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

8/6/2019 2011 MEMS Betz Boiling SHPiSHPo Pattern

http://slidepdf.com/reader/full/2011-mems-betz-boiling-shpishpo-pattern 1/4

SIGNIFICANT BOILING ENHANCEMENT WITH SURFACES COMBINING

SUPERHYDROPHILIC AND SUPERHYDROPHOBIC PATTERNS

Amy Rachel Betz 1 , James R. Jenkins2 , Chang-Jin “CJ” Kim2 and Daniel Attinger 1 1Columbia University, New York, NY, USA

2University of California, Los Angles (UCLA), CA, USA

ABSTRACT

In this work we describe the manufacturing and

characterization of patterned surfaces with large spatial

contrast in wettability. We find drastic enhancement of pool

boiling performance in water. In comparison to a

hydrophilic SiO2 surface with a wetting angle of 7º, surfaces

combining superhydrophilic and superhydrophobic patterns

can quadruple the heat transfer coefficient (HTC).

Superhydrophilic surface with hydrophobic islands can

increase the critical heat flux (CHF) by 80%. This

performance enhancement is important for applications such

as electronics cooling, because the increased HTC allows a

greater amount of heat to be removed at a lower wall

superheat.

INTRODUCTION

Boiling is an efficient process to transfer large amounts

of heat at a prescribed temperature because of the large

latent heat of vaporization. The term flow boiling describes

the boiling of liquids forced to move along hot surfaces,

while in pool boiling, the topic handled in this paper, the

liquid is stagnant and in contact with a hot solid surface [1].

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

temperature until a transition from high HTC to very low

HTC occurs, which signifies the formation of a vapor filminsulating the liquid from the heated surface, a phenomenon

called dry out.

As of today, the performance of boiling surfaces has

been increased by using wicking structures to prevent dry

out [2], by increasing the surface area with fins or fluidized

bed [2-5], and by enhancing the wettability of the surface

[4-8]. The latter objective is justified by experiments of

Wang and Dhir [9], showing that the critical heat flux was

increased by enhancing surface wettability. Wettability can

be enhanced by either increasing the surface roughness or

with microstructure or nanostructure coatings. For instance,

Jones et al. [10] have shown that a well-chosen roughness

can double or triple the heat transfer coefficient. Significant

heat transfer enhancement has also been obtained withsurfaces coated with a µm-thick carpet of nanometer

diameter wires (nanowires) [4-6]. The CHF enhancement

was attributed to coupled effects such as the multi-scale

geometry [4, 6] and the superhydrophilicity of the nanowire

arrays [5, 6].

In previous work [11] we took advantage of

microlithography techniques to design surfaces combining

hydrophobic and hydrophilic zones for pool boiling

experiments. We showed that a hydrophilic network with

hydrophobic islands can increase CHF by 65% and HTC by

100% compared to a hydrophilic wafer with a wetting angle

of 7º. We also found that increasing the wettability contrast

increased the CHF. In [11] we varied the size of the patterns

as well as the connectivity of the hydrophobic and

hydrophilic patterns. Hydrophilic surfaces with hydrophobic

islands were called hydrophilic networks meaning that any

two hydrophilic regions could be joined without passing

over a hydrophobic zone. Hydrophobic surfaces with

hydrophilic islands were called hydrophobic networks. We

found that hydrophilic networks increased both the HTC

and CHF while hydrophobic networks only increased the

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-

fabrication to create superhydrophilic networks with

superhydrophobic islands. Our intuition is that the

superhydrophilic surfaces might improve rewetting [12] and

the superhydrophobic islands might improve nucleation

[13]. We characterize the pool boiling performance of these

surfaces and compare it to state-of-the-art enhanced

surfaces.

DESIGN AND MANUFACTURING

We designed our superhydrophilic surfaces with

superhydrophobic patterns on the basis of our recent work

[11] where micromanufactured surfaces with spatial

contrasts of wettability exhibited increased pool boiling

performance. All the surfaces investigated in the present

work are superhydrophilic with either hydrophobic islands

or superhydrophobic islands. We varied the size of the

superhydrophobic patterns based on the range of active

nucleation site sizes calculated by the theory in [14].

The manufacturing process is shown in figure 1. The

test surfaces were made on a double-sided polished and

oxidized 500 µm thick silicon wafer. On the back side we

deposited thin film resistive heaters. The heaters were made

from sputtered Indium Tin Oxide (ITO) approximately 300

nm thick. The target resistance for the ITO heaters was 50 Ω

per square. Copper electrodes were thermally evaporatedover the ITO, leaving 1 cm2 of ITO exposed. The copper

electrodes were 1 µm thick to minimize their resistance and

therefore the power loss in the system. A 100 nm layer of

SiO2 was deposited to electrically passivate the heater. On

the top surface of the wafer, the silicon dioxide was first

removed from the top side only using CF4 gas in a reactive-

ion etching (RIE) machine. Next, a random array of silicon

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

8/6/2019 2011 MEMS Betz Boiling SHPiSHPo Pattern

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Figure 1. Process flow for the fabrication of the resistive

heater (backside) and the combination of superhydrophilicand superhydrophobic patterns (front side). Not drawn to

scale.

Figure 2. (a) SEM image of nanostructured black silicon

surface, (b, c) chrome masks of the fractal and regular arrays of circles, and (d) the completed surface (fractal)

submerged in water; bubbles promptly form over the

superhydrophobic spots making them visible to the naked

eye. The light green is (super)hydrophobic and the darker

green is superhydrophilic.

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 hydrophobicislands amidst the hydrophilic network of oxide-covered

black silicon microstructures, shown in figure 2d. Finally,

the photoresist etching mask was removed in acetone and

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 measurementof the heater area and the measurement of the electrical

power. The maximum uncertainty on the superheat was

estimated as ±1.5 K, due to the thermocouple uncertainty,

temperature acquisition and heater/wafer thickness

measurement uncertainties. For superheat values less than 1

K the uncertainty on the HTC can be greater than 100 %.

This error decreases as the superheat increases and is less

than 20 % of the HTC at superheats above 5 K.

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Polycarbonate chamber

Thin film K-type

thermocouplePower Supply

Submerged

cartridge heaters+ -

Silicon

Silicon dioxide

Indium tin oxide

Copper

Teflon®

PDMS

Silicon

Silicon dioxide

Indium tin oxide

Copper

Teflon®

PDMS

Polycarbonate chamber

Thin film K-type

thermocouplePower Supply

Submerged

cartridge heaters+ -

Silicon

Silicon dioxide

Indium tin oxide

Copper

Teflon®

PDMS

Silicon

Silicon dioxide

Indium tin oxide

Copper

Teflon®

PDMS

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

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 ca 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

surfaces that we refer to in figure 5 using the wetting angle

values for the base surface and islands, in parentheses:

superhydrophilic surfaces with hydrophobic islands

(0º/120º), a superhydrophilic surface made from nano-

structured oxidized silicon (0º), and superhydrophilic

surfaces with superhydrophobic islands (0º/150º). We also

compared the boiling performance of these surfaces to our

previous work using micropatterned hydrophilic and

hydrophobic networks [11] and to state-of-the-art

nanostructured surfaces [4, 15] for pool boiling.

The results for the HTC are plotted in figure 5a. We

find that superhydrophilic surface with superhydrophobic

islands (0º/150º) can quadruple the HTC, while the (0º/120º)

and the (0º) surfaces both have a moderate increase in HTC

compared to a hydrophilic SiO2 (7º) surface. Figure 5b

a

b

a

b

Figure 5. (a) The Heat Transfer Coefficient (HTC) versus

heat flux for the current work is higher than the best HTC values to date for flat nanoengineered surfaces [4, 11, 15].

Note, however, at low heat flux < 30W/cm2, that

thermocouple reading error induces a large variance of the HTC. As the heat flux and superheat increase, the error

becomes negligible. (b) Boiling curves for this work

compared to the previous work of [4, 11, 15].

shows that the superhydrophilic wafer with hydrophobic

islands (0º/120º) can increase CHF by 80 % compared to a

hydrophilic SiO2 (7º) surface. The (0º/150º) and (0º)

surfaces did not show any significant change in CHF. There

was no significant difference in the performance between

the regular and fractal arrays.

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We would also like to note that that the surfaces with

superhydrophobic islands (0º/150º) show a HTC 100%

higher than the best state-of-the-art nanoengineered surfaces

[4, 11, 15].

All the surfaces tested in this work facilitated bubble

nucleation. For comparison the hydrophilic SiO2 (7º)

surface, tested in [11], required a superheat over 15 K

before significant nucleation occurred and the surface was

not saturated with bubbles until the heat flux was close toCHF. The (0º) and (0º/120º) surfaces showed significant

nucleation with a superheat of 10 K and the surfaces with

superhydrophobic islands (0º/150º) promoted nucleation at

an even lower superheat and heat flux. For this surface

(0º/150º) the entire heated area was saturated with bubbles

at heat flux q” = 25 W/cm2 and superheat ΔT = 3 K, which

is consistent with the idea that an increase in hydrophobicity

increases the number of nucleation sites.

Explaining the observed trends is complex because pool

boiling is a transient, multiphase phenomenon; visualization

is difficult especially for the violent boiling near CHF, and

the geometry and wettability of these enhanced surfaces is

complex. We conjecture that the enhancement in HTC isdue to an increase in the number of nucleation sites from the

superhydrophobic and hydrophobic islands as well as from

cavities in the nanostructured surfaces. The HTC

enhancement could also be attributed to the increased

surface area from the nanostructures. The increase in critical

heat flux may be due to increased surface wettability or

wettability contrast, moderation of instabilities, or from

wicking in the nanostructures. More analysis with simpler

experiments and multiscale modeling are probably needed

to identify the mechanisms enhancing heat transfer.

CONCLUSIONS

In summary we have combined micro- andnanoengineering techniques to manufacture flat surfaces

with large spatial contrast in wettability. In comparison with

a very hydrophilic surface, these surfaces typically enhance

pool boiling performance. Superhydrophilic surfaces with

superhydrophobic islands quadruple the heat transfer

coefficient compared to a very hydrophilic surface, without

significantly improving the critical heat flux. We have also

shown that superhydrophilic surfaces with hydrophobic

islands can double the heat transfer coefficient and increase

the critical heat flux by 80 %, compared to a very

hydrophilic surface.

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