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2011 PRL Lee Underwater RestRetGas SHPo Drag Reduction

2011 PRL Lee Underwater RestRetGas SHPo Drag Reduction

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Underwater Restoration and Retention of Gases on SuperhydrophobicSurfaces for Drag Reduction
Choongyeop Lee and Chang-Jin Kim
 Mechanical and Aerospace Engineering Department, University of California Los Angeles (UCLA), Los Angeles, California 90095, USA
(Received 25 August 2010; published 7 January 2011)Superhydrophobic (SHPo) surfaces have shown promise for passive drag reduction because theirsurface structures can hold a lubricating gas film between the solid surface and the liquid in contact with it.However, the types of SHPo surfaces that would produce any meaningful amount of reduction get wetunder liquid pressure or at surface defects, both of which are unavoidable in the real world. In this Letter,we solve the above problem by (1) discovering surface structures that allow the restoration of a gas blanketfrom a wetted state while fully immersed underwater and (2) devising a self-controlled gas-generationmechanism that maintains the SHPo condition under high liquid pressures (tested up to 7 atm) as well as inthe presence of surface defects, thus removing a fundamental barrier against the implementation of SHPosurfaces for drag reduction.
DOI:10.1103/PhysRevLett.106.014502PACS numbers: 47.85.lb, 68.08.Bc, 81.40.Pq, 83.50.Rp
Recently, structured hydrophobic surfaces exhibitingsuperhydrophobicity have shown promise as gas-lubricated surfaces because their surface structures canhold a gas film when submerged in a liquid [18] [Fig.1(a)]. Some have even demonstrated effective sliplengths [9] up to hundreds of micrometers [6,7], which are large enough to benefit regular (i.e., large) fluidic systems.Drag reduction for turbulent flows has also been reported[8]. Superhydrophobic (SHPo) surfaces are considered asuperior alternative to the existing bubble injection method[10] for drag reduction because the stable gas upon thesurfaces makes the SHPo method passive (i.e., energyefficient) and simple (i.e., easy to implement). Moreover,it has been shown that the minimized solid-liquid contacton SHPo surfaces can resist surface fouling [11]. Despiteits great potential, drag reduction by SHPo surfaces hasbeen considered strictly limited to laboratory conditionsbecause of one main unanswered question: Can they retainthe gas under real conditions? This problem is ratherfundamental and should be addressed first, so that morepractical issues like biofouling and cost are even relevant.Because the wetting transition of a SHPo surface is spon-taneous, any liquid impregnation, incited by variousinstigators [12,13], has an irrevocable effect against drag reduction, as illustrated in Figs.1(a)and1(c). For example, the surface may get wet and lose its slip effect if it hasdefects, the liquid is under pressure [12], or thegas diffusesaway over time [13].Recently, several approaches have been suggestedto increase the stability of the gas layer on a SHPosurface against liquid pressure [7,14,15]: e.g., nanostruc- turing the sidewall of the microstructures [7] and pressur-izing the gas layer [14,15]. However, these approaches are only preventive measures. They are ineffective once thegas layer is disrupted. The ability to restore underwatersuperhydrophobicity even after the surface structures be-come wetted is more desirable. A successful schemeshould be able to displace the liquid that has impregnatedthe surface structures with new gas and reform a stable gasfilm, as illustrated in Fig.1(d). Note the recovery of theSHPo state shown for sessile droplets surrounded by air[16,17] is not helpful for drag reduction, which pertains to the entire surface being fully immersed underwater.To restore a stable gas layer, we reason that the new gasshould not grow vertically off the surface structures beforespreading laterally between them. We propose that thisgoal can be achieved by designing the surface structuresto satisfy a certain geometric criterion, given belowfor post structures (see supplementary material fordetails [18], which addresses the case of grate structuresas well):
FIG. 1 (color online). Loss of slip by wetting transition and ahypothetical scenario to restore underwater superhydrophobicity.
PRL
106,
014502 (2011)PHYSICAL REVIEW LETTERS
week ending7 JANUARY 2011
0031-9007
=
11
=
106(1)
=
014502(4) 014502-1
Ó
2011 The American Physical Society
 
ffiffiffi 
2
À
2
 ffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi 
ð
1
À
Þ
= 
À
1
þ
sin
p;
adv
2cos
p;
adv
<H=L<
À
cos
b;
rec
2sin
p;
rec
½
1
À
 ffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffiffi 
 
ð
1
À
Þ
=
Š
 ;
(1)where
,
,
L
,
are the gas fraction (
¼
1
À
D
2
=
4
L
2
,
D
is the diameter of posts), height and pitch (center-to-center distance) of the posts, and contact angle (CA),respectively. For the CA
, the subscripts ‘adv’and‘recmean advancing and receding, and subscripts
p
and
b
refer to the surface of the posts and the bottomsurface between the posts, respectively. The upper boundvalue of 
H=L
shown in Eq. (1) was derived from a geo-metric requirement that the gas should grow with lessresistance in the lateral direction than in the vertical direc-tion. The maximum gas pressure the interfaces can sus-tain against vertical (i.e., undesirable) growth is
Á
P
v
¼ð
D
sin
p;
rec
Þ
=L
2
, while the minimum pressure neededto sustain the lateral growth (i.e., the two vertical contactlines on the sidewall of a post merge and depart from thewall) is
Á
P
l
¼ð
L
cos
b;
rec
þ
2
sin
p;
rec
Þ
=HL
. The firstand second term represent the resistance by the bottomsurface and that by the post sidewall, respectively. For thebubble to grow laterally without vertical outgrowth, thegaspressure should be higher than
Á
P
l
but lower than
Á
P
v
,providing a qualitative guideline for the design of SHPosurfaces that allow the restoration of a stable gas layer. Thelower bound value of 
H=L
in Eq. (1) was derived fromanother geometric requirement that, once the gas film isformed, the liquid-gas meniscus should not touch the bot-tom surface as a result of the liquid pressure, on thecondition that the height of the posts should be greaterthan the maximum sagging depth of the meniscus [2].When
CA
rec
on the bottom surface is 110
, correspond-ing to a smooth surface of a highly hydrophobic material(e.g., Teflon
Ò
), there is only a limited regime that satisfiesthe right-hand side of Eq. (1) [Fig.2(a)]. In order to increase this
CA
b;
rec
further, expanding the regime of satisfactory values,wepropose tonanostructurethebottomsurface and render it a solid-gas composite. According tothe Cassie-Baxter equation [19],
cos
c
¼
þð
1
À
Þ
cos
;
(2)where
isthe intrinsicCA ona smoothsurfaceand
c
istheapparent CA on the nanostructured surface.
¼
110
,
c
can be increased to 173.4
by employing nanostructureswith a gas fraction of 0.99. Accordingly, the geometricregime of posts that satisfy Eq. (1) is significantly expandedif the bottom surface is nanostructured [Fig.2(a)]. Thisapproach is schematically represented in Fig.2(b). Whenthe microstructures become wetted, a residual gas remainsin between the nanostructures due to their high resistanceagainst liquid impalement, keeping the bottom surfaceSHPo. When there is an influx of gas, the large contactangle on the SHPo bottom surface helps the gas spread pastthe posts laterally and recover the gas layer among themicrostructures.Based on the aforementioned geometrical requirementsfor successful gas spreading, hydrophobic microstructureswere constructed on a substrate surface covered in hydro-phobic nanostructures, as shown in Fig.2(c). To fabricatesuch hierarchical SHPo surfaces, nanostructures wereformed on a 4 in. silicon wafer using a black siliconmethod, on which a gas fraction over 99% and contactangle over 175
were reported previously [2]. After depos-iting and patterning Au (
$
200 nm
) as electrodes for
FIG. 2 (color). Proposed scheme to restore gas film under-water, shown for micropost. (a) Estimated range of height-to-pitch ratio (
H=L
) that allows formation of a gas film betweenposts as function of their gas fraction with
CA
b;
rec
as a parameter.Red line represents the minimum
H=L
and black line themaximum
H=L
acceptable, following Eq. (1). Microposts of varying gas fraction and pitch (while height is fixed at
50
m
),denoted with
d
, have been fabricated on both smooth andnanostructured bottom surfaces and tested. The gas film resto-ration was achieved only when the acceptable zone was ex-panded due to the increased
CA
rec
on the nanostructured bottomsurface, qualitatively agreeing with the theory. (b) Schematicrepresentation of the successful gas film formation. (c) Scanningelectron microscopy images of a test surface fabricated based onthe above criteria.
PRL
106,
014502 (2011)PHYSICAL REVIEW LETTERS
week ending7 JANUARY 2011
014502-2
 
electrolysis on the bottom surface,
50
m
-thick negativephotoresist (KMPR1050, Microchem) was spin coated onthe wafer, and microstructures (posts or grates) with vary-ing pitches and gas fractions were patterned out of thephotoresist. Finally, to make all the surfaces hydrophobic,2 wt% Teflon
Ò
AF solution (Dupont) was spin coated.To replenish the gas layer lost upon wetting, electrolysiswas deemed better suited than other gas-generation meth-ods such as thermal, pneumatic, and chemical on accountof its low power consumption [20], the stability of thegenerated gases [21], its easy integration into a system,and its compatibility with water. In this study, we used aline pattern of thin-film gold on the bottom surface as thecathode [Fig.2(c)] and a copper wire in the water as theanode to perform electrolysis. The placement of the elec-trodes on the bottom surface imposes a self-controlled (i.e.,self-activating and self-limiting) generation of gas becausethe electrolytic circuit closes, starting gas generation, onlywhen and where the microstructures become wetted (i.e.,the liquid touches the cathode), and opens, halting the gasgeneration, as soon as the dewetting is complete.A series of experiments were conducted to verify theeffectiveness of the proposed scheme by restoring under-water superhydrophobicity under the worst-case scenarioof all the microstructures being wet. Before applying anyvoltage, the water tank was first subjected to a moderatevacuum (1–2 kPa), which made all the microstructures wetbut not the nanostructures. After the wetting was con-firmed,weapplied10Vbetweenthecathodeonthesampleand the anodewire 1 cm above the sample inside thewater,starting electrolysis. As a reference, we prepared a controlsurface having microposts on a smooth bottom surface[Fig.3(a)]. In this case, the generated gas tended to pro-duce several individual bubbles, which protruded over thetop of the posts rather than forming a film, failing to coverthe surface evenly (see video S1 in [18]). For the proposedsurface having microposts on a nanostructured bottom[Figs.3(b)and3(c)], in comparison, a nonwetted area was gradually recovered as the gas film spread withoutprotruding over the microposts. The entire test area(
2 cm
Â
2 cm
) became dewetted after several minutes(see videos S2 and S3 in [18]). A schematic illustrationof bubble generation on the wetted surface of microposts isshown in Fig. S6 in [18] along with the test setup.A dewetting process begins with patches of gas filmappearing at random locations in a wetted area. Afterthat, the growth of gas occurs mainly via Oswald ripening[22], since the gas is interconnected everywhere viathe thin residual layer on the bottom surface between thenanostructures. In Oswald ripening, the gas inside thesmaller bubbles is transported to the larger bubbles (i.e.,a gas film) due to the difference in Laplace pressures,leading to the continuous growth of a large gas film untilthe gas film covers the whole area. The current approachwas also applied to regenerate a gas layer on a surface of grating microstructures as well, as shown in Fig.3(d)andvideo S4 in [18].The total power consumption needed for complete res-torationof thegas film onthe testarea of 
2 cm
Â
2 cm
wasestimated to be about 6 mW for 150 sec. This value, whilemuch larger than the inherent power requirement due tothe Teflon
Ò
layer covering the electrodes and the accom-panying components in the test setup, is nonethelessmuch smaller than that needed for a thermal method(e.g., 1–100 W [20]). It is worth noting that the presenceof nanostructures on the bottom surface offers anotheradvantage for practical applications. When a liquid im-pregnates microstructures on a smooth bottom surface, thewetting tends to spread rapidly to the surrounding area,leading to a cascade of wetting over the entire area [6]. Incontrast,withthebottomsurfacenanostructuredand super-hydrophobic in its own right against liquid pressure, oursurfaces confine the wetting to limited regions and resistfurther liquid spreading. This feature helps restore a gaslayer on microstructures with surface defects [23].Another important implication of our surface for prac-tical applications is that our surface can retain a stable gaslayer even under high liquid pressure. An electrolyticallygenerated gas automatically adjusts its pressure to that of the liquid, such that a gas layer on our surface can effec-tively resist high liquid pressure. We experimentally veri-fied that a gas layer can be retained on our surface underpressurized liquid (tested up to 7 atm) by employing thecurrent gas restoration scheme. This feature can signifi-cantly expand the applicability of a SHPo surface to a
FIG. 3 (color online). Demonstration of restoration of under-water superhydrophobicity. (a) Gas generation on microposts(
100
m
pitch,
50
m
height, 95% gas fraction) with thesmooth bottom surface. (b),(c) Gas generation on microposts[
100
m
pitch for (b) and
50
m
pitch for (c), both
50
m
height and 95% gas fraction] with the nanostructured bottomsurface. (d) Gas generation on microgrates (
50
m
pitch,
50
m
height, 80% gas fraction) with the nanostructured bottomsurface.
PRL
106,
014502 (2011)PHYSICAL REVIEW LETTERS
week ending7 JANUARY 2011
014502-3

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