Environmental Applications of Interfacial Materials with Special Wettability.

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Critical Review

Environmental Applications of Interfacial Materials with Special Wettability Zhangxin Wang, Menachem Elimelech, and Shihong Lin Environ. Sci. Technol., Just Accepted Manuscript • DOI: 10.1021/acs.est.5b04351 • Publication Date (Web): 01 Feb 2016 Downloaded from http://pubs.acs.org on February 4, 2016

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Environmental Science & Technology

Environmental Applications of Interfacial Materials with Special Wettability Critical Review Environmental Science & Technology

Submitted: December 24th, 2015

Zhangxin Wanga, Menachem Elimelechb, and Shihong Lina,c* a

Department of Civil and Environmental Engineering Vanderbilt University, Nashville, Tennessee 37235-1831 b

Department of Chemical and Environmental Engineering Yale University, New Haven, Connecticut 06520-8286 c

Department of Chemical and Bimolecular Engineering Vanderbilt University, Nashville, Tennessee 37235-1831

ACS Paragon Plus Environment


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ABSTRACT Interfacial materials with special wettability have become a burgeoning research area in materials science in the past decade. The unique surface properties of materials and interfaces generated by biomimetic approaches can be leveraged to develop effective solutions to challenging environmental problems. This critical review presents the concept, mechanisms, and fabrication techniques of interfacial materials with special wettability, and assesses the environmental applications of these materials for oil-water separation, membrane-based water purification and desalination, biofouling control, high performance vapor condensation, and atmospheric water collection. We also highlight the most promising properties of interfacial materials with special wettability that enable innovative environmental applications and discuss the practical challenges for large-scale implementation of these novel materials.


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INTRODUCTION

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Recent advancements in elucidating the mechanisms of special wetting properties observed in biological surfaces have inspired the development of artificial materials with various types of special wettability1-9. This biomimetic approach emphasizes the indispensable role of appropriate surface morphology in imparting desired wetting properties that cannot be achieved by tailoring the material chemistry alone10-17. Based on this approach, a large number of techniques have been developed to fabricate interfacial materials with special wettability by either bottom-up synthesis or modification of existing substrates to acquire the requisite surface chemistry and morphology5,18-20.

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A wide range of applications enabled by interfacial materials with special wettability have been proved conceptually or realized in practice21. These applications include selfcleaning textile22-25, oil-water separation26, anti-icing and anti-fogging glass6,27-30, atmospheric water collection31,32, chemical shielding33, corrosion control34-43, and biological adhesion mitigation3,44-50 Beyond these applications, which are of tangible daily-life benefits, novel materials with special wettability have also advanced scientific research and technological developments. For example, these materials have led to smart microfluidics with excellent friction control51-56, template driven patterning of nanoparticles57-64, and precise liquid reprography65,66.

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Interfacial phenomena play a critical role in many environmental processes, including membrane-based separations67-75, adsorption76-81, biological fouling44,82-87, corrosion88-91, interfacial phase transition92-95, and catalytic surface reaction96-98. As wettability is one of the most important surface properties, the ability to engineer surface wetting may open up vast opportunities for innovating and enhancing environmental processes that are controlled or heavily affected by interfacial phenomena.

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This review article provides a critical assessment of environmental applications of interfacial materials with special wetting properties. We first introduce the concept of special wettability, its enabling mechanisms, and fabrication techniques of materials with different types of special wettability. We then review various environmental applications enabled by materials with special wetting properties by examining their working mechanism and effectiveness. Finally, we discuss the practical challenges that must be addressed for these materials to realize their full application potential in environmental systems.

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SURFACES WITH SPECIAL WETTABILITY

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Surface Wetting Properties. The wettability of a solid surface is a macroscopic representation of the interaction between the liquid and the substrate solid material. The most common way to quantify surface wettability is by measuring the contact angle (CA)



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of a sessile liquid drop on a solid surface in air (Figure 1A). The alternative approach of measuring the CA of a captive bubble (Figure 1B) is also often used.

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Figure 1. (A) Definition of contact angle (CA), , based on a sessile liquid drop on a solid surface. (B) Definition of CA based on a captive bubble. (C) Advancing CA, ( ): the maximum CA of a sessile drop before its boundary expands upon increase of drop volume. (D) Receding CA, ( ): the minimum CA of sessile drop before its boundary shrinks upon reduction of drop volume. (E) Sliding angle, : the minimum tilting angle at which the liquid drop starts to slide along the surface. The advancing and receding CA ( and ) can also be defined in this setting as the frontier CA and the tail CA, respectively. (F) Super-repellent surface as characterized by ultrahigh CA and ultralow . (G) A superlyophobic but sticky surface as characterized by both very high CA and . In extreme cases, a liquid drop can stick to a vertical or even a reversed horizontal surface of this kind. (E) Lyophilic but non-sticky surface as characterized by very low CA and ; the liquid does not bead up or stick to the surface.

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A surface is typically considered hydrophobic if the water CA is higher than 90°, or hydrophilic if the water CA is lower than 90°. The convention in the materials science community defines a superhydrophobic surface as a surface not only with a very high water CA (>150°), but also with very low CA hysteresis or sliding angle (to be defined later), usually less than 5° or 10°19,99,100. On the other hand, the definition of superhydrophilic surface is controversial. While some suggests a maximum water CA of 5° as the upper limit48,101, others confine the definition of superhydrophility to only a rough or porous surface99. Note that the classification of surface wettability also applies to oil and other low surface tension liquids, in which the “hydro” in the wettability descriptor is replaced with “oleo” (meaning oil in Latin).

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CA alone, however, does not fully capture the wetting behavior of a surface. The maximum and minimum CA of a liquid droplet with a given solid-liquid boundary are


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defined as the advancing CA, (Figure 1C), and the receding CA, (Figure 1D), respectively102-104. CA hysteresis (CAH) is usually defined as the difference between and (i.e. − )105,106. As a result of pinning, CAH only occurs on surfaces with either morphological or chemical heterogeneities107,108. While CA quantifies the affinity between the liquid and the solid surface, CAH quantifies the mobility of the liquid on the solid surface. An alternative measure of the mobility of a liquid drop on a surface is the sliding angle, , defined as the tilting angle of a flat solid surface at which the liquid drop starts to slide109 (Figure 1E).

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As discussed earlier, a surface is typically considered superhydrophobic or superoleophobic (i.e. super-repellent) if the CA is high and CAH or is low (Figure 1F). However, systems also exist where these two requirements are not met simultaneously. For example, a liquid drop can have both high CA and CAH so that it beads up on a vertical surface or even on a reverse horizontal surface without sliding or falling off110112 (Figure 1G). On the other hand, a system can have both low CA and CA-hysteresis, as exemplified by a surface that is highly slippery to liquids with very low CA6 (Figure 1H).

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Special Wettability. Special wettability typically refers to surface wetting properties that are not commonly encountered in daily life. Some of the most investigated surfaces of special wettability include those that are extremely repellent to water (superhydrophobic)100, to oil (superoleophobic) 15,20,113, or simultaneously repellent to both water and oil (omniphobic) 6,11. There are also surfaces that are in-air hydrophilic but oleophobic (i.e. wetted by water but not oil in air)20; such surfaces are more challenging to develop because liquids of a lower surface tension, such as oil, usually wet a surface more readily than water which has a very high surface tension.

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In addition to surfaces of homogeneous wettability, there exist surfaces of patterned wettability that are partially hydrophobic and partially hydrophilic114-117. Smart surfaces that can switch wettability in response to a variety of environmental stimuli have also been developed12,20,118,119. A schematic diagram illustrating the concepts and relations between different types of surface wettability is given in Figure 2A.



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Figure 2. (A) The relations between different types of most investigated surfaces with special wettability. A surface is considered specially wettable if it has wetting properties that are not usually observed in daily life materials, which include not only those that are super wetting or non-wetting but also those with heterogeneous and stimuli-responsive switchable wetting properties. We note that oleophilicity is not explicitly listed here, as most materials are oleophilic due to the low surface tension of oil. (B) Lotus leaf as an example of superhydrophobic surface120. (C) Fresh rose petal as an example of superhydrophobic but strongly adhesive surface111. (D) Rice leaf as an example of superhydrophobic surface with anisotropic adhesion121. (E) Sharkskin as an example of underwater superoleophobic surface16. (F) The overwing of a desert beetle Stenocara as an example of surfaces with patchy wettability (i.e., heterogeneously wettable)122. (G) Salvinia molesta as another example of heterogeneously wettable surface. The tip of the microstructure is hydrophilic while the rest of the structure is hydrophobic123. In all these examples (from Figure 2B to 2G), multi-scale surface architectures, as highlighted by scanning electron microscopy images shown below the photographic images, are critical to the special wetting property. Figures 2B to 2G are reproduced from Ref. 120, 111, 121, 16, 122, and 123, with permissions.


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Many of the surfaces with special wettability have their biological prototypes in nature16,17. For instance, superhydrophobic surfaces that are non-adhesive, adhesive, and directionally adhesive as can be found on a lotus leaf120,124, a rose petal110,111, and a rice leaf121,125, respectively (Figures 2B, C, D). On the other hand, underwater superoleophicity has been discovered on sharkskin126,127 (Figure 2E) or fish scales128,129, imparting the desired properties for hydrodynamic drag reduction and bio-adhesion resistance. Common to all these surfaces is the presence of a multi-scale surface texture that is the key for creating artificial surfaces with the desired special wettability13,15,16.

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Natural surfaces can also have spatially heterogeneous surface wetting properties. For example, the hardened forewings of Namib desert beetles have microscopic bumps composed of hydrophilic tips and hydrophobic peripheries122 (Figure 2F). This unique structure is responsible for the ability of desert beetles to harvest water effectively from the atmosphere. Another example is the surface of the floating fern Salvinia molesta, which has hydrophobic microtextures with hydrophilic tips and is thus capable of retaining attached air bubbles underwater123,130(Figure 2G).

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MECHANISMS AND FABRICATION TECHNIQUES

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On a perfectly smooth (i.e., non-textured) and chemically homogeneous solid surface, the contact angle, , relates to the surface tensions between solid and liquid, , between solid and gas, , and between liquid and air, , by Young’s equation131: − − = 0

(1)

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The Young’s equation can be derived from a force balance at the air-liquid-solid triple phase boundary line or by minimizing the total interfacial Gibbs free energy of the system. A CA measured on a non-textured surface is defined as the intrinsic CA ( ).

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To date, the highest intrinsic water CA of all materials is about 130°, measured from a closely packed monolayer with –CF3 surface functional groups132,133. The Young’s relation cannot explain a plethora of superhydrophobic surfaces with CA significantly higher than 150° or oleophobic surfaces that repel liquids of very low surface tensions. The missing piece is surface texture, which has been identified as an indispensible characteristic for attaining special wetting properties in many biological and engineered surfaces. In this section, we discuss the underlying principles behind several important types of special wettability and briefly summarize the techniques used in fabricating materials with special wettability.

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Wenzel vs. Cassie Baxter State. For a sessile liquid drop contacting a rough surface in air, there are two possible states: the Wenzel state and the Cassie-Baxter state.



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In the Wenzel state, the liquid fully wets the textured surface so that the liquid-solid contact area is maximized134,135. The apparent contact angle for Wenzel state, , can be related to the intrinsic contact angle, 136: (2) =

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Here, is the surface roughness defined as ratio between the total surface area and the projected surface area, which is always greater than unity. According to eq. 2, surface roughness will always amplify the intrinsic wettability of a surface (Figure 3A), whether it is hydrophilic ( 0) or hydrophobic ( 0), provided the system is in a Wenzel state137. For example, an ultrahigh CA can result from a Wenzel state as long as >90° and the surface roughness is sufficiently high. However, the liquid drops in a Wenzel state system are highly immobile due to pinning, leading to significant CAH5.

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Figure 3. (A) Wenzel state: the rough surface is fully wetted by the liquid droplet; the surface roughness amplifies the intrinsic wetting properties. (B) Cassie-Baxter state: the liquid droplet is supported by a composite surface of the solid substrate and trapped air; surface roughness increases the CA whether the intrinsic CA is lower or higher than 90°. (C) A classic reentrant structure showing a local CA less than 90°11,138 (adapted from Ref.11). (D) Another typical reentrant structure (spherical particles or cylindrical fibers) with a local CA less than 90°. The structures in (C) and (D) suggests from that a Cassie-Baxter state can exist even with an intrinsic CA lower than 90°, which is only possible with reentrant surface texture. (E) Free energy of the system as a function of the position of the liquid-air interface. A system in the Cassie-Baxter state C-B1 has to overcome an energy barrier (C-B 2) to transition to Wenzel state with a lower system free energy.

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Another possible wetting state is the Cassie-Baxter state in which the sessile drop is supported by a composite surface of air and the substrate solid (Figure 3B)102. The original Cassie-Baxter theory was developed for a more general scenario of a chemically heterogeneous surface. For a physically rough surface, air can be trapped in the “pockets”


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between the liquid and the solid substrate, in which case the Cassie-Baxter theory can apply, with air being the ultra-low surface tension “chemical heterogeneity”. 102,108. For a system in the Cassise-Baxter state, the apparent CA, , can relate to the intrinsic CA, , by 107 (3) = −

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where and are the area fractions of the solid-liquid and liquid-air (vapor) interface, respectively, satisfying the relation + = 1. Because air, being part of the composite surface supporting the liquid droplet, is the most hydrophobic and oleophobic material, with an intrinsic CA of 180° for any liquid, is always higher than .

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In fact, it is possible that is significantly higher than 90° even if is lower than 90°. In other words, materials comprising hydrophilic or oleophilic smooth surfaces may lead to hydrophobic or oleophobic rough surfaces in Cassie-Baxter state, but not in Wenzel state10. Another important characteristic of a system in the Cassie-Baxter state is the weak CAH due to very low degree of pinning14,17 . Therefore, the Cassie-Baxter state is not only essential for achieving oleophobicity, but also critical for developing superrepellent surfaces with very low surface adhesion.

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For low surface tension liquids (e.g. oil, alcohol), thermodynamic equilibrium analysis suggests that the Cassie-Baxter state is not a thermodynamic stable state, i.e., the free energy of a Cassie-Baxter system is always higher than that of a Wenzel system139,140. Therefore, unlike superhydrophobicity which can be achieved simply by introducing a high level of roughness on a low surface tension solid surface, oil repellence (oleophobicity) is more challenging to attain due to the absence of the thermodynamically stable Cassie-Baxter state for low surface tension liquids10,139,141,142.

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The key to impart oleophobicity lies in the creation of a re-entrant surface texture to enable a Cassie-Baxter state that is thermodynamically metastable10,11,140,143. A re-entrant texture is a concave topography in which the solid fraction of a cross section of the composite surface decreases as the cross section approaches the “bottom surface”, such as the inverted trapezoid in Figure 3C138. Another more practical way to create re-entrant geometry is to use cylindrical or spherical textures, such as electrospun fibrous networks or deposited nanoparticle layers20. The bottom-half of such structures provides the reentrant geometry required for the existence of the metastable Cassie-Baxter state.

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From a force balance perspective, a re-entrant structure is required to achieve a stable liquid-air-solid triple phase boundary when the local CA is lower than 90° (Figure 3C and 3D). From an energetic perspective, in order to transition from a metastable CassieBaxter state (C-B 1 in Figure 3E) to a thermodynamically stable Wenzel state, the system has to overcome an energy barrier corresponding to another Cassie-Baxter state (C-B 2, Figure 3E) of a higher system free energy144. Therefore, the system is “trapped” in the Cassie-Baxter state of lower system free energy, even if that is not a thermodynamically



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stable state with a global free energy minimum. A thermodynamic metastable CassieBaxter state is only possible with a re-entrant texture, because only with such a texture will the intrusion of liquid into the pore space of the composite layer expand the area of the liquid-air contact, which is energetically unfavorable due to very high surface energy of a liquid-air interface.

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Transition from Cassie-Baxter state to Wenzel state can occur upon increasing hydraulic pressure or shrinking of the liquid drop due to evaporation145, in which case the superlyophobicity breaks down. Therefore, the robustness of super-liquid-repellence, i.e. the resilience of the system against the Cassie-Baxter to Wenzel transition, is an important aspect when developing super-repellent surfaces138,146,147. Numerous studies have been conducted to elucidate the geometric factors dictating such robustness, leading to smart material morphological design based on careful consideration of the local interfacial energy landscape11,140,148.

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Oleophobic/Hydrophilic Surfaces: In-Air vs. Underwater. Because water has a higher surface tension (72.8 mN/m at 20°C) than most other liquids, interfacial thermodynamics dictate that if a surface is hydrophilic, it should as well be oleophilic in air. Therefore, it is practically infeasible for a chemically homogeneous surface to simultaneously acquire both oleophobicity and hydrophilicity in air. However, recent advances in materials science have identified the methods to engineer surfaces with this unusual wetting property149,150.

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The key to design a surface with both in-air oleophilicity and hydrophobicity is the creation of a chemically heterogeneous surface with intercalating hydrophilic and oleophobic moieties20. In the presence of oil, the liquid-solid interface is dominated by the oleophobic constituents, which prevent the oil from wicking the surface. In contact with water, however, the surface texture reconfigures to increase the interfacial contact between the hydrophilic functional groups and water to reduce the system enthalpy via hydrogen bonding, which results in surface hydrophilicity150-152.

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On the other hand, surfaces that are in-air hydrophilic can be underwater oleophobic. Biological examples of this underwater oleophobicity include fish scale, clamshells, and shakskin16,127. These surfaces are typically in-air superhydrophilic and thus prefer to be strongly hydrated underwater. The energetically unfavorable dehydration process, which the system has to undergo before oil contacts the surface, prevents the oil from wetting the surface underwater and provides self-cleaning function to the natural surfaces with this wetting property128,153.

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Switchable Surfaces. Smart surfaces have also been developed that can switch their wetting properties in response to changes in environmental conditions12. Typical stimuli triggering change of wettability include pH119,154, temperature155,156, ultra violet (UV) radiation157,158, electrical field159,160, and magnetic field161. Many of these stimuli-


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responsive surfaces switch between hydrophobic (underwater oleophiphilic) and hydrophilic (underwater oleophobic) states and are thus suitable for controllable oil-water separation.

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The most common approach to stimulate the transition of wetting properties is by chemically transforming the surface functional groups. For example, varying the pH around the pKa of the functional groups in an ionizable polymer coating can alter the surface wettability by adjusting its surface charge119,154; an uncharged hydrophobic and underwater oleophilic surface can become hydrophilic and underwater oleophobic when it is charged. Other common environmental factors that can serve as stimuli for wettability transition include UV-radiation (photo-responsive) 156-158,162 and temperature (thermal responsive) 155,163.

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A different approach to create surfaces with switchable wettability involves a phenomenon called electrowetting on dielectric164, which has impact only on polar liquids (e.g., water) but not on non-polar liquids (e.g., oil) 160. Upon the application of a strong electric field, an originally omniphobic Cassie-Baxter surface becomes wetted by water but not by oil, therefore enabling a smart surface that switches its water affinity but maintains oleophobicity. Another interesting approach for controlling the surface wetting through transition between the Cassie-Baxter and the Wenzel states is the application of a magnetic field to alter the surface morphology161. A surface composed of ferromagnetic micro-nails with low surface tension is omniphobic due to the presence of the reentrant structure. However, in the presence of a magnetic field, the deforming surface morphology loses its reentrancy and thus render the surface omniphilic.

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Slippery Liquid Infused Porous Surface (SLIPS). A noteworthy category of very robust omniphobic and anti-adhesion surfaces is the slippery liquid-infused porous surface (SLIPS) method, inspired by the slippery surface of pitcher plants7. A SLIPS is constructed simply by infusing a porous solid substrate with a perfluorinated lubricant. This ultralow surface tension lubricant locked up in the porous substrate does not mix with and cannot be replaced by any tested liquids in contact with the surface6. A SLIPS works with a mechanism categorically different from a Cassie-Baxter surface. For most liquids, both the CA and CAH on SLIPS are very low. Therefore, a SLIPS is considered simultaneously “slippery but wetted”165.

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Without resorting to air pockets for supporting the contacting liquids, a SLIPS can sustain robust omniphobicity under extreme pressure6. A SLIPS does not lose its high repellence due to the evaporation of liquid droplets (in air) or the dissolution of entrapped air (underwater). Furthermore, a SLIPS is also self-repairing due to the facile reconfiguration of a disturbed lubricant liquid film6,166. Because of these advantages, a SLIPS has been proposed for many applications such as fouling inhibition167-169, enhanced condensation170, anti-icing and anti-frosting surfaces29, and drag reduction18,171.



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Fabrication Techniques. The techniques for fabricating interfacial materials with special wettability are heavily dependent on their enabling mechanisms. These materials can be standalone, such as electrospun fiber mats 10,172,173, or be acquired by modifying substrate surfaces of different materials with a wide range of techniques. The fabrication approaches can be either top-down, such as templating and photolithography, or bottomup, such as surface sol-gel and layer-by-layer deposition18.

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The fabrication of surfaces with very high water CA is relatively straightforward, as it typically only requires a highly textured surface composed of materials with low surface free energy18,19,174. A multitude of such techniques have been developed and will not to be discussed here. Selected fabrication techniques of other “more interesting” surfaces with special wettability, such as those that are omniphobic, in-air and underwater oleophobic but hydrophilic, as well as smart surfaces with stimuli-responsive switchable wettability, are listed in Table 1. Readers interested in developing surfaces with special wettability should refer to the plentiful review articles in materials science5,18-20,175

311 Table 1. Selected Fabrication Techniques for Surfaces with Special Wettability Wettability

Omniphobic

Materials (Substrate/Coatings)

Fabrication Method

Cellulose/ Poly Glycidyl methacrylate (PGMA) and pentadecafluorooctanoyl chloride

Atom Transfer Radical Polymerization (ATRP)

Glass/ Poly methyl methacrylate (PMMA) and fluorine-end-capped polyurethane

Casting

Poly 3,4-ethylenedioxythiphene (PEDOT) film / poly perfluorodecyl acrylate (PFA)

Chemical Vapor Deposition (CVD)

Poly perfluoroalkyl ethyl methacrylate (PPFEMA) / polycarprolactone (PLA)

Electrospinning and CVD

Standalone mat of PMMA and polyhedral oligomeric silsesquioxane (POSS)

Electrospinning

Any surface/ Fluorodecyl POSS

Dip-coating

Alumnia/ 1H,1H,2H,2H-perfluorooctyltrichlorosilane

Dip-coating

Glass / silica nanoparticles (SiNPs) coated by perfluoropolyether (PFPE) derivative

Dip-coating

Silicon nanostructure/ heptadecafluoro-1,1,2,2- tetrahydrodecyl trichlorosilane CF2-(CF2)7(CH2)2SiCl3

Etching and molecular phase deposition

Silicon nanostructure/cellulose nanocrystal coated by fluorinated trichlorosilane

Plasma-Etching

Acrylic fabrics/perfluoroalkyl acrylate copolymer and methoxymethyl melamine resin

Plasma and pad-dry-cure method

Standalone mat of polydimethylsiloxane (PDMS) and polytetrafluoroethylene (PTFE)

Plasma discharge

Glass/ SiNPs coated by (Tridecafluoro-1,1,2,2,-tetrahydrooctyl) trichlorosilane n-C6F13(CH2)2SiCl3

LBL assembly

Glass or Printing paper/ SiNPs coated by fluorinated diblock copolymer

Polymerization and Sol-gel

Cotton fabric/ diureapropyltriethoxysilane [bis(aminopropyl)-terminated polydimethylsiloxane] and 1H,1H,2H,2H-perfluorooctyl-triethoxysilane (PFOTES)

Sol-gel

Poly ethylene terephthalate (PET)/colloidal silica, tetraethyl orthosilicate (TEOS), and heptadecafluoro-1,1,2,2-tetrahydrodecyl triethoxysilane

Sol-gel

Polypropylene (PP) / SiNPs coated by perfluoroalkyl methacrylic copolymer

Spin-coating

Quartz glass substrates/ Aligned carbon nanotubes (ACNT) coated with heptadecafluorodecyl trimethoxysilane

Pyrolysis

Metals/ perfluorocarboxylic acid in ethanol

Solution-immersion

Ref. 176

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185

186 187

188

189

190

191

40,19

Cotton textiles/ SiNPs coated by 1H,1H,2H,2H-perfluorodecyl trichlorosilane

Solution-immersion

Nylon Cotton blended fabric/ fluorosilane

Solution-immersion

Silicon wafer/ PMMA and POSS

Spraying


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In-Air Oleophobic Hydrophilic

Underwater Oleophobic Hydrophilic

Templated PDMS, or polyurethane (PU), or ultra-high-molecular-weight polyethylene (UHMWPE), or PTFE

Template

Gold plate/ Fluorinated 3,4- ethylenedioxypyrrole (EDOP) and 3,4propylenedioxypyrrole (ProDOP) monomers

Electrochemical Polymerization and Electrodeposition

Nanopyramidal gold film/ 1H,1H,2H,- 2H-perfluorodecanethiol

Electrodeposition

Silicon/ Perfluorinated polyethylene glycol oligomers (f-PEG)

Grafting

Various substrates/ SiO2 coated with poly diallydimethylammonium chloride (PDDA) and sodium flurooctanoate (PFO)

Spray casting

152

Glass slide / Polycrystalline anatase TiO2 thin film

Sol-gel and UV illumination

198

Spin-coating

149

Dip-coating or Spin-coating

151

Stainless steel mesh / polyacrylamide hydrogel

Photoinitiated polymerization

199

Stainless steel mesh / zeolite crystal

Dip-coating and crystallization

PVDF membrane / poly(3-(N-2-methacryloxyethyl-N,N-dimethyl) ammonatopropanesultone (PMAPS) zwitterionic polyelectrolyte brush

ATRP

201

Cellulose paper / nanofibrillated cellulose hydrogel

Dip-coating and cross-linking

202

Silicon wafers or glass slides / copolymer-fluorosurfactant complex

Spin-coating

150

Sapphire with standard multi-step (RCA) cleaning method (no coating applied)

RCA cleaning

203

Brass abraded by grit silicon carbide papers (no coating applied)

Abrasion

204

Silicon wafer or Polyester fabrics/ POSS and polyethyl methacrylate (PEMA)

Spin coating or Dip coating with water annealing

Glass/ Polystyrene (PS) and montmorillonite (MMT) modified with perfluoropolyether cationic ammonium salts (FOMMT) Stainless steel mesh or polyester fabric / fluorodecyl POSS and cross-linked poly(ethylene glycol) diacrylate (x-PEGDA)

Wettability Oleophobic (w/ PFO) Oleophilic (w/ SDS) Oleophobic (w/o magnetic field) Oleophilic (w/ magnetic field)

Stimuli Responsive

Materials (Substrate/Coating) Etched aluminum surfaces/ Poly diallydimethylammonium chloride (PDDA) and poly sodium 4-styrene sulfonate (PSS) Metal electrode/Ni nanowires with hemisphere cap coated with 1H,1H,2H,2Hperfluorodecanethiol

Superhydrophilic (Temp.40°C)

Silicone substrate/ poly(Nisopropylacrylamide) (PNIPAAm)

Hydrophilic/Oleophobic (Temp=10°C) Hydrophobic/Oleophilic (Temp=40°C)

Stainless steel mesh/ Poly(methyl methacrylate)-b-poly(Nisopropylacrylamide) (PMMA-b-PNIPAAm) block copolymer

195

196

197

27,28

200

205

LBL deposition and counterion exchange

206

Template-assisted eletrodeposition

161

Polymerization

155

Solution casting

163

Omniphobic (dark) Omniphilic (w/UV)

Silicon wafer/ TiO2 and SWNT coated with 1H,1H,2H,2H-perfluorodecyltrichlorosilane (FDTS)

Composite liquid phase deposition

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Hydrophobic (dark) Superhydrophilic (w/UV)

Copper substrate/multiwall carbon nanotubes

Spray casting

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Superhydrophobic (dark) Superhydrophilic (w/UV)

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CVD

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Stainless steel mesh/ aligned ZnO nanorod

In-situ crystallization

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Oleophobic (w/ low voltage) Oleophilic (w/ high voltage)

Nanonail covered substrate/ floropolymer

Photolithography and CVD

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Nylon membranes/ fluorodecyl POSS and crosslinked polydimethylsiloxane (x-PDMS)

Dip-coating

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Textile or polyurethane sponge/Silica Nanoparticles grafted with Poly(2-vinylpyridine-bdimethylsiloxane) block copolymer (P2VP-bPDMS)

Block-copolymer grafting

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Hydrophilic/UW Oleophobic (High pH) Hydrophobic/UW Oleophilic (low pH)

Nanostructured copper foil/ mixture of long chain saturated fatty acid and alkane

Solution-immersion

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ENVIRONMENTAL APPLICATIONS

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The elucidation of the mechanisms of special wettability has led to the creation of artificial materials with special wetting properties. These advanced materials have enabled or enhanced several environmentally relevant processes, including oil-water separation, membrane processes, vapor condensation, fog collection, and biofouling mitigation. In this section we review each of these environmental applications of interfacial materials with special wettability by first introducing their environmental relevance, assessing the state of the art, and finally discussing the challenges to overcome to realize large-scale practical applications. Oil-Water Separation, A natural application for materials with special wettability is the separation of oil from water by taking advantage of the differential affinities of oil and water towards these materials26. Removing oil from water is an indispensable process for effective water reuse in many areas including oil and gas production207, as well as petrochemical, pharmaceutical, metal processing, and the food industries208. Oil-water separation also plays a crucial role in oil spill cleanup, which is of significant environmental concern209. Conventional methods for removing oily components from water include physical skimming, centrifugation, oxidation, solvent extraction, flotation, and biological degradation207,210,211. Some of these processes suffer from problems such as high energy-consumption, limited effectiveness, and extensive use of chemicals.

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Figure 4. (A) A hydrophobic/oleophilic filter for separation of oil/water mixtures. (B) A hydrophobic/oleophilic sponge for adsorbing oil from oil-in-water emulsion. (C) and (D) A hydrophilic/oleophobic filter for separation of oil/water mixtures and oil-in-water emulsion, respectively. (E) A hydrophobic/oleophilic filter switches to a hydrophilic/oleophobic filter upon exposure to an environmental stimulus, which can be UV light, temperature, electric and magnetic field, and pH.

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Wettability based separation is a highly effective, energy efficient process for removing oil from water26,212. In general, there are two major types of wettability based oil-water separation systems: selective filters and superhydrophobic absorbents23,137. A selective filter is a porous barrier that allows selective permeation of some components but rejects the others. Many of these selective barriers are fabricated by modifying metal or polymer meshes with characteristic pore sizes of tens or even hundreds of micrometers. These filters primarily operate primarily based on selective wettability rather than size exclusion2,158,199. On the other hand, microfiltration membranes with special wettability have also been developed for highly effective oil-water separation, especially for stabilized emulsions of micrometer or submicrometer sized oil droplets201,213-215. These wettability based selective filters can effectively separate both immiscible oil water mixtures as well as dispersed oil-in-water emulsions, usually with a separation efficiency (or rejection rate) above 99%160,199,202,216,217.

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Many selective filters for oil-water separation are superhydrophobic, but oleophilic (Figure 4A) 2,23,216,218-222. Although such filters are particularly suitable for water-in-oil emulsions222, they have limited applications as they do not facilitate gravity driven separation for phase separated oil-water mixtures 151 and cannot separate oil-in-water emulsion. The more recent development of superhydrophilic-oleophobic materials137,151,152,199-202,215,223-225 leads to a better route for gravity-driven separation of oil-water mixtures or oil-in-water emulsions. Another noteworthy category of materials are those with stimuli-responsive wettability119,158,160,226,227. These smart materials with controllable wetting properties have been developed both in the form of both selective filters and preferential absorbents for on-demand oil water separation.

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Superhydrophobic absorbents are highly porous, sponge-like materials that are superhydrophobic and oleophilic. They can absorb oil from water by up to tens of times of the adsorbent original weight228-233. An interesting idea for implementing superhydrophobic absorbents for cleaning up oil spills in ocean or surface water is to equip a boat surface with these porous materials as a mobile scavenger for oil232. Effective and economical regeneration of these absorbents, however, remains a significant challenge for their large-scale practical applications.

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Water Purification and Desalination Membranes. The wettability of a membrane is one of the most critical material properties that dictate its performance. Some membrane processes are strongly dependent on surface wetting property, such as membrane distillation67 and membrane-based gas stripping234,235, in which the non-



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wetting condition is pivotal to the process viability. However, even for membrane processes based on other mechanisms such as size exclusion (e.g. nano- and ultrafiltration) and solution-diffusion (e.g. reverse osmosis, forward osmosis), wettability still plays an important role in membrane performance236-242. In this subsection, we will present several examples highlighting how special wettability can markedly enhance the performance of membrane processes.

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Membrane distillation. Membrane distillation (MD) is an emerging thermal desalination process using a hydrophobic microporous membrane67. In an MD process, a hot saline feed stream is separated from the cold pure distillate stream by a hydrophobic, porous membrane. The trans-membrane difference of partial vapor pressure induced by the temperature difference drives vapor transport across the membrane, while the hydrophobic membrane rejects the direct passage of the liquid feed solution that contains salts and other contaminants. MD can utilize low temperature waste heat to desalinate highly saline brine solutions that cannot be treated by conventional reverse osmosis desalination, such as shale gas produced water243. In addition, MD also has the advantage of small system footprint and low capital cost244. It can also be utilized as a low-cost thermal separation process in hybrid-membrane processes for resource recovery from wastewater245,246, energy recovery from waste heat247, and draw solution regeneration for forward osmosis processes248-250.

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In an MD process, the hydrophobic membrane serves as a medium for water vapor transfer and as a barrier for liquid transfer. Therefore, it is of vital importance to maintain the non-wetting condition of an MD membrane to prevent the feed stream from passing through the membrane in its liquid form. Typically, MD membranes are made of hydrophobic materials such as polytetrafluoroethylene (PTFE) prepared via meltingstretching technique, and polyvinylidene fluoride (PVDF) and polypropylene (PP) prepared via phase inversion67,251. However, their application in industrial-scale systems has been hindered by low water flux and low long-term wetting resistance. In particular, if the feed stream is enriched with surface-active agents (e.g. surfactants), these membranes will be wetted by the surface-active agents and fail as a barrier for liquid transfer, resulting in significantly compromised rejection of salt and other undesirable contaminants.

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Approaches to mitigate wetting of MD membrane include the development of composite hydrophilic/hydrophobic membranes252, superhydrophobic membranes253-255, and omniphobic membranes256. To fabricate superhydrophobic MD membranes, a commercial hydrophobic PVDF membrane was modified by coating perfluorinated TiO2 nanoparticles on the membrane surface253. Compared to the pristine PVDF membrane, the modified composite membrane showed a significant higher water CA and drastically reduced CAH. Such a membrane also showed significantly improved anti-wetting performance compared to the pristine PVDF membrane in direct contact MD experiments in which added ethanol lowered the overall surface tension of the feed solution. A similar


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approach can be applied with electrospun nanofiber mats, which offer particularly high promise for MD membranes due to their ultra-high porosity. Superhydrophobic electrospun nanofiber mats produced from a blend of silica nanoparticles and PVDF exhibited higher water flux and long-term wetting resistance compared to commercial flat sheet PTFE and PVDF membranes255.

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Recently, an omniphobic MD membrane was developed by perfluorinating a silica fibrous membrane decorated with nanoparticles256. The fabricated omniphobic membrane was found to be superior to a commercial PTFE membrane as it resisted wetting by low surface tension liquids including mineral oil, ethanol, and decane. The oleophobicity of the fabricated MD membrane stemmed from both the low surface tension and the multiscale (i.e. both the fiber and the nanoparticle scales) re-entrant structures of the membrane10. The versatile wetting resistance of the omniphobic membrane resulted in superior anti-wetting performance in an MD process. Specifically, it was shown that with the addition of surfactants to the feed solution, the salt rejection of an MD process was drastically crippled with a PTFE membrane, but unaffected with an omniphobic membrane. Imparting MD membrane with omniphobicity is a promising direction to enhance the robustness of operation and enable MD to be more versatile in treating a wider range of feed waters. However, successful application of omniphobic membranes in MD requires further work, including assessment of long-term operation and development of scalable fabrication methods.

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Pressure and Osmosis Driven Membrane Processes. Membrane processes based on size exclusion and osmosis mechanisms can also benefit substantially from enhanced surface wetting properties257,258. For example, it has been well established that increasing the hydrophilicity of membranes can improve membrane performance by mitigating organic or biological fouling in ultrafiltration241,259, nanofiltration236,260, reverse osmosis238,261, and forward osmosis262-264.

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The underlying antifouling mechanism of hydrophilic membranes is attributed to the hydration layer formed on a highly hydrophilic surface. Such hydrated layers create an energetic barrier that the organic or biological foulants have to overcome (i.e. to dehydrate the surface) before they can attach onto the membrane surface265. Typical organic or biological foulants are either hydrophobic or have hydrophobic moieties, and thus have a stronger tendency to bind with a hydrophobic surface due to the long-range hydrophobic interaction in water266,267. We note that the mechanism of superhydrophilic membrane for fouling mitigation shares similarity with that of superhydrophilicunderwater oleophobic filters for oil-water separation. Numerous studies have reported the preparation of superhydrophilic membranes by coating nanoparticles237,262,268 or grafting polymers 238,269-271 that are highly hydrophilic, showing that the modified membrane with improved wettability can lead to better performance with slower flux decline over time.



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Surfaces with special wettability can bring anti-fouling performance to the next level. Recent studies suggest that novel ultrafiltration membranes with in-air hydrophilicity and oleophobicity offer anti-fouling performance that is unmatched by membranes that are inair oleophilic217,272. The hydrophilic/oleophobic membranes were obtained by incorporating a functional polymer that contains both hydrophilic and oleophobic moieties into a PVDF membrane. Compared to PVDF membranes without any modifier or with poly ethylene glycol (PEG)—a common surface coating agent to impart hydrophilicity—the hydropholic/oleophobic PVDF membrane demonstrated superior resistance against fouling by proteins (bovine serum albumin), natural organic matter (humic acid), oil-water emulsion, as well as bacteria (Escherichia coli and Staphylococcu aureus). The enhanced anti-fouling performance was evidenced not only by the significantly slower flux decline, but also by the remarkably higher performance recovery upon membrane cleaning217.

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Biofouling Control. Biological fouling (or biofouling), the accumulation of microorganisms and their excreted matter on surfaces, has been a major challenge to the long-term performance and reliability of engineered systems. For example, biofouling of marine vessel surfaces leads to persistent detrimental impacts, including significantly increased hydrodynamic drag and expedited corrosion via microbial induced corrosion or microbial deterioration of applied anti-corrosion coating86,273-275. Typical marine biological foulants include proteins, bacteria, Ulva spores, Navicula diatoms, tubeworm larva, and barnacles, spanning a very broad size-scale, from tens of nanometers to hundreds of micrometers276,277. In addition to marine biofouling, microbial biofouling is also a major concern in numerous other environmentally relevant systems such as heat exchangers in power plants84,85, water treatment and distribution systems87,278-281, and environmental sensors275,282. Biofouling in these systems results in reduced efficiency of mass and heat transfer, pipe blockage, potential secondary contamination, and even complete failure of the systems.

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For microbial fouling, a typical biofouling process has four critical stages: conditioning, attachment, colonization, and biofilm growth283. Therefore, measures to mitigate microbial fouling can either focus on hindering cell attachment or on inhibiting microbial growth. Early biofouling coatings mostly focused on inhibiting microbial growth by applying biocidal antifoulants such as tributyltin (TBT). It is estimated that TBT-based biocides have been applied to over 70% of the global marine fleet273. However, TBT-based antifouling coatings pose environmental and ecological problems by having deleterious effects on various marine organisms284,285. Consequently, regulations are being developed for a global TBT phase-out and a transition to TBT-free anti-fouling coatings273.

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Engineering the surface morphology and wetting properties using a biomimetic approach may offer an alternative route for developing environmentally friendly


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antifouling coatings. For example, lotus-leaf inspired superhydrophobic surfaces haven been acclaimed for their self-cleaning property in air, as the water droplets rolling off the leaf can easily collect the contaminants on its surface 44. Excellent short-term (hours) underwater anti-microbial adhesion performance of superhydrophobic surfaces has also been widely reported286-291.

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However, the complexity of biological fouling poses tremendous challenges for designing a long-term robust underwater anti-biofouling surface. Engineered superhydrophobic materials with a Cassie-Baxter interface are found to lose their superhydrophobicity within a moderate time frame (weeks) upon exposure to euphotic seawater277,292. This observation can partially be explained by the fact that the underwater Cassie-Baxter state is not sustainable: the air pockets in a Cassie-Baxter interface vanish overtime due to dissolution of the trapped air into the water293. Furthermore, even the short-term effectiveness of superhydrophobic surfaces is highly dependent on both the material used and the type of microorganisms involved in biofouling 289,294.

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A more robust strategy for underwater biofouling mitigation may be to create in-air superhydrophilic surfaces that are underwater superoleophobic. Similar to the mechanism of anti-oil-fouling, the water molecules in the highly hydrated coating layer act as an energetic barrier to cell or protein adhesion, thereby preventing protein adsorption settlement of microorganisms 265,295,296. This mechanism has been adopted by several natural marine anti-fouling surfaces such as sharkskin, fish scale, and clamshell297. Following this principle, polymers with poly (ethylene glycol) side chains (i.e. PEGylated polymers) are often used to impart strong hydrophilicity for anti-biofouling surfaces298300 . Other hydrophilic surface coatings successfully implemented for biofouling mitigation include zwitterionic polymers and polymers integrating oligosaccharide moieties301.

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It is important to stress that biofouling is a complex phenomenon and so is the mechanism for biofouling mitigation using microtextured surfaces with special wettability297. The surface wetting property might not be the only player in combating biofouling. For example, the microtexture on the sharkskin can reduce hydrodynamic drag, which in turn promotes fast water movement in the vicinity of the skin and deters the settlement of marine organisms 302-304. Therefore, the hydrodynamic aspects of the system should also be considered when designing anti-biofouling surfaces in dynamic systems. On the other hand, microtextured surfaces also discourage the settlement certain marine organisms larger than the characteristic length scale of the surface texture305.

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SLIPS is another promising potential avenue for battling biofouling both in air and under water. Several representative bacteria, including Staphylococcus aureus, Pseudomona aeruginosa, and Escherichia coli have been used as model microbial foulants to challenge a PTFE-impregnated SLIPS50,167. Superior anti-adhesion performance of SLIPS was observed as compared to the pristine PTFE membrane or to a PEGylated surface167. Due to the absence of surface roughness that microorganisms can



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anchor onto and the ultralow surface tension of the infused liquid, SLIPS can potentially be a highly robust approach for biofouling mitigation.

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Enhanced Vapor Condensation. Vapor condensation plays an important role in a wide variety of natural and engineered systems. It has significant impact on several environmentally relevant processes at the water-energy nexus such as thermal power generation, heat management, water distillation, and atmospheric water collection95. Enhancing the performance of vapor condensation can result in higher efficiencies of energy generation and energy usage, or lead to more energy-efficient means of augmenting the fresh water supply.

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Depending on the morphology of the condensate, vapor condensation is classified in two major categories: film-wise condensation (FWC) and drop-wise condensation (DWC) 306-309. FWC occurs when the condensing surface is hydrophilic, in which case the condensate forms a liquid film over the wetted condenser surface (Figure 5A). In comparison, DWC occurs on a hydrophobic condensing surface, with the condensate being discrete droplets on the surface rather than a continuous liquid film (Figure 5B). Because a liquid film of condensate creates substantial resistance to heat transfer, DWC offers a significantly higher heat transfer rate than FWC, and is therefore usually the preferred mode of condensation95.

(C) Jumping

(B) Drop-wise

(D) Flooding

HTC Enhancement

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(E) Fine-textured hydrophobic

Coarse-textured hydrophobic Smooth Hydrophobic

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Heat Flux

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Figure 5. (A) Film-wise condensation on a smooth hydrophilic surface. (B) Drop-wise condensation on a smooth hydrophobic surface. (C) “Jumping” condensation on a superhydrophobic surface. (D) “Flooding” condensation on a superhydrophobic surface310. (E) Heat transfer coefficient (HTC) as a function of heat flux for different condensation modes95. A higher HTC at a given heat flux indicates faster heat transfer kinetics. Figures 5A to 5D are reproduced from ref. 308 with permission. Figure 5E is adapted from ref. 95.

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Superhydrophobic surfaces can further enhance the rate of condensation heat transfer by promoting DWC with spontaneous droplet departure95,311. With a hierarchical morphology that imparts superior anti-adhesion property, a superhydrophobic surface can


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drastically increase the heat transfer rate by efficient removal of the small droplets from the condenser surface. The improvement in heat transfer performance and the associated environmental and economic benefits can be substantial. As an example, General Electric has developed a ceramic-based highly stable superhydrophobic coating that can augment the heat transfer performance of a steel surface by a factor of 5 to 8 compared to an FWC with an untreated hydrophilic surface (Figure 5E)312. This superhydrophobic coating technology has been estimated to lead to significant saving of fossil fuel for power plants, and a potential annual reduction of more than 20 million tons of CO2 emission in the United States via a 5% reduction of condenser pressure in coal power plants313.

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Achieving high performance vapor condensation using superhydrophobic surfaces, however, can be technically challenging. Two modes for vapor condensation on a superhydrophobic surface are possible: the “jumping” mode and the “flooding” mode310. When the vapor saturation level is low, water droplets forming on a superhydrophobic condenser can undergo coalescence-driven ejection (Figure 5C)314, which enhances heat transfer compared to DWC on a non-textured hydrophobic surface. Such a “jump” condensation occurs only if the nucleation site density is low so that the spacing between the forming droplets is significantly larger than the length scale of the nano-textures. Recently, a superhydrophobic thermally conductive surface has been applied as the condenser for air-gap membrane distillation315. It was shown that the “jumping” mode condensation served to enhance the overall mass transfer kinetics, possibly by improving the mass transfer coefficient in the air gap.

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For a high vapor saturation level or very high heat transfer rate, however, the nucleation site density could increase to the extent that the distance between adjacent droplets is of a length scale similar to that of the nano-texture, in which case the condenser surface, though being superhydrophobic, can be flooded by the strongly pinned condensate in a Wenzel state (Figure 5D). Such “flooding” mode of condensation yields no benefits for the heat transfer rate compared to DWC on a non-textured hydrophobic surface316,317.

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In light of possible of different condensation modes with contrasting consequences, successful implementation of a textured superhydrophobic surface for enhancing condensation rate requires better control of nucleation density by engineering both surface chemistry and morphology. Another possible strategy to promote high performance DWC is using a SLIPS30,170. The distinct advantage of SLIPS over textured superhydrophobic surfaces is the combination of the ultra-low liquid adhesion, which is essential for efficient droplet removal, and the absence of surface roughness, which leaves no possibility for Wenzel state pinning caused by condensation in the microscopic air pockets170.

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Overall, the development of superhydrophobic surfaces for high performance vapor condensation is still in its infancy. Although a plethora of recent studies have been conducted to further elucidate its mechanism310,316-324 or to test new materials for this



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application170,325,326, many practical considerations remain to be addressed before fullscale industrial application. In particular, uncertainties remain regarding the long-term chemical and mechanical stability of these coating materials as well as their economical and scalable fabrication. Nonetheless, the demonstrated potential enhancement of heat transfer performance by these novel materials, and the tremendous economic and environmental benefits as a consequence of such enhancement, suggest a promising future of engineering surface wetting properties for high performance vapor condensation.

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Atmospheric Water Collection. Another important environmental application of interfacial materials with special wettability for vapor condensation is atmospheric water collection from fog or dew in areas where fresh water is scarce327. With suitable meteorological conditions, atmospheric water collection using well-designed water collectors, can be an energy-free approach to harvesting high-quality water to augment the fresh water supply in arid areas. The challenge, however, is efficiency, which directly impacts the unit cost of water production via fog or dew collection.

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Biological systems provide significant insights for designing high performance surfaces for atmospheric water collection. Examples include water-capturing desert beetles whose overwings bear both hydrophilic and hydrophobic patches122, and watercollecting spider silk with a periodic structure comprising highly hydrophilic spindleknots and less hydrophilic joints328. These efficient natural water-collection systems suggest that an ideal fog-harvesting surface should comprise hydrophilic and hydrophobic regions, the former to promote nucleation and the latter to confine the forming droplets until they reach a critical size for droplet departure.

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Following this principle, micro-patterned surfaces with heterogeneous wetting properties have been developed32,329,330. In a recent study where hydrophilic spots were created by inkjet printing of polydopamine onto a superhydrophobic surface, it was observed that a well-designed heterogeneously wettable surface can more than double the water collection rate compared to a superhydrophobic surface330. However, results from other studies with heterogeneous wettable surfaces revealed trivial32 or even negative329 impacts of patterned wettability on water collection rate. The effectiveness of a patterned superhydrophobic/superhydrophilic surface in enhancing water collection rate seems to be dependent on the pattern of the patches and the operation conditions, including the surface tilting angle331. More comprehensive and systematic investigations are needed to further unravel the influence of pattern geometry and wettability on the droplet formation rate as well as the surface mobility of the condensate droplets.

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Outlook

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Many environmental processes are governed or heavily affected by interfacial phenomena in which surface wetting plays a critical role. Therefore, the ability to tailor surface wettability creates tremendous opportunities to develop novel environmental applications or enhance existing environmental processes. Several examples of environmental applications empowered or augmented by materials with engineered surface wettability have been discussed in this review. These include oil-water separation, membrane separations for desalination and water purification, biofouling mitigation, enhanced vapor condensation, and atmospheric water collection. Interfacial materials with special wettability have also been used in other environmentally relevant applications, such as corrosion inhibition36,332-335, drag reduction51,52,171,336, and catalytic surface reaction337-340.

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Innovations in materials science have historically fueled advances in environmental science and engineering. This has been the case in the development of environmental catalytic materials96,97,341,342, water purification and desalination membranes343-345, environmental sensors346,347, and various environmental applications of nanomaterials348352 . Interfacial materials of special wettability have been a bourgeoning research field in materials science for the past decade; the field is still growing at a fast pace7. The science and technology in this field have gained sufficient maturity to be leveraged for developing novel solutions to pressing environmental problems in which interfacial phenomena are so pivotal.

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Although significant progress has been made to fabricate interfacial materials with various types of special wettability, full-scale implementation of these materials in environmental applications still requires further research efforts to understand their longterm performance in complex and challenging environmental conditions. In the mean time, the materials science community continues its efforts to make materials with novel wetting properties more robust and sustainable, and to develop techniques for scalable fabrication of these materials. We believe these advances in materials design and fabrication will further enhance the development of creative and effective solutions to challenging problems concerning environmental interfaces.

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Acknowledgement

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We acknowledge the financial support from Bureau of Reclamation, Department of Interior, via DWPR Agreement R15AC00088, and the partial support to this effort from the Advanced Research Projects Agency-Energy (ARPA-E), U.S. Department of Energy, via Grant DE-AR0000306.



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Environmental Applications


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Surfaces with Special Wettability ACS Paragon Plus Environment

Bio-inspired titanium dioxide materials with special wettability and their applications.

Hierarchically nanostructured materials for sustainable environmental applications.

Wettability of elastomeric impression materials and voids in gypsum casts.

Soft interfacial materials: from fundamentals to formulation.

LED-controlled tuning of ZnO nanowires' wettability for biosensing applications.

Environmental degradation of composites for marine structures: new materials and new applications.

Bioinspired super-wettability from fundamental research to practical applications.

Interfacial dynamics of two immiscible fluids in spatially periodic porous media: the role of substrate wettability.

Recent Progress in Advanced Nanobiological Materials for Energy and Environmental Applications.

Polydopamine and its derivative materials: synthesis and promising applications in energy, environmental, and biomedical fields.

Interfacial properties and design of functional energy materials.

Interfacial Materials for Organic Solar Cells: Recent Advances and Perspectives.

Laser photopolymerization of dental materials with potential endodontic applications.

Effect of disinfectant solutions on the wettability of elastomeric impression materials.

Environmental efficiency of energy, materials, and emissions.

Modification of the Interfacial Interaction between Carbon Fiber and Epoxy with Carbon Hybrid Materials.

Modeling of soft interfacial volume fraction in composite materials with complex convex particles.

Organic-inorganic hybrid materials: nanoparticle containing organogels with myriad applications.

Absorbing materials with applications in radiotherapy and radioprotection.

Interfacial sciences in unconventional petroleum production: from fundamentals to applications.

Use of tar pitch as a binding and reductant of BFD waste to produce reactive materials for environmental applications.

SiO2 system.

New Cork-Based Materials and Applications.

Electrospun Nanofibers: New Concepts, Materials, and Applications.