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SIGNIFICANT BOILING ENHANCEMENT WITH SURFACES COMBINING

SUPERHYDROPHILIC AND SUPERHYDROPHOBIC PATTERNS


Amy Rachel Betz1, James R. Jenkins2, Chang-Jin “CJ” Kim2 and Daniel Attinger1
1
Columbia University, New York, NY, USA
2
University of California, Los Angles (UCLA), CA, USA

ABSTRACT experiments. We showed that a hydrophilic network with


In this work we describe the manufacturing and hydrophobic islands can increase CHF by 65% and HTC by
characterization of patterned surfaces with large spatial 100% compared to a hydrophilic wafer with a wetting angle
contrast in wettability. We find drastic enhancement of pool of 7º. We also found that increasing the wettability contrast
boiling performance in water. In comparison to a increased the CHF. In [11] we varied the size of the patterns
hydrophilic SiO2 surface with a wetting angle of 7º, surfaces as well as the connectivity of the hydrophobic and
combining superhydrophilic and superhydrophobic patterns hydrophilic patterns. Hydrophilic surfaces with hydrophobic
can quadruple the heat transfer coefficient (HTC). islands were called hydrophilic networks meaning that any
Superhydrophilic surface with hydrophobic islands can two hydrophilic regions could be joined without passing
increase the critical heat flux (CHF) by 80%. This over a hydrophobic zone. Hydrophobic surfaces with
performance enhancement is important for applications such hydrophilic islands were called hydrophobic networks. We
as electronics cooling, because the increased HTC allows a found that hydrophilic networks increased both the HTC
greater amount of heat to be removed at a lower wall and CHF while hydrophobic networks only increased the
superheat. HTC at low values of superheat. In the present work we
focus on these promising hydrophilic networks, further
exploring the effects of wettability contrast using nano-
INTRODUCTION fabrication to create superhydrophilic networks with
Boiling is an efficient process to transfer large amounts superhydrophobic islands. Our intuition is that the
of heat at a prescribed temperature because of the large superhydrophilic surfaces might improve rewetting [12] and
latent heat of vaporization. The term flow boiling describes the superhydrophobic islands might improve nucleation
the boiling of liquids forced to move along hot surfaces, [13]. We characterize the pool boiling performance of these
while in pool boiling, the topic handled in this paper, the surfaces and compare it to state-of-the-art enhanced
liquid is stagnant and in contact with a hot solid surface [1]. surfaces.
Pool boiling performance is measured with two parameters:
the heat transfer coefficient (HTC) and the critical heat flux
(CHF). The CHF is measured by increasing the surface DESIGN AND MANUFACTURING
temperature until a transition from high HTC to very low We designed our superhydrophilic surfaces with
HTC occurs, which signifies the formation of a vapor film superhydrophobic patterns on the basis of our recent work
insulating the liquid from the heated surface, a phenomenon [11] where micromanufactured surfaces with spatial
called dry out. contrasts of wettability exhibited increased pool boiling
As of today, the performance of boiling surfaces has performance. All the surfaces investigated in the present
been increased by using wicking structures to prevent dry work are superhydrophilic with either hydrophobic islands
out [2], by increasing the surface area with fins or fluidized or superhydrophobic islands. We varied the size of the
bed [2-5], and by enhancing the wettability of the surface superhydrophobic patterns based on the range of active
[4-8]. The latter objective is justified by experiments of nucleation site sizes calculated by the theory in [14].
Wang and Dhir [9], showing that the critical heat flux was The manufacturing process is shown in figure 1. The
increased by enhancing surface wettability. Wettability can test surfaces were made on a double-sided polished and
be enhanced by either increasing the surface roughness or oxidized 500 µm thick silicon wafer. On the back side we
with microstructure or nanostructure coatings. For instance, deposited thin film resistive heaters. The heaters were made
Jones et al. [10] have shown that a well-chosen roughness from sputtered Indium Tin Oxide (ITO) approximately 300
can double or triple the heat transfer coefficient. Significant nm thick. The target resistance for the ITO heaters was 50 Ω
heat transfer enhancement has also been obtained with per square. Copper electrodes were thermally evaporated
surfaces coated with a µm-thick carpet of nanometer over the ITO, leaving 1 cm2 of ITO exposed. The copper
diameter wires (nanowires) [4-6]. The CHF enhancement electrodes were 1 µm thick to minimize their resistance and
was attributed to coupled effects such as the multi-scale therefore the power loss in the system. A 100 nm layer of
geometry [4, 6] and the superhydrophilicity of the nanowire SiO2 was deposited to electrically passivate the heater. On
arrays [5, 6]. the top surface of the wafer, the silicon dioxide was first
In previous work [11] we took advantage of removed from the top side only using CF4 gas in a reactive-
microlithography techniques to design surfaces combining ion etching (RIE) machine. Next, a random array of silicon
hydrophobic and hydrophilic zones for pool boiling nanostructures (figure 2a) was formed using the black

978-1-4244-9633-4/11/$26.00 ©2011 IEEE 1193 MEMS 2011, Cancun, MEXICO, January 23-27, 2011
in a deep reactive-ion etching (DRIE) machine. The height
of the nanostructures was usually less than 1 µm. It should
also be noted that nanostructured surfaces similar to the
ones we use here have been shown to enhance pool boiling
heat transfer in [4, 15]. Then, to ensure the hydrophilic
wettability of the surface, the silicon structures were
oxidized by exposure to oxygen plasma in the RIE machine
for 30 minutes, resulting in a silicon dioxide layer
approximately 30 nm thick. A layer of Teflon®
fluoropolymer or Cytop® was then spin-coated at 2500 rpm
for 30 seconds and annealed at 250 °C or 125 °C,
respectively. The thickness of the polymer coating was less
than 100 nm. Zonyl FSN surfactant was added to AZ5214
photoresist to improve its wettability on the hydrophobic
surface and was subsequently spin-coated at 3000 rpm for
30 seconds. The photoresist was patterned by
photolithography into regular arrays of 50 µm diameter
hexagons, circles ranging from 25 µm to 100 µm in
diameter, or fractal arrays of circles ranging from 10 to 540
µm in diameter, shown in figures 2b and c.With the
photoresist as a mask, the hydrophobic layer was etched by
oxygen plasma for 3 minutes, thus defining hydrophobic
Figure 1. Process flow for the fabrication of the resistive islands amidst the hydrophilic network of oxide-covered
heater (backside) and the combination of superhydrophilic black silicon microstructures, shown in figure 2d. Finally,
and superhydrophobic patterns (front side). Not drawn to the photoresist etching mask was removed in acetone and
scale. the wafer was cleaved into chips.
SETUP
During the heat transfer experiments the chip was
placed in a polycarbonate chamber open to the atmosphere,
filled with degassed and deionized water as shown in figure
3. For more details see [11]. The resistive heater and
electrodes were encased in a 5-10 mm thick layer of PDMS
for electrical and thermal insulation. The water was
maintained at the saturation temperature of 100 °C with
submerged cartridge heaters. A data acquisition system
(OMEGA DAQ-55) was used to record the temperature
measured on the back of the wafer, Tmeas. From that
temperature, the temperature at the wafer-water interface
Tw= Tmeas-q”t/k was determined using Fourier’s law, where
q”, t and k are the respective heat flux, wafer thickness and
silicon thermal conductivity. For each data point the
temperature is obtained by averaging three hundred readings
over about three minutes. A 750 W power supply (Agilent
N5750A) was used to apply a given heat flux to the heater.
The CHF is determined as the heat flux corresponding to the
last observed stable temperature, beyond which a sudden
dramatic increase in temperature is observed.
The maximum combined uncertainty on the heat flux
was estimated as ±1.5 W/cm2, caused by the measurement
Figure 2. (a) SEM image of nanostructured black silicon of the heater area and the measurement of the electrical
surface, (b, c) chrome masks of the fractal and regular power. The maximum uncertainty on the superheat was
arrays of circles, and (d) the completed surface (fractal) estimated as ±1.5 K, due to the thermocouple uncertainty,
submerged in water; bubbles promptly form over the temperature acquisition and heater/wafer thickness
superhydrophobic spots making them visible to the naked measurement uncertainties. For superheat values less than 1
eye. The light green is (super)hydrophobic and the darker K the uncertainty on the HTC can be greater than 100 %.
green is superhydrophilic. This error decreases as the superheat increases and is less
than 20 % of the HTC at superheats above 5 K.

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Power Supply Thin film K-type
Submerged thermocouple
+- cartridge heaters
a
Silicon

Silicon dioxide

Indium tin oxide

Copper

Teflon®

PDMS

Polycarbonate chamber
Figure 3. Pool boiling setup for heat transfer experiments.

RESULTS AND ANALYSIS


Figure 4 shows the results of our manufacturing
process. The structured silicon oxide surface shown in
figure 2a and 4a was perfectly wetting, in the sense that a
drop several millimeters in diameter placed on the surface b
spread over the entire chip with an area around 10 cm2.
Figure 4b shows the wetting of a drop on the structured
surface coated with Cytop® an amorphous fluoropolymer.
Figure 4c shows the wetting of a drop on the structured
surface coated with Teflon®. Indeed we have achieved both
superhydrophilic regions and superhydrophobic regions
with a wetting angle above 150º.
a b c

Figure 4. spreading of water drops on the three different


surfaces: (a) spreading on the superhydrophilic surface, the
drop will continue to spread outside the field of view,
indicating a wetting angle close to 0º (b) hydrophobic
surface made with Cytop® has a wetting angle of 120º and
(c) a superhydrophobic surface made from Teflon® shows
wetting angles over 150º.
The results from our heat transfer measurements are
shown in figure 5. In this work we tested three types of Figure 5. (a) The Heat Transfer Coefficient (HTC) versus
surfaces that we refer to in figure 5 using the wetting angle heat flux for the current work is higher than the best HTC
values for the base surface and islands, in parentheses: values to date for flat nanoengineered surfaces [4, 11, 15].
superhydrophilic surfaces with hydrophobic islands Note, however, at low heat flux < 30W/cm2, that
(0º/120º), a superhydrophilic surface made from nano- thermocouple reading error induces a large variance of the
structured oxidized silicon (0º), and superhydrophilic HTC. As the heat flux and superheat increase, the error
surfaces with superhydrophobic islands (0º/150º). We also becomes negligible. (b) Boiling curves for this work
compared the boiling performance of these surfaces to our compared to the previous work of [4, 11, 15].
previous work using micropatterned hydrophilic and
hydrophobic networks [11] and to state-of-the-art shows that the superhydrophilic wafer with hydrophobic
nanostructured surfaces [4, 15] for pool boiling. islands (0º/120º) can increase CHF by 80 % compared to a
The results for the HTC are plotted in figure 5a. We hydrophilic SiO2 (7º) surface. The (0º/150º) and (0º)
find that superhydrophilic surface with superhydrophobic surfaces did not show any significant change in CHF. There
islands (0º/150º) can quadruple the HTC, while the (0º/120º) was no significant difference in the performance between
and the (0º) surfaces both have a moderate increase in HTC the regular and fractal arrays.
compared to a hydrophilic SiO2 (7º) surface. Figure 5b

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superhydrophobic islands (0º/150º) show a HTC 100% [4] Li, C., Z. Wang, P.I. Wang, Y. Peles, N. Koratkar, and
higher than the best state-of-the-art nanoengineered surfaces G.P. Peterson, "Nanostructured copper interfaces for
[4, 11, 15]. enhanced boiling", Small, vol.4, pp. 1084-1088, 2008.
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nucleation. For comparison the hydrophilic SiO2 (7º) Cho, and A. Majumdar, "Nanowires for enhanced
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boiling is a transient, multiphase phenomenon; visualization saturated water", Journal of Heat Transfer-
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complex. We conjecture that the enhancement in HTC is [9] Wang, C.H. and V.K. Dhir, "Effect of surface
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