution to cool high power density components. The
arate liquid-vapor pathways. A contoured fin was fab-
advantages of a two-phase cooling system have garnered
ricated to remove vapor along the contour of the land
keen attention of researchers to develop passive geome-
11-12
with the re-wetting liquid supply to the nucleation sites
tries to enhance the performance. Pool boiling, however,
2 notes: occurring through the sidewalls of the fins. This efficient
is a simple technique that does not involve complicated

CONTACT Professor Satish G. Kandlikar sgkeme@rit.edu Mechanical Engineering Department, Rochester Institute of Technology,  Lomb Memorial Dr.,
Rochester, NY, , USA
Color versions of one or more of the figures in this paper can be found online at www.tandfonline.com/uhte.
©  Taylor & Francis Group, LLC

13-15 mechanism resulted in a CHF of 300 W/cm2 at a
3 notes: wall superheat of 4.9°C, which is remarkable con-
sidering that no porous coatings were employed. To
improve the performance further using separate liquid-
vapor pathways, Jaikumar and Kandlikar [6,7] developed
three microchannel surfaces identified as (i) sintered-
throughout, (ii) sintered-fin-tops, and (iii) sintered-
16-18
channels. These surfaces were developed using screen
3 notes: printing and sintering on an open microchannel surface.
A record CHF of 420 W/cm2 at a wall superheat of 1.7°C
19 with an HTC of 2.9 MW/m2 °C was achieved. Another
5/25/2021
asad Sonavane heat transfer surface comprises nucleating regions and
feeder channels was developed by Jaikumar and Kandlikar
[8]. This configuration was designed by spacing the nucle-
ating regions based on the departure bubble diameter and
20-22 the hydrodynamic stability theory, and providing feeder
3 notes: microchannels to supply liquid to nucleating regions. This
configuration resulted in a CHF of 394 W/cm2 at a wall
superheat of 5.5°C and an HTC of 713 kW/m2 °C.
Altering the liquid wettability by texturing surfaces
has been explored by various research groups. Betz et al.
[9] showed that creating islands of hydrophobic regions
surrounded by hydrophilic regions significantly enhances
the heat transfer performance. Chu et al. [10] fabri-
cated microstructures on a silicon substrate and identified
roughness induced wettability as the main enhancement
mechanism. O’Hanley et al. [11] created a range of sur-
faces to study the separate effects of roughness, wettability
23-26
4 notes: and porous structures on the pool boiling performance.
The microstructures and coatings discussed earlier,
have contributed to a significant increase in CHF or HTC.
However, these enhancement features are either larger
than 100 μm deep or involve complex fabrication process
27 that are prohibitive. They further offer significant thermal
resistance which reduces the heat dissipation capability of
asad Sonavane
the structured/engineered surfaces. In the current study,
we explore the possibility of developing coatings that
28-29
are less than 10 μm in thickness to increase the boiling
2 notes: heat transfer performance. Graphene, a two-dimensional
layered material, has gathered interest in the field of heat
30-31 transfer enhancement due to its wetting behavior and is
2 notes:
an active research topic. Previous research in the field of
graphene as an enhancement for two-phase heat transfer
coatings is mainly focused on boiling colloids and its
resulting self-assembly characteristics.
Table 1 summarizes the heat flux obtained by boiling
colloidal graphene and graphene oxide (GO) by previous
researchers. Ahn et al. [12] boiled colloidal reduced
graphene oxide (RGO) to study the effect of graphene
base layer deposition due to self-assembly. Kim et al. [13]
experimentally investigated the effects of concentration
of GO colloids on a nichrome wire heater and concluded
that GO deposition on the surface forms a smooth
HEAT TRANSFER ENGINEERING 1275
Table . Literature summary of high performing surfaces with GO
and graphene colloids.
Author’s Heat flux (W/cm ) Enhancement mechanism
Ahn et al. []  Base layer deposition
Kim et al. []  Laminated film
Ahn et al. []  Wetting characteristics
Park et al. []  Self-assembly characteristics
laminated film which results in an increase in CHF.
Ahn et al. [14] also conducted an experimental study to
understand the effect of RGO flake aggregation on CHF
on a one and two-sided coating on Ni-Cr wire. Park et al.
[15] further demonstrated that the nanofluids contain-
ing graphene nanosheets can be exploited to maximize
CHF by the self-assembly characteristic of nanofluids.
However, the capillarity and surface wettability effects by
boiling nanofluids are still not fully understood. Funda-
mental understanding of the underlying bubble dynamics
can be achieved by directly coating a GO or graphene
layer on the substrate.
Graphene has shown promise in heat transfer enhance-
ment to improve the CHF and HTC during pool boiling.
In this paper, we explore the possibility of improving
the pool boiling performance by coating graphene or
GO as opposed to boiling the graphene-based colloids.
Furthermore, the coatings will provide an insight on
the underlying boiling mechanism. An electrochemical
exfoliation process involving cleaving and reduction in a
single step was used to produce graphene and GO solution
[16]. A simple dip coating process transfers the graphene
and GO coating on a copper substrate. The character-
ization of the coated surface was conducted by X-ray
diffraction (XRD), Fourier Transform Infrared (FTIR)
spectroscopy, thermogravimetric analysis (TGA), and
scanning electron microscopy (SEM). The pool boiling
performance with distilled water at atmospheric pressure
is obtained for the surfaces developed. High speed imag-
ing was conducted to understand the underlying boiling
mechanism.
GO/Graphene preparation
The solution containing GO and graphene was gener-
ated as described in Ref. [16]. The GO/graphene col-
loidal solution was prepared in an electrochemical cell
in which cleaving of the graphite electrode and reduc-
tion of the resulting GO solution were carried out in
a single step. An electrochemical process was employed
to generate the solution in a single step using oxygen
embrittlement. The cell consisted of graphite (2 cm ×
2 cm; and a thickness of 0.70 cm) as the anode and
the copper test chip (1.7 cm × 1.7 cm copper test sec-
tion) as the cathode (Figure 1). A detailed explanation
 1276 A. JAIKUMAR ET AL.

Figure . Schematic of the electrochemical test section used to prepare GO/graphene solution.

for the test chip is available in Ref. [6]. The electrolyte

consisted of carbon tetrachloride and deionized water.
32
5/25/2021 The percentage of carbon tetrachloride used for produc-
asad Sonavane ing the G/GO solution was 10% by volume. A poten-
tial was applied between the electrodes which introduced
a current density of 300 mA/cm2 . This current density
was sufficient to cause the oxidation of water to produce
oxygen at the graphite anode to cleave the surface into
graphene. The gap between the cathode and anode was
maintained at 1 mm by a Teflon spacer to hold the elec-
trodes firmly in position. Electrical contact was estab-
lished with insulated copper leads. As a result of the pro-
cess, the temperature of the bath increased from 293 K to
343 K.

33-34
2 notes: Dip coating
The copper test section (see Figure 2(b)) was thoroughly
cleaned in a 6M hydrochloric acid solution and washed
in distilled water before the dip coating process. The test
section was prepared to ensure that only the 1 cm2 boil-
ing surface was exposed to the colloidal solution and
35-36
the rest of the chip was covered with a layer of Kaptons
2 notes: tape. The exposed 1 cm2 of the copper test section was
Figure . (a) Schematic of the pool boiling experimental setup []
immersed in the GO/graphene solution for different dura-
(b) Copper test section used in this study.
tions. Four chips were prepared by dip coating for 120 s,
37-38
2 notes:
300 s, 600 s, 1200 s, respectively. The dip coating dura- Pool boiling experimental setup
tion of 60 s yielded nonuniform coating and was not stud-
ied further. The thickness of the coatings was determined An experimental setup similar to Jaikumar and Kand-
39-41 using a laser confocal microscope (LCM) and is summa- likar [6] was used in the pool boiling tests (Figure 2a).
3 notes:
rized in Table 2. The coating thickness was obtained by
Table . Summary of dip coated test chips with coating duration
calculating the average step height between the coated
42-43 and thickness.
2 notes: and non-coated regions along the four edges of the test
chip. It must be noted that the thickness was obtained Chip # Coating duration (s) Thickness (µm)
only at the edge locations between the coated and non-   .
coated regions. The variability in thickness along different   .
  .
regions of the test chip was characterized using the height   .
map obtained using the LCM.
 HEAT TRANSFER ENGINEERING 1277

The setup consisted of a ceramic chip holder encapsu- The boiling surface temperature was obtained by using
lating the test chip on all sides except the boiling region eq. (1) and is given by,
on the top and the copper heater block contact region at  
 x1
the bottom. This ensures minimal heat losses to the atmo- Twall = T1 − q (3)
kCu
sphere during testing. A detailed description of the cop-
per test section used in this study has been previously where Twall is the boiling surface temperature and x1 is the
reported [6] and is shown in Figure 2(b). A quartz glass distance between the boiling surface and thermocouple
water bath was assembled over the test chip and was held T1 ; x1 was 1.5 mm for all the test surfaces.
44-47
4 notes: between the middle and bottom garolite place. The glass
water bath was chosen to aid visualization. A rubber gas-
Test surface characterization
ket was introduced between the quartz water bath and the
test section to ensure a good seal. A tight compression The coated surfaces were characterized using X-ray
seal was achieved by fastening four bolts that connected diffraction (XRD), Fourier transform Infrared spec-
the middle and bottom garolite plates. The garolite plate troscopy (FTIR), thermogravimetric analysis (TGA),
was further mounted on a Z-axis stage (not shown in fig- and scanning electron microscopy (SEM). The results
ure) to facilitate movement to establish contact with the obtained with each characterization process are presented
test heater block. A water reservoir was assembled over below.
the middle garolite plate to replenish water in the quartz
bath upon high rates of evaporation encountered during
XRD
the testing process. The top aluminum plate was provided
with two openings for the saturation thermocouple probe Material information on the chips was obtained using a
48-49
and a 60-VDC, 200 W capacity cartridge heater to main- Rigaku DMAZ-IIB XRD equipment. The GO/graphene
2 notes: tain the water in the reservoir at saturation temperature. solution was dip coated on the copper test section and
The bottom section of the test setup consisted of a cop- allowed to dry. The XRD of the air dried sample is shown
per heater block with four, 200 W cartridges inserted into in Figure 3. GO has a characteristic two theta reflection
them. The heater block was housed on a ceramic sleeve fit- arising from (002) plane that depends on the number of
ted into an aluminum base. Furthermore, the aluminum graphene layers and the distance between layers. Besides
base was supported on four compression springs to pro- GO peaks (A, B and C), the other 2θ transitions (D, E, F,
vide the required degree of freedom to establish contact G, H) are due to copper as reported in Joint Committee
50-51
with the test section and also to account for any expansion on Powder Diffraction Standards (JCPDS) Copper: data
2 notes: during the testing procedure. The bottom garolite plate file # 04–0836.
was lowered to make contact with the copper heater block.
A grafoil paper was used as a thermal interface material to
FTIR
minimize contact resistance.
A National Instruments cDaq-9172 data acquisition The FTIR spectrum of GO/graphene showed peaks at
system with NI-9213 temperature module was used to 3290 cm−1 , 1624 cm−1 , and 1411 cm−1 as seen in Figure 4.
record the temperature. A LabVIEWVR virtual instru- The peak at 3290 cm−1 was attributed to O-H stretching
ment displayed and calculated the real-time surface tem-
perature and heat flux.
The heat flux to the test section was calculated using
52 Fourier 1D conduction equation
5/25/2021
asad Sonavane
dT
q = −kCu (1)
dx

The temperature gradient dT/dx was calculated using

the three point backward Taylor’s series approximation

dT 3T1 − 4T2 + T3
= (2)
dx 2x

where, T1 , T2 , T3 are the temperatures corresponding to

the top, middle, and bottom of the test chip under study. Figure . XRD obtained with chip .
 1278 A. JAIKUMAR ET AL.
Figure . FTIR results obtained with chip  with background cor-
rected spectrum.
from water. The peak is strong and it overlaps with
C-H stretching at 2930 cm−1 . The peak at 1624 cm−1 was
attributed to the presence of aromatic rings (C = C) and
the peak at 1411 cm−1 was due to C-H bending. The aro-
matic CH2 and C-O peaks overlap causing them to be
absent in their expected locations. These results show the
presence of carboxyl group in the GO/graphene coated on
copper.
TGA
Composition of the GO/graphene solid material was
studied using a TA Instruments Q500 Thermogravimet-
ric analyzer (TGA). The sample was heated at 5°C/min
53-54
from 25°C to 500°C under nitrogen atmosphere in an
2 notes:
aluminum hermetic pan. The resultant thermograph
(Figure 5) demonstrates the loss of mass of the sample
as a function of increasing temperature and revealed the
55-56 presence of both graphene and GO. As indicated on the
2 notes: thermograph, GO being less thermally stable, starts to
lose mass below 100°C which is usually associated with
57
5/25/2021
asad Sonavane
Figure . TGA results obtained with dip coated GO/graphene solu-
tion on an aluminum hermetic pan.
removal of adsorbed water and gas molecules. The loss of
mass at 200°C is attributed to the decomposition of GO,
yielding CO and CO2 as the by-products. Similar results
were reported in Refs. [17,18]. The loss of mass at higher
temperatures corresponds to the remaining unstable
carbon from graphene [19]. It is reported that complete
decomposition of graphene occurs post 800°C which
is beyond the measuring capability of the aluminum
hermetic pan used in this study [20]. The percentage
composition of GO and graphene were 12.5% and 87.5%,
respectively.
SEM
The morphology of the substrates was studied using a
JSM-6400V scanning electron microscope (SEM), JEOL,
Ltd., Tokyo, Japan at an accelerating voltage of 15 kV.
Figure 6 shows the SEM micrographs of GO/graphene
coated on the copper test section at different magnifica-
tions. At lower magnification of 250×, graphene demon-
strated mixed morphology- granules like structure that
are approximately 1 µm wide. The structures appear to
be in columns running parallel to each other (Figure 6a).
The substrate when titled at 70°, showed vertically aligned
graphene microstructures structures that were approx-
imately 5 μm tall when measured at 1800× magni-
fication (Figure 6b). When a magnification of 650×
(Figure 6c) was employed, sheet like structures are seen
which is in agreement to previously reported SEMs on
graphene coatings [14]. The presence of carbon and oxy-
gen coating on copper substrate was further confirmed
by energy-dispersive X-ray (EDX) analysis represented in
Figure 6(d).
Contact angle
The contact angle was measured using a VCA Optima
instrument by dropping 2 μL droplets on chips 1 – 4.
The dip coated test chips exhibited hydrophobic contact
angles. Chip 1 was segmented into a 4 × 4 matrix and
the static contact angle was measured in each segment as
shown in Figure 7(a). The figure shows the hydrophobic
contact angles was between 90° and 122° for this surface.
Chip 2 also had a hydrophobic surface with the contact
angles measuring between 117° and 128° throughout as
seen in Figure 7(b). Similar hydrophobic contact angles
were observed on chip 3 and 4. Since the contact angles
were consistently hydrophobic, we measured the rough-
ness values (Ra ) for the four chips to explain the CHF
enhancement.
The morphology of chip 1 and chip 2 obtained
using a scanning laser confocal microscope are shown
in Figure 7(c) and (d), respectively. Figure 7(e) shows
the variation of roughness with thickness for chip 1–4.
Changes in roughness may be one possible explanation

Figure . SEM micrographs showing GO/graphene structures coated on chip  obtained at a magnification of (a) × (b) × (c) ×
(D) EDX analysis conducted on chip .
for the CHF enhancement. Another explanation could
be due to the presence of both graphene and graphene
oxide. This is in agreement with the TGA results obtained
which suggests that the coated surfaces consisted of both
graphene and GO.
Uncertainty analysis
An uncertainty analysis was conducted similar to Jaiku-
mar and Kandlikar [6]. The uncertainty in heat flux arises
due to three contributing factors which are the thermo-
couple calibration, thermal conductivity of copper, and
the distance between the thermocouples. The method
of partial sums was used to calculate the uncertainty
for each contributing factor. The thermocouple measure-
ments had the largest factor of uncertainty. Each ther-
mocouple was individually calibrated in the testing tem-
perature range. Thermocouple accuracy and precision
errors were accounted for while calculating the uncer-
tainty. Based on each contributing factor the total uncer-
tainty in heat flux and HTC is calculated. The uncer-
tainty was indicated as error bars in each data marker in
Figures. 8 and 9. At high heat fluxes, which is the main
interest of this study, a maximum uncertainty of 6% was
obtained in CHF for all the surfaces investigated here.
Results
The pool boiling performance of the four dip coated
surfaces (see Table 2) is investigated here. The main
HEAT TRANSFER ENGINEERING 1279
objective of this study was to obtain an experimental
database for surfaces coated with a mixture of graphene
and GO. The study also aims to understand the effect
of coating thicknesses on the pool boiling performance.
A simple dip coating process was employed to transfer
the colloidal solution onto the copper substrates and
subsequently air dried to form a stable layer. Pool boiling
tests were conducted with distilled water at atmospheric
pressure.
A typical pool boiling curve which relates the heat flux
dissipated and the wall superheat was used to character-
ize the performance of the surfaces investigated. The wall
superheat is the difference between the surface tempera-
ture and the saturation temperature of the boiling liquid.
The test chips investigated here were pushed to CHF to
establish the maximum heat dissipating capability of the
coated surfaces. An enhancement is achieved when the
pool boiling curve is shifted to the left when compared to
a plain uncoated baseline chip. The focus of this current
study was to achieve an increase in CHF and HTC when
compared to the baseline chip. The plain uncoated base-
line chip attained a CHF of 128 W/cm2 at a wall superheat
of 20°C with a HTC of 65 kW/m2 °C.
Figure 8 shows the pool boiling curves obtained
with GO/graphene surfaces. Chip 1 reached a CHF of
182 W/cm2 at a wall superheat of 19°C. This translated
to an enhancement of 42% in CHF compared to a plain
chip. Chip 2 had a CHF of 128 W/cm2 while chip 3
and 4 had CHF of 124 W/cm2 . The CHF of chip 2,
3, and 4 are very close to the baseline chip indicating
1280 A. JAIKUMAR ET AL.
Figure . Contact angles and height map measured on (a, c) chip  (b, d) chip  and (e) Variation of roughness with coating thickness for
chips –.
that the dip coating process resulted in multiple layers of
graphene and GO being deposited. Closer examination of
the results revealed that thinner coatings performed bet-
ter than thicker coatings.
Figure 9 shows the heat transfer performance plot
where the HTC is plotted against the heat flux. The
capability of a surface to efficiently dissipate heat can be
established from this plot. The general trend indicated
that HTC increased with wall superheat. Chip 1 had the
highest HTC of 96 kW/m2 °C which translated to an
enhancement of 47% when compared to a plain chip.
Chip 2, 3 and 4 had HTC’s of 86 kW/m2 °C, 64 kW/m2 °C
and 63 kW/m2 °C.
Figure 10 shows the effect of coating thickness on
the CHF. The dip coatings durations were varied for the
four chips to obtain coating thicknesses of 1 μm, 5 μm,
7.5 μm, and 8.6 μm for chip 1, 2, 3, and 4, respectively.
Note that the coating thicknesses were average values at
the edge location separating the coated and non-coated
regions. For chip 1, the thickness seems to vary at the
 HEAT TRANSFER ENGINEERING 1281

Figure . Pool boiling curves obtained for chip – with distilled Figure . Effect of coating thickness on the CHF.
water at atmospheric pressure.

central regions of the chip as seen from the LCM images identified as the underlying heat transfer enhancement
of the height plots. This is further substantiated by the mechanism. First, the bubble dynamics on chip 1 and
increase in roughness measured on this chip. The figure plain chip were compared to observe any visible change
illustrates that the thinnest coating with the highest in the bubble nucleation and departure patterns. The
58-59 roughness had the best performance with a CHF of images were obtained at a heat flux of ∼15 W/cm2 .
2 notes: 182 W/cm2 . With an increase in thickness the number of Figure 11 shows the bubble sequence for a chip 1 and a
graphene layers is expected to increase. Chips 2, 3, and plain chip from nucleation to departure at the same time
4 do not exhibit significant variation in the hydrophobic step (except for Figure 11 (d) and (h)). Figure 11 (a-d)
60
contact angles and have lower roughness values which shows the nucleation, growth, and departure of a bubble
results in lower CHF values. originating on chip 1. The total time taken for this cycle
asad Sonavane was 8.25 ms. Similar nucleation, growth, and departure
sequence was obtained for a plain chip as shown in
High-speed images and discussion Figure 11 (e-h). The corresponding cycle time for the
High-speed images were captured using a Photron- plain chip was 13.25 ms. The images indicate that the
61-62 Fastcam high-speed camera. Change in wettability was bubbles grew faster on a GO/graphene-coated surface due
2 notes: to the hydrophobic nature of the surface. For example, at
t = 7.5 ms the contact line has almost completely receded
for chip 1 whereas on the plain chip the contact line is
still seen to occupy a significant area on the copper test
chip.
The images indicate very similar behavior between
the plain chip and GO/graphene-coated surface. The
images further suggest that bubbles departing on a
63-64
GO/graphene-coated surface were smaller than that on
2 notes: a plain surface. The hydrophobic nature of the coat-
ings influenced the departure diameters to be smaller
and resulted in faster growth rates. The bubble depar-
ture diameter was measured to be 1.39 mm on chip
65-66 1 and the corresponding bubble departure diame-
2 notes: ter for a plain chip was 2.06 mm. However, fur-
ther analysis is required to confirm the enhancement
mechanism taking into account the surface morphol-
Figure . Heat transfer performance curves obtained with chip ogy. This is currently being pursued in the author’s
–. laboratory.
1282 A. JAIKUMAR ET AL.

Figure . Bubble nucleation and departure pattern obtained with (a-d) chip  (e-h) plain chip.

Conclusions iv) The pool boiling performance resulted in a CHF of

182 W/cm2 and a HTC of 96 kW/m2°C with chip
A colloidal solution containing graphene and graphene
1 which translated to an enhancement of 42% in
oxide was prepared in an electrochemical cell using oxy-
CHF and 47% when compared to a plain uncoated
gen embrittlement of a graphite electrode. The mixture
chip. Roughness augmented wettability change was
comprising graphene and GO was transferred to the cop-
identified as the enhancement mechanism.
per test section using a simple dip coating process. Four
v) The effect of coating thickness was also studied.
heat transfer surfaces were prepared by dip coatings for
Four heat transfer surfaces (chip 1–4) with coating
120 s, 300 s, 600 s, and 1200 s, respectively. Pool boiling
thicknesses of 1 μm, 5 μm, 7.5 μm and 8.6 μm
tests were conducted with distilled water at atmospheric
were tested for their pool boiling performance.
pressure. The following conclusions are drawn from this
Chip 1 with the thinnest coating had the highest
study:
CHF while an increase in coating thickness sig-
i) The test chips were characterized using XRD, FTIR,
nificantly hampered the boiling performance. This
TGA, and SEM. XRD spectrum identified the char-
parametric trend can be explained by the rough-
acteristic 2θ peak for GO. FTIR and TGA showed
ness change induced by the variation in thickness
the presence of both graphene and GO mixture in
as reported previously.
the prepared electrochemical solution.
vi) High-speed images captured revealed similar bub-
ii) SEM images showed granule like structures that
ble nucleation and departure patterns for chip 1
were approximately 1 μm wide. Furthermore, at a
and a plain uncoated chip. The time steps however
tilt angle of 70° vertically aligned graphene struc-
were different. Chip 1 took 8.25 ms from nucleation
tures that were approximately 5 μm tall were
to departure while the plain chip took 13.75 ms for
observed. It can be said that the coating technique
the same cycle. This observation suggested that the
employed dictated the morphology of the surface.
bubbles originating on GO/graphene surface took
EDX X-ray analysis conducted on chip 1 also con-
1.6 times lesser time than a bubble departing from
firmed presence of carbon and oxygen in the coated
a plain chip due to the hydrophobic nature of the
test surfaces.
coated surfaces. The measured bubble departure
iii) Contact angles for the coated surfaces (chip 1–4)
diameters for chip 1 and the plain uncoated sur-
were measured. All the chips exhibited hydropho-
face were 1.39 mm and 2.06 mm, respectively. The
bic contact angles. Therefore, the effect of wet-
smaller diameter is expected to influence the liquid
tability could not explain the CHF enhancement
re-wetting pathways on the test chip. The change
observed here. Instead, we investigated the effect
in hydrophobic contact angles and the roughness
of roughness on the chips. The thinnest coating of
induced is also expected to affect the relative mer-
1 µm had the highest roughness while the rough-
its of nucleation and re-wetting flow patterns on the
ness of chips 2, 3, and 4 was significantly lower.
heater surface.

Nomenclature
CHF Critical heat flux
FTIR Fourier transform infrared spectroscopy
GO Graphene oxide
HTC Heat transfer coefficient
kCu thermal conductivity of copper, W/m°C
q” heat flux, W/m2
Ra roughness, m
SEM Scanning Electron Microscopy
Twall wall temperature,°C
TGA Thermogravimetric analysis
x distance, m
XRD X-ray diffraction
Acknowledgments
This work was conducted in the Thermal Analysis, Microflu-
idics and Fuel Cell Laboratory in the Mechanical Engineering
Department at Rochester Institute of Technology, Rochester,
NY. The authors would like to thank Dr. K.S.V. Santhanam for
manufacturing the graphene solution. The authors would also
like to thank Dr. Surendra Gupta for his assistance with the
XRD equipment. The authors gratefully acknowledge the finan-
cial support provided by the National Science Foundation under
CBET Award No. 1335927.
Notes on contributors
Arvind Jaikumar is currently
pursuing his Ph.D. in Microsys-
tems Engineering in the Thermal
Analysis Microfluidics and Fuel
Cell Laboratory at Rochester
Institute of Technology (RIT).
He obtained his bachelors in
mechanical engineering from
Visvesvaraya Technological
University, Karnataka, India,
and his Master of Science in
mechanical engineering from
RIT, Rochester, USA. He is cur-
rently engaged in creating micro/nanostructures and coatings
for enhancement in pool boiling heat transfer.
Satish G. Kandlikar is at RIT
since 1980 and is currently the
Gleason Professor of Mechani-
cal Engineering. He received his
Ph.D. degree from the IIT Bom-
bay in 1975. He has worked
extensively in the area of flow
boiling and CHF phenomena at
microscale, single-phase flow in
microchannels, electronics cool-
ing, and water management in
PEM fuel cells. He has published
over 400 journal and conference
papers. He is the recipient of the 2012 ASME Heat Transfer
HEAT TRANSFER ENGINEERING 1283
Memorial Award. His recent work on pool and flow boiling has
produced exceptionally high heat fluxes along with very high
heat transfer coefficients.
Anju Gupta is currently an
Assistant Professor in the Chem-
ical Engineering program and
Principal Investigator of the
Soft Nanomaterials Labora-
tory at Rochester Institute
of Technology. Her research
interests include formation of
microemulsions, self-assemblies,
nanostructured composites and
their characterization using ther-
mal analysis (DSC, TGA) and
electron microscopy (cryogenic
SEM and TEM) techniques for Biomedical and Environmental
applications.
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Annotations

Pool Boiling Enhancement through Graphene and Graphene

Oxide Coatings
Jaikumar, Arvind; Kandlikar, Satish G.; Gupta, Anju

01 Prasad Sonavane Page 1

25/5/2021 20:29
Test chips were dip-coated.

02 Prasad Sonavane Page 1

25/5/2021 20:29

03 Prasad Sonavane Page 1

25/5/2021 20:30

04 Prasad Sonavane Page 1

25/5/2021 20:30
Techniques (processes/equipments) needed to characterize surfaces.

05 Prasad Sonavane Page 1

25/5/2021 20:31

06 Prasad Sonavane Page 1

25/5/2021 20:31
Contact angles measured indicated hydrophobic wetting behaviour.

07 Prasad Sonavane Page 1

25/5/2021 20:32

08 Prasad Sonavane Page 1

25/5/2021 20:33
Roughness was seen to be an influencing factor for CHF enhancement. Contact angle was not.

09 Prasad Sonavane Page 1

25/5/2021 20:40
One of the recently identified enhancement mechanisms is the existence of separate liquid-vapour
pathways. References are given.
10 Prasad Sonavane Page 1
25/5/2021 20:38

11 Prasad Sonavane Page 1

25/5/2021 20:44

12 Prasad Sonavane Page 1

25/5/2021 20:45
Very interesting. A contoured fin was fabricated.

13 Prasad Sonavane Page 2

25/5/2021 20:53

14 Prasad Sonavane Page 2

25/5/2021 20:54
Useful table summarizing the results obtained using rGO and GO as colloids with references.

15 Prasad Sonavane Page 2

25/5/2021 20:44

16 Prasad Sonavane Page 2

25/5/2021 20:46

17 Prasad Sonavane Page 2

25/5/2021 20:46
Technique to develop microchannel s/fs.

18 Prasad Sonavane Page 2

25/5/2021 20:46

19 Prasad Sonavane Page 2

25/5/2021 20:47
A record CHF was achieved using microchannel s/fs.

20 Prasad Sonavane Page 2

25/5/2021 20:55
21 Prasad Sonavane Page 2
25/5/2021 20:48

22 Prasad Sonavane Page 2

25/5/2021 20:48
In this configuration (Ref. 8) nucleating regions were spaced based on the departure bubble
diameter.

23 Prasad Sonavane Page 2

25/5/2021 20:49

24 Prasad Sonavane Page 2

25/5/2021 20:57
Electrochemical exfoliation involving cleaving and reduction was used to produce graphene and GO
solution (Ref. 16).

25 Prasad Sonavane Page 2

25/5/2021 20:49
Comments on work of Betz, Chu, and O'Hanley.

26 Prasad Sonavane Page 2

25/5/2021 20:56

27 Prasad Sonavane Page 2

25/5/2021 20:58

28 Prasad Sonavane Page 2

25/5/2021 20:51

29 Prasad Sonavane Page 2

25/5/2021 20:51
Advantage of a coatings over other enhancement techniques.

30 Prasad Sonavane Page 2

25/5/2021 21:03

31 Prasad Sonavane Page 2

25/5/2021 21:03
A section on GO/Graphene preparation
32 Prasad Sonavane Page 3
25/5/2021 21:05
Experimental setup.

33 Prasad Sonavane Page 3

25/5/2021 21:05

34 Prasad Sonavane Page 3

25/5/2021 21:06
A section on dip-coating.

35 Prasad Sonavane Page 3

25/5/2021 21:06

36 Prasad Sonavane Page 3

25/5/2021 21:06
Kaptons tape can be used to isolate the s/f that needs to be exposed to the fluid.

37 Prasad Sonavane Page 3

25/5/2021 21:09

38 Prasad Sonavane Page 3

25/5/2021 21:09
A section on experimental setup.

39 Prasad Sonavane Page 3

25/5/2021 21:07
LCM is used to determine the thickness of the coatings.

40 Prasad Sonavane Page 3

25/5/2021 21:07

41 Prasad Sonavane Page 3

25/5/2021 21:08

42 Prasad Sonavane Page 3

25/5/2021 21:08
Coating thickness variation with dip-coating times.
43 Prasad Sonavane Page 3
25/5/2021 21:08

44 Prasad Sonavane Page 4

25/5/2021 21:13

45 Prasad Sonavane Page 4

25/5/2021 21:13
A quartz water bath was used to aid visualization.

46 Prasad Sonavane Page 4

25/5/2021 21:19

47 Prasad Sonavane Page 4

25/5/2021 21:19
Sections on each of the techniques used to characterize the s/f.

48 Prasad Sonavane Page 4

25/5/2021 21:15

49 Prasad Sonavane Page 4

25/5/2021 21:15
A cartridge heater was used to maintain the temperature at saturation.

50 Prasad Sonavane Page 4

25/5/2021 21:17

51 Prasad Sonavane Page 4

25/5/2021 21:17
Function of compressions springs at base explained.

52 Prasad Sonavane Page 4

25/5/2021 21:21
A, B, and C belong to GO.

53 Prasad Sonavane Page 5

25/5/2021 21:30
54 Prasad Sonavane Page 5
25/5/2021 21:31
EDX can be used to further confirm the presence of carbon and oxygen coating.

55 Prasad Sonavane Page 5

25/5/2021 21:34

56 Prasad Sonavane Page 5

25/5/2021 21:35
Instrument to measure contact angle.

57 Prasad Sonavane Page 5

25/5/2021 21:27
GO starts decomposing after 200C leading to CO and CO2.

58 Prasad Sonavane Page 8

25/5/2021 21:41

59 Prasad Sonavane Page 8

25/5/2021 21:42
Thinnest coating with the highest roughness had the best performance.

60 Prasad Sonavane Page 8

25/5/2021 21:42

61 Prasad Sonavane Page 8

25/5/2021 21:46

62 Prasad Sonavane Page 8

25/5/2021 21:47
Growth rate was higher on GO s/fs.

63 Prasad Sonavane Page 8

25/5/2021 21:46

64 Prasad Sonavane Page 8

25/5/2021 21:47
Bubble departure diameteers were lower for GO s/fs.
65 Prasad Sonavane Page 8
25/5/2021 21:48
The ratio of diameters seems equivalent to CHF enhancement.

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25/5/2021 21:47