9 International Conference on Nanochannels, Microchannels and Minichannels th nd June 19 22 , Edmonton, Canada

th

DRAFT ICNMM2011-58141
NANO-ENGINEERED SURFACES WITH HETEROGENEOUS WETTABILITY FOR BOILING HEAT TRANSFER ENHANCEMENT
Amy Rachel Betz Columbia University Department of Mechanical Engineering New York, NY, USA James Jenkins University of California, Los Angeles Department of Mechanical Engineering Los Angeles, CA, USA

Chang-Jin CJ Kim University of California, Los Angeles Department of Mechanical Engineering Los Angeles, CA, USA

Daniel Attinger Columbia University Department of Mechanical Engineering New York, NY, USA

ABSTRACT In this work we describe the manufacturing and characterization of multi-scale patterned heterogeneous wettability surfaces. We find drastic enhancements of the pool boiling performance of water. In comparison to a hydrophilic SiO2 surface with a wetting angle of 7, we find that surfaces combining superhydrophilic and superhydrophobic patterns can increase the heat transfer coefficient (HTC) by 300% and can increase the critical heat flux (CHF) by more than 100%. 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 m-thick carpet of nanometer diameter wires (nanowires) [4-6]. The CHF enhancement was attributed to coupled effects such as the multi-scale geometry [4, 11, 12] and the superhydrophilicity of the nanowire arrays [5, 6]. Another method for increasing HTC was first proposed in the work of Hummel in 1965 [13]. Hummel manufactured surfaces of heterogeneous wettability by patterning non-wetting epoxy resins on wetting metallic surfaces. The non-wetting patterns act as nucleation sites. In the work of [14, 15] it is shown that bubbles nucleate on hydrophobic islands at significantly lower heat fluxes and superheat values compared to hydrophilic surfaces. The number of nucleation sites is directly proportional to the HTC [16]. The wetting area around the patterns prevents the expanding bubbles from blanketing the surface [13]. The work of Hummel was characterized by plotting the wall superheat (Tw Tf) versus the HTC and comparing his heterogeneous surfaces to the homogeneous wetting surface. The increase in HTC was most significant at low superheat. For example, at 1K superheat there is a 500% increase in HTC from 2 -12 kW/m2K, where as at 5.6 K superheat there is a 200% increase from 5.1 to 15.9 kW/m2K. In the work of [14] they show a 250% increase in HTC at a superheat of 16 K compared to the wetting surface. The heterogeneous surfaces did not increase CHF compared to the wetting surface in either work.

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In our previous work [17] we showed, for the first time, that a hydrophilic network with hydrophobic islands can increase both the HTC and CHF. Compared to a hydrophilic wafer with a wetting angle of 7 we find a 65% increase in CHF, a 100% increase in the maximum HTC and 600% increase in HTC at a superheat of 9.5 K from 8.8 kW/m2K to 54 kW/m2K. .In that work we inferred that increasing the wettability contrast increased the CHF. In this work we further explore the effects of wettability contrast with nano-fabrication to create superhydrophilic networks with superhydrophobic islands for pool boiling experiments. Our intuition is that the superhydrophilic surfaces will increase rewetting [18] and the superhydrophobic islands will promote nucleation [16]. We characterize the pool boiling performance of these surfaces and compare it to state-of-the-art enhanced surfaces. DESIGN AND MANUFACTURING OF THE HETEROGENEOUS WETTABILITY SURFACES We designed our surfaces with heterogeneous wettability based on our findings in [17] In that work we explored 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 increase the HTC at low values of superheat. Therefore in this work we only manufactured surfaces with superhydrophilic networks of heterogeneous wettability. We varied the size of the superhydrophobic patterns based on the range of active nucleation site sizes calculated by the theory in [19]. It should also be noted that nanostructured surfaces similar to the ones we use to create the superhydrophilic and superhydrophobic surfaces have been shown to enhance heat transfer in [4, 11].

Figure 1. SEM images of the different patterns investigated in this work show fractal (a), hexagonal (b) and circular patterns (c). The lighter areas are superhydrophilic nanostructures and the darker areas are the superhydrophobic patterns. The softness of the images is due to the nanostructured base surface (d). The manufacturing process is shown in figure 2. The test surfaces were made on a double-sided polished and oxidized 500 m 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 cm2 of ITO exposed. The copper electrodes were 1 m 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 silicon method [20] in a deep reactive-ion etching (DRIE) machine. The height of the nanostructures was usually less than 1 m. 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 was then spincoated at 2500 rpm for 30 seconds and annealed at 250 C . 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

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patterned by photolithography into regular arrays of 50 m diameter hexagons, circles ranging from 25 m to 100 m in diameter, or fractal arrays of circles ranging from 10 to 540 m in diameter. With the photoresist as a mask, the hydrophobic layer was etched by oxygen plasma for 3 minutes, thus defining hydrophobic islands amidst the hydrophilic network of oxidecovered black silicon microstructures. Finally, the photoresist etching mask was removed in acetone and the wafer was cleaved into chips.

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 of 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.
Thin film K-type Power Supply Submerged thermocouple +cartridge heaters
Silicon Silicon dioxide Indium tin oxide Copper Teflon PDMS

Polycarbonate chamber

Figure 3. Pool boiling setup for heat transfer experiments. Figure 2. Process flow for the fabrication of the resistive heater (backside) and the combination of superhydrophilic and superhydrophobic patterns (front side). Not drawn to scale. POOL BOILING SET UP 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 [17]. 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-qt/k was determined using Fouriers 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

RESULTS The boiling curves are shown in figure 4. We tested our surfaces with heterogeneous wettability (0/150) as well as several nanostructured superhydrophilic surfaces (0) and compared them to a hydrophilic SiO2 wafer with a wetting angle of 7. Both the superhydrophilic and the heterogeneous wettability surfaces show an increase in HTC and CHF. The heterogeneous wettability surfaces show the greatest enhancement. These surfaces demonstrated a 300% increase in HTC and more than a 100% increase in CHF compared to the SiO2 wafer. We also compared the boiling performance of these surfaces to state-of-the-art nanostructured surfaces [4, 11] in figure 5. We found that our surfaces reach HTC more than 50% and slightly higher CHF than other state-of-the-art surfaces.. All the surfaces tested in this work showed an increase in bubble nucleation. For comparison the hydrophilic SiO2 (7) surface, tested in [17], required a superheat over 13 K before

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significant nucleation occurred and the surface was not saturated with bubbles until the heat flux was close to CHF. The (0) surfaces showed significant increase in nucleation once the superheat exceeded 10 K and the surfaces with superhydrophobic islands (0/150) promoted nucleation even at low superheat and heat flux. For this surface (0/150) the entire heated area was saturated with bubbles at heat flux q = 25 W/cm2 and superheat T = 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 believe the enhancement in HTC is due to an increase in nucleation sites from the superhydrophobic islands as well as from cavities in the nanostructured surfaces. It 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 and visualization is needed to confirm the mechanisms enhancing heat transfer.

Figure 5. Comparison of this work to other state-of-the-art nanoengineered surfaces.

CONCLUSIONS In summary we have micro and nanoengineered patterned flat surfaces with high contrast in wettability. These surfaces typically enhance pool boiling performance. Superhydrophilic surfaces with superhydrophobic islands increase the heat transfer coefficient by 300% compared to a hydrophilic surface and increase the critical heat flux by more than 100%. In future work we hope to identify the physical mechanisms that increase the pool boiling performance.

REFERENCES

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