Nature-inspired Liquid Infused Systems for Superwettable Surface

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Review

Nature-inspired Liquid Infused Systems for Superwettable Surface Energies Zahra Ashrafi, Lucian A. Lucia, and Wendy E. Krause ACS Appl. Mater. Interfaces, Just Accepted Manuscript • Publication Date (Web): 23 May 2019 Downloaded from http://pubs.acs.org on May 23, 2019

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ACS Applied Materials & Interfaces

Nature-inspired Liquid Infused Systems for Superwettable Surface Energies Zahra Ashrafi†, Lucian Lucia‡†§*, Wendy Krause†

ZA: https://orcid.org/0000-0002-7205-8127 LL: https://orcid.org/0000-0003-0157-2505 WK: https://orcid.org/0000-0001-8527-4470

†Fiber and Polymer Science, NC State University, Campus Box 7616, Raleigh, North Carolina 27695, United States

‡Department of Forest Biomaterial, NC State University, Campus Box 8005, Raleigh, North Carolina 27695, United States; Department of Chemistry, NC State University, Campus Box 8204, Raleigh, North Carolina 27695, United States

§State Key Laboratory of Bio-based Materials & Green Papermaking, Qilu University of Technology / Shandong Academy of Sciences, Jinan, PR China 250353

*[email protected] KEYWORDS: liquid infused systems, slippery surfaces, super-wetting, super-antiwetting, repellency

ACS Paragon Plus Environment

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ABSTRACT

The development of an innovative interfacial wetting strategy known as liquid infused systems offers great promise for the advanced design of super-wetting and super-antiwetting substrates to overcome the drawbacks of textured surfaces classified under the heading of Cassie/Wenzel states. The potential value of nature-inspired surfaces has significant potential to address scientific and technological challenges within the field of interfacial chemistry. The objective of the current review is to provide insights into a fruitful and young field of research, highlight its historical developments, examine its nature-inspired design principles, gauge recent progress in emerging applications, and offer a fresh perspective for future research.

INTRODUCTION

Many phenomena dealing with wettability in nature, such as the water-resistance properties of duck feathers,1,2 the self-cleaning effects of lotus leaves and cicada wings,3,4 the anisotropic surfaces of the rice leaf and filefish skin,5,6 and the legs of water strider,7 inspire research efforts to uncover the mechanisms of the special wettability on these surfaces. Such efforts are of paramount significance because potential solutions have vast implications for resolving a wide variety of real-world challenges.

Despite several decades of intense research that has resulted in the fabrication of complex liquidrepellent micro-/nanostructured surfaces in the so-called Cassie/Wenzel state, relying on reductions in surface energy and enhancing surface roughness, these surfaces still show


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limitations to treat real life challenges due to their low durability upon wear damages.8-11 Following the Cassie state strategy, fabricating surfaces that are repellent to low surface tension liquids such as organic liquids and alcohols are much more difficult to achieve due to the low surface tension and polarity of the liquids themselves.12,13 To address this deficiency, broad attention has been drawn to the wettability of a liquid/liquid/solid tri-phase and air/liquid/liquid/solid tetra-phase systems.14,15

Inspired by the antiwetting behavior of oil droplets on fish skin and Pitcher plant of the genus Nepenthes, liquid infused systems (LIS) as an alternative interfacial wetting concept was introduced.16,17 This strategy is based upon infusing a barrier liquid phase into porous solid materials to induce slippery and repellent character toward liquids of differing polarity. Contrary to Cassie state systems, the intermediary liquid layer in liquid infused systems separates the solid substrate from the contaminating liquid through preventing direct contact between the substrate and the targeted contaminating liquid.

This review focuses on nature-inspired principles and underlying mechanisms to design and fabricate liquid infused systems. In order to provide a proper context for the work contained herein, a brief background on main milestones and theories in the field of wetting will be provided. It will also discuss in detail that how the liquid infused technology can address some of the intrinsic limitations of repellent surfaces inspired by the Cassie/Wenzel state. At the core of soil porous templates, super-wettability and super-spreading properties of gels, another class of liquid infused systems will be discussed to demonstrate their great promise for the fabrication of


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supraparticles and ultrathin solid films. Then, emerging applications of these materials according to recent advances in this young field of research will be highlighted. Finally, perspectives on future research developments in this field will be given.

BACKGROUND

“Wetting”, as a technical term for the current review, is limited to the wetting of solids by liquids that represents an intrinsic property of a solid surface under the control of intermolecular adhesive interactions between the two phases.18 Young was a pioneer who in 1805 promoted the concept of “contact angle”, the angular displacement equilibrium behavior of a droplet on a flat and perfectly smooth surface.19 Discovery of low-surface-energy polymers such as fluoropolymers and silicones allowed for the development of surfaces with higher contact angles.11,12 Later developments lead to a deeper understanding of the critical factors controlling wettability such as surface topographic structure.12 In 1936, Wenzel22 explained how the roughness of a solid surface enhances apparent water contact angle and hydrophobicity. The paper entitled “Wettability of Porous Surfaces” in 1944 by Cassie and Baxter23 introduced the “composite wetting model”, a theory of the wettability of porous surfaces, in which drops rest on an interface whose intrinsic energetics are a composite of the roughness features and trapped air. These theoretical insights into wetting of non-ideal surfaces were very illuminating and still applicable after more than a century. These theories are briefly highlighted in Table 1.


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The famous “Lotus Effect” phenomena familiar to most surface scientists was understood in detail in 1948.3 Approximately twenty years ago, visualizing the surface of the lotus and rice leaves uncovered how the cooperation of micro- and nanoscale two-tier structures and the arrangement of the them on the surface are key structural aspect basis for self-cleaning properties.3,24 This finding prompted a flood of biomimetic approaches for the design of microstructure-based superhydrophobic materials.11,17,26,27 A time-line of several major milestones in the area of repellent surfaces is depicted in Figure 1. These findings sparked extensive developmental work that attempted to replicate the surface characteristics of natural examples, which allowed super-wetting/antiwetting surfaces fabrication from a wide range of materials (i.e., polymers, metals, and inorganic materials such as ceramic and glass). But to have a more robust repellent system, nature-inspired liquid impregnated systems were developed which resist even complex liquids with low surface energy that would completely wet typical microstructured surfaces.28,29,30


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Table 1. Main theories in the field of wetting. The contact angle (θ) of a liquid drop on an ideal (smooth and chemically homogeneous) solid surface, defined by the mechanical equilibrium of the interfacial energies between the solid–liquid (γSL), solid–vapor (γSV), and liquid– vapor (γLV) interfaces can be obtained from Young equation. Wetting states on rough surfaces are mainly described by two models: first, is the Wenzel model in which liquid penetrates inside the rough surface at the point of contact, and the area of the drop’s solid–liquid interface is enlarged by a factor r; second, is the Cassie-Baxter model for the composite interface, in which liquid sits on top of the roughness features, with trapped air pockets. Here, ϕs is the area fractions of the solid on the surface and the liquid– solid contact area is smaller than that in Wenzel. An intermediate state between Wenzel state with high adhesion and Cassie-Baxter state with low adhesion on a same textured surface may also occur when a droplet partially wets a textured surface under external stimuli such as observed by a pushing force. In this case, the drop sinks inside the texture towards a more stable impaled state and displays a strong pinning of the contact line on the surface texture.


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Figure 1. Timeline of the evolution of the field of wettability that emerged in 1804 and is ongoing today. The micrograph of lotus leaf is reproduced with permission from ref 27. Copyright 2008 Royal Society of Chemistry. The micrograph of fish scales is reprinted with permission from ref 31. Copyright 2009 WILEY-VCH.


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LIQUID INFUSED INTERFACIAL MATERIALS

Biomimetics cover the work involved in revealing the mechanism of the wetting phenomena on the surfaces of plants or animals that has consequently sparked extensive developments of artificial superwettability systems. A total of 64 wetting states have been introduced over the past two decades that have been described in detail by Jiang and colleagues.32 Among these extreme wetting states, artificial superhydrophobic materials in a water/solid/air tri-phase system (water wettability on a solid surface in air) have been an area of intensive exploration.33,34 One of the most demanding extreme wetting state concepts is superoleophobicity in which a localized surface repels oil droplets. Due to the low surface tension of most oils, design and fabrication of superoleophobic surfaces is extremely challenging.35,36 In 2009, the concept of the oil-repelling action of fish scales inspired research on inducing wettability among oil/water/solid tri-phases. An interesting phenomenon that fish and clamshells can engage in is keeping their body clean in oil-polluted water; this approach has inspired researchers to study and innovate strategies for fabricating underwater superoleopobic surfaces.37,38

Related research measured oil contact angle of fish scales both in air and in water and showed that superoleophilic properties (complete wetting) of scales in the water/air/solid system were transformed to superoleophobic properties (oil contact angle of 156.4 ± 3.0º) in an oil/water/solid system by substituting the air phase with a water phase. This oil repellent property results from micro- and nanostructures and high-water content of the hydrogel layers of the fish skin.37 In attempts to identify the reasons for such behavior, a study quantified the contact angle of silicon


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oil on fish scales submerged in water with and without a mucus layer by using a needle-free drop deposition technique coupled with illumination to decipher the drop contact area. This work highlighted the importance of the mucus layer formation on fish scales as part of its defense mechanism. Unprecedented oil contact angles of ~ 180º were observed for underwater fish scales containing the mucus layer that possessed specific chemical functional groups. However, in the absence of this mucus layer, the angle reduced to 150º, which could be attributed to the hierarchical micro- and nano-structures on the fish scales.39

Inspired by this biomimetic approach, the concept of slippery liquid-infused porous surfaces (SLIPS) was introduced in 2011 in which a surface is infiltrated with a lubricating liquid, a strategy that provides a straightforward and promising solution for exceptional liquid superwettability and super-antiwettability properties.16 For example, Pitcher plant leaves offer a remarkably simple alternative strategy to design liquid-repellent surfaces. Unlike the lotus strategy that depends on micro- and nano-roughness to exhibit antiwetting properties, Nepenthes Pitcher special leaves use surface microtexture to entrap an immiscible liquid (water) that acts as an effective continuous repellent layer. This wet and slippery surface causes a “hydrophobic” insect to slip and fall into the pitcher plant by repelling the oils on their feet, making escape nearly impossible. The prey-capture effectiveness of the leaf’s surface is further enhanced in moist environments (Figure 2). 40-42


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Figure 2. a) Image of Nepenthes pitcher plant reprinted with permission from ref 48. Copyright 2016 American Chemical Society. b) SEM image of the slippery zone of pitcher plant is reproduced with permission from ref 40 Copyright 2004, National Academy of Sciences of the USA. c) Schematic illustration of a liquid infused surface. d) Filefish N. septentrionalis. e) Sideview and f) Top-view of filefish skin with hook-like microspines. Filefish picture and corresponding SEM images are reprinted with permission from ref 6. Copyright 2013 WILEYVCH.

The liquid infused technology can address some of the intrinsic limitations of repellent surfaces that can be attributed to the Cassie state. First, air pockets trapped within the surface texture of the Cassie state are vulnerable and fragile spots under external constraints over time. To improve the performance of a Cassie state system, the liquid-solid contact area needs to be minimized through enhancing the air gaps among surface features or reducing the diameter of each


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individual feature. However, all of these modifications make the system much more susceptible to irreversible failure under external forces. A recent study took a more realistic approach to investigate the lifetime of Cassie state superhydrophobic surfaces underwater. They observed that these surfaces are prone to rapid irreversible decay and are therefore not thermodynamically and mechanically stable in underwater experiments.43 However, the lubricating liquid layer can serve not only as a repellent layer, but also protect the underlying solid substrate from decomposition. Second, air is generally more compressible compared to liquids. Therefore, trapped air cannot withstand high pressures as effectively as the liquid layer in liquid infused materials. In other words, the intensity at which the liquid pressure threshold on the surface can sustain without being impaled by the external liquid is much higher for liquid infused materials. Other than the action of external forces, increases in pressure can occur for several other reasons such as the existence of surface defects due to mechanical damage or fabrication imperfections. Next, the smooth surface properties of the caged liquid layer at the molecular scale illustrate small contact angle hysteresis (CAH) even under large external applied forces, which is not the case in the Cassie state where the trapped air acts an ineffective cushion against impalement, resulting in liquid penetration into the textured surface, transition to the Wenzel state, and a significant accompanying CAH increases. Finally, most of the liquid-repellent surfaces are effective only for high-surface-tension liquids such as neat water, whereas liquid-impregnated materials repel immiscible liquids of virtually any surface tension. There is strong interest in designing surfaces that repel low surface tension liquids, such as organic liquids, and complex and physiological fluids, such as crude oil and blood for high performance clothes, screens in electronic devices, optical instruments, microfluid handling, and so forth.44,45


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Several efforts have explored the role of re-entrant or doubly re-entrant textures in order to make Cassie state surfaces applicable for repelling low surface tension liquids such as oils, organic solvents, and alcohols.13 Although these latter studies have been showed that re-entrant topography improves the repellency properties of the surface to a great extent, it still is not a satisfactory condition because repellency properties can be compromised at elevated pressures. In a recent study, novel superoleophobic surfaces with the ability to repel low surface tension liquids (Ethanol and n-Octane) were fabricated by combining doubly re-entrant microtopography with lubricant infused porous surfaces (Figure 3). 3D direct laser writing was utilized to fabricate doubly re-entrant micropillars with nano-roughness on top of each pillar (Figure 3b). The top nanostructures were precisely impregnated with a lubricant layer (oil Krytox 103) by employing a robotic microdroplet deposition setup that was capable of softly touching just the top of the doubly re-entrant micropillars. The doubly re-entrant features play a key role in both superoleophobicity properties as demonstrated by how it is able to hold the lubricant layer on top without penetration into the micropillar gaps. This study provides a proof-of-concept for investigating heterogeneous Cassie state liquid infused systems for additional repellency and robustness.46


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Figure 3. SEM and schematic images of doubly re-entrant micropillars with flat and nanoroughness on top of each pillar. A) re-entrant micropillars with flat tops. The inset picture shows a 6 µL ethanol drop deposited on a surface composed of the doubly re-entrant micropillars with a static contact angle of 158 ± 5°. B) Doubly re-entrant micropillars with nano-roughness on top. C) Liquid infused superoleophobic doubly re-entrant surfaces surface formed by combination of a doubly re-entrant structure and a lubricant infused porous surface. Reprinted with permission from ref 46. Copyright 2018 WILEY-VCH.

The first research attempts that used the term SLIPS, slippery liquid-infused porous surfaces, discussed that contrary to other surface antiwetting models which show no self-healing ability, a lubricating film in SLIPS serves as a self-healing coating by simply flowing towards any


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damaged areas by virtue of surface-energy-driven capillary action. This work also pioneered the designing of impregnating nano-/micro-structured surfaces by incorporating several lubricating liquids to repel other immiscible liquids with a broad range of surface tensions.16,47

DESIGN PRINCIPLES

In the process of designing liquid infused substrates, two critical criteria must be fulfilled: 1) The surface energy of the lubricating liquid and solid underlying substrate should be well matched in order to create a durable/stable system. 2) The lubricant and external targeted liquid must be immiscible. In order to prepare a robust system, attractive forces between intermediary liquid layer and the solid substrate should be energetically more favorable than the external contaminating liquid. In the best scenario, the surface energy of the solid substrate matches the impregnating liquid, viz., the surface energy of the surface must be higher than the surface tension of the liquid, while it mismatches the external contaminating liquid to some extent. That way, the intermediary liquid layer will spontaneously wet out the substrate and form a sturdy covering film at the interface. As such, if the intrinsic surface energy of the solid substrate does not match the infusing liquid layer, it can be modified through chemical functionalization.


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Solid Substrate

To fabricate a liquid infused system, a porous template needs to be strategically designed in order to confine the impregnating liquid. 2D and 3D porous templates made of metals, ceramics, and polymer networks and gels can be constructed through bottom–up or top–down approaches. Bottom up techniques such as electrospinning, self-assembly, layer-by-layer, sol-gel,49 etc., are based on the arrangement and orientation of 0D and 1D materials as the basic building blocks. Three different possible 3D liquid-impregnated surfaces can be formed through the arrangement and orientation of 0D simple particles which are shown in Figure 4.


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Figure 4. Possible 3D liquid-impregnated surfaces by arrangement and orientation of 0D simple spherical particles. A) Particles serve to simply hold the infused liquid in place. B) Particles partially or totally absorb infused liquid in their structure. C) empty half spherical particles act as reservoirs for trapping liquids in their hollow structure.

For instance, tunable underwater superoeophobic films can be fabricated by assembling hydrophilic spherical and non-spherical latex particles that give rise to both cauliflower-like and single-cavity designs. The underwater oleophobicity of the films is mainly attributed to the formation of a water-lubricant layer on the hydrophilic latex particles shell surface after the film is immersed in water. The water contact angle of the film assembled from spherical latex particles was highest followed by the cauliflower-like and single-cavity designs (Figure 5).50


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Figure 5. First row; TEM images of a) spherical, b) cauliflower-like, and c) single-cavity latex particles. The inset pictures are 3D schematic image of the latex particles. Second and third row; schematic drawing of contact states of an oil droplet (L1) on a surface assembled from each correspondent particles in water media (L2). S represents solid particles and the pale blue around each latex particle represents the hydrophilic polyacrylic acid shell that forms after the film is immersed in water. Reprinted with permission from ref 50. Copyright 2011, Wiley-VCH.


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The top–down techniques are based on micro-/nano structured templates that are constructed by a number of techniques such as etching,51 lithography,16,52-54 laser, plasma, direct deposition, chemical treatments, and electrochemical anodizing.55 A study reported that anodized alumina surfaces composed of innumerable nanopores were designed to serve as nano-reservoirs to hold low surface tension liquid such as perfluorooctyl acid. After filling up the reservoirs with the assistance of vacuum pumping, substrates displayed superamphiphobicity with contact angles higher than 150 for water, glycerol, CH2I2, hexadecane, and rapeseed oil. When the coating liquid on the top surface is damaged or depleted, low surface energy liquids trapped in the nanoreserviors move to the outermost surface, a phenomenon that is thermodynamically driven. This particular study provided a proof-of-concept example of designing liquid impregnated surfaces that are capable of intrinsic self-healing.8

Solid templates can be flat or possess micro, nano, or hierarchical micro/nano roughness. However, surface topography is an essential part of the design for holding the liquid layer in place through capillary forces.56 Enhancing surface area by introducing hierarchical textures on the surface also increases repellency through more efficient hosting of repellent liquid because solid underlying substrates and liquid layers being held together through either physical bonds, e.g., van der Waals forces, hydrogen bonds, or chemical bonds that include covalent or a combination of both (Figure 6).


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Figure 6. Liquid-impregnated surfaces by arrangement and orientation of 0D spherical building block particles possess: A) None. B) Micro. C) Hierarchical micro/nano roughness.

Dissimilar to lotus leaves which show high repellency and low CAH because of the hierarchical structures, it is been shown that lubricant infused surfaces with uniform nanofeatures offer the most shear-tolerance among flat, microscale, nanoscale, and hierarchically textured liquid infused surfaces subjected to various high shear spinning rates. However, as it was discussed under high acceleration spinning conditions, the capillary length of the lubricant layer is smaller than several microscale features; therefore, the lubricant can be simply depleted in which the underlying substrate is revealed, while the LIS with uniform nanoscale features provide a more robust smooth overcoating layer. Hierarchically textured surfaces properties can then mediate between the micro- and nanostructured surfaces.57 Surface features can display either random or highly ordered orientations. Highly oriented rough surfaces are particularly beneficial for studying the effects of rough structure geometries on differing forms of failure that liquid infused systems are susceptible to such as fluid drainage under shear or gravity forces. Several research efforts have applied existing theories which govern liquid layers entrapped in textured surfaces to describe the role of surface roughness in preventing the infused liquid layer from draining under external forces that it may counter.58-60 It has been discussed that the rough structures


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amplitude, aspect ratio, and gap distance should suit the capillary length of the intermediary liquid layer in order to create a robust system in dynamic fluid environments.58,61 For instance, an analytical model suggested that manipulating the aspect ratio of the surface grooved pattern, with grooves of different width and depth, plays an important role in wicking liquid film due to capillary forces.58 It should be note that the dynamic of drainage is significantly impacted by surface features design if upward or inward. For example, upward features such as bumps/pillars textures cause a different flow behavior in comparison to inward features like arrays of individual holes/pores. Further investigation on optimization of more complicated topographical structures- geometry, size, and spacing- is still required.

Lubricating Liquid Layer

The liquid layer inherent properties provide a dynamic molecularly smooth, homogeneous, low hysteresis, and defect-free interface which is difficult to discover in other materials. However, while liquid layers show the ability to actively self-restore under failure regimes, in practical applications, the dynamics of the fluid layer is fairly complex and not sufficiently responsive to external drainage-forces. If the system is not stable enough, targeted liquids can displace the infused liquid layer by forcing it from the substrate. A recent study visualized the state of a lubricating thin film (silicone oil of viscosity ƞ = 10 cP) confined in a transparent polymethylpentene (PMP) substrate under a static droplet of another liquid by confocal optical interferometry. It was observed that a droplet can adopt three distinct forms under these circumstances as shown in Figure 7 Ι.62 The first state (L1) is l µm water droplet on a flat PMP


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substrate impregnated with silicone oil and shows a wrapping layer. The second state (L2) is water droplet with 60 wt% aqueous sucrose solution which forces the silicon lubricating layer away and forms small pockets underneath without a significance change inapparent contact angle observations. In the third state (L3), a dodecanol droplet completely displaces the silicon oil lubricant layer and wet the PMP substrate. Further investigation explained that the lubrication states for different combinations of solid substrate/lubricating liquid layer/liquid droplet arise from balance interfacial tensions and van der Waals interactions between solid and infusing liquid.62

For a solid substrate made of ultraviolet-cured polymer (NOA 61, Norland) with a hexagonal array of microposts, lubricated with perfluorinated oil by different surface treatments, three wetting states under static conditions were observed (Figure 7 ΙΙ): a stable lubricant film under a droplet of water (SL1), micro-sized lubricant pockets on top of surface roughness (SL2), and complete displacement of lubricant when there is no surface treatment with lubricant layer. These results emphasize that lubricating liquid layer properties are a critical design element for a stable robust liquid infused system.62


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Figure 7. Equilibrium lubrication states for lubricant-infused solid surfaces. Ι) Flat: L1, stable lubricant film (0.1 mm scale bar, θ app = 90), inset 1 (10 µm scale bar) showing the absence of a contact line. L2, unstable lubricant film forms small pockets (0.3 mm scale bar, θ app = 90), inset 1 (15 µm scale bar) shows the three-phase contact line, while inset 2 (40 µm scale bar) is a zoomed-in image of the lubricant pockets. L3: lubricant is completely displaced from by a dodecanol droplet (0.1 mm scale bar, θ app = 23). ΙΙ) With hexagonal array of microposts (diameter DD = 26 µm, pitch p = 50 µm and height hp = 30 µm): SL1, 200 nm fluoropolymer coating; SL2, vapour-phase silanization with perfluorosilane; SL3, no surface treatment. Adapted with permission from ref 62. Copyright 2017, Springer Nature.


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If the lubricant is not selected carefully, “lubricant cloaking” can occur which is the encapsulation of the droplet within a thin layer of lubricant. Cloaking enhances the depletion of the impregnated liquid which can trigger the eventual failure of the system. Interfacial energies of the lubricant and targeted liquid need to be considered. The selected pair not only must be immiscible, but it is better to avoid the ones which show similar surface tension, molecular structure, and polarity, especially when the system is designed for repelling low surface tension liquids.53,63-65 If the targeted droplet has high surface tension, a lubricating liquid must have moderate to high surface tension to overcome the cloaking problem. Lists of the miscibility and cloaking for the different pair of lubricant liquids and low-surface-tension liquids, are outlined herein.65 The viscosity of the lubricant layer is a key factor in determining dynamics of droplet shedding behavior whether it slips or rolls off the surface.53 It has also been shown that for a given external shear-driven flow a lower lubricant viscosity results in accelerated droplet velocity and more infused fluid being detained.66,67 Possible wetting configurations of a liquid infused surface outside and underneath a targeted droplet are shown in Figure 8.


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Figure 8. I) The criterion for cloaking a water droplet with oil infused substrate in air is given by the spreading coefficient, 𝑆𝑜𝑤 = 𝛾𝑤𝑎 ― 𝛾𝑤𝑜 ― 𝛾𝑜𝑎, where γ is the interfacial tension between the two phases designated by subscripts w, o, and a. Thus, Sow > 0 implies that the oil will cloak the water droplet, whereas Sow< 0 implies otherwise. II) Wetting configurations of a liquid infused surface at lubricating liquid-solid substrate-air and lubricating liquid-solid substrate-targeted liquid. III) Gating reconfiguration of a liquid infused membrane. Transport of liquid/gas (purple) will be gated by pressure-induced deformation of the gating liquid (green) which provides a unique strategy for selective, responsive, tunable and antifouling multiphase separation. When the pressure is removed, a non-fouled pore returns to its original liquid-filled state and if there are any particles (orange/yellow), they can be easily rinsed. Inspired from ref 68,69.

Another design element of the lubricating layer that is critical to be considered is thermal stability. Obviously, a liquid layer evaporates after time or elevated temperatures. A potential


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solution to address this issue is employing ionic liquids which display ultralow vapor pressures (~ 10−12 mmHg) because their bulky structure remains in the liquid state for a longer period of time and at higher temperatures. Nevertheles, their complex molecular structure requires more efforts to devise a system with the appropriate interfacial energy between the solid substrate and the ionic liquid layer.70 Moreover, it is been demonstrated that Teflon solid template infused with perfluorinated Krytox 105 repels droplets of complex fluids, e.g., crude oil at 200 C.67 Stabilization and effectiveness of a lubricant thin layer is pivotal to exploring ways to alleviate liquid depletion and improve liquid retention and functionality for developing a thorough, rational system for future practical design.

LIQUID DISPERSED GELS

In contrast with post-impregnation of the porous underlying matrix with liquid, another potentially promising approach is utilizing liquid dispersed gels as robust repelling substrates.71 Gels fundamentally consist of a liquid medium dispersed in a solid 3D cross-linked network assimilated via physical or chemical interactions. Gels are known as a class of soft and flexible materials that can entrap high liquids contents of up to 99% of their dry weight. Owing to their distinctive liquid sorption and retention capacity, they have attracted extensive attention for the development of super-wetting and super-antiwetting surfaces. In response to depletion of the lubricant layer, self-lubricating gels capable of regulate the supplying of dispersion liquid to the surface have been designed.72-74 If the dispersion phase is water, it is a hydrogel; similarly, if it is composed of liquid organic phase, it is an organogel. There are also organohydrogels which


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concurrently employ water and oil as the dispersion medium and quickly adapt their hydrogel or organogel properties in response to the surrounding liquid phase (Figure 9).

For instance, in an underwater situation, the hydrogel component can become dominant and the surface of the organohydrogel become superoleophobic. However, when submerged in an oilbased environment, the surface of the organohydrogel gradually can become more organogel-like and display superhydrophobic properties. The anisotropic hetero-networks of organohydrogels restrict their volume change considerably contrary to the volume changes typically observed in homogeneous networks of organogels or hydrogels. More in-depth information on recent progress of antiadhesion organogel materials are discussed in a specialized review.75

Figure 9. Representative hydrogel, organogel, and organohydrogel systems formed from hydrophilic, oleophilic, hydrophilic, and oleophilic composite networks, respectively.

The super-wettability and super-spreading properties of gels and other liquid infused surfaces tend to show great promise for the fabrication of ultrathin solid films with controlled thicknesses. The entrapped liquid in these surfaces may act as a precursor film for facilitating complete and


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quick spreading of the liquids over the surface by boosting the advancement of a three-phase contact line, while the defects or impurities on a solid surface can induce local pinning, thus restricting infinite spreading of liquids. Following this strategy, a variety of versatile functional multilayer/composite thin films for various potential applications can be promoted including self-cleaning, controllable liquid transport, antifogging, liquid separation, and so forth (Figure 10).76-78 Meanwhile, the extreme liquid repellency and low adhesion properties of liquid-infused gel surfaces can be exploited for the synthesis of supra-particles by evaporation of sessile drops containing nano- or microcolloids. This novel energy efficient approach facilitates fabrication process of supra-particles with various size and compositions which can be used in as selfpropelling particles, small-scale magnetic stirring, storage materials, and catalysts (Figure 10).79,80Such liquid layers can be converted into various functional thin polymer films with adjustable thicknesses (nm- to mm-) through one-step polymerization of the reactants. The current strategy offers opportunities for large-scale synthesis of versatile functional thin films for wide range of applications such as protection, antifogging and antireflection coating lenses and windows, or in nano-fluidics chip technologies such as precursor films for spreading sub-micron scale drops.77,78


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Figure 10. Schematic for supra-particle formation on a superlyophobic liquid infused surface. Due to the high liquid repellency, the shape of the evaporating drop remains spherical throughout the process (left). A thin layer/multilayer/composite solid film formation on a liquid infused superlyophilic surface confined in a two-dimensional space. The rapid spreading of the liquids over the surface enables generating an ultrathin uniform film (right).


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Liquid infused porous membranes are promising alternatives for developing a selective, responsive, tunable, and antifouling phase separation mechanism (Figure 8 III). As a matter of fact, the lubricant liquid’s abilities to flow and readily reconfigure and adapt impart a responsive means not possible with rigid solid materials. In this regard, gels as soft textured solids provide an advanced set of possibilities which arise from their elastic deformation that allow for customized dynamic fluidic functions. The sensitivity of the system to deformation can be tuned by altering effective pore size under different conditions and stimuli which affect the volume fraction and movement of the lubricant liquid.81 Pores can be filled with liquids that display strong affinity toward solid substrates. Consequently, miscible substances can penetrate and be separated, e.g., water-infused membranes/hydrogels for oil-water separation allow the water phase to pass. The system may still allow an immiscible substance to flow through without any contact with the solid surface under specific pressures that may be described as a gating threshold. In both cases, unlike bare pores, the fouling problem by the transport substance will be suppressed. Following this liquid-gated pores strategy, researchers have been able to sort multiphase mixtures air–water–oil and suspensions containing particles larger than the pore diameter without pore clogging and fouling issues.69

ANISOTROPIC LIQUID INFUSED INTERFACIAL MATERIALS

Surfaces with anisotropic wetting properties, widely found in nature, are a new concept in the field of surface engineering. For example, it is been demonstrated that the anisotropic rolling/pinning oleophobicity of water-infused filefish Navodon septentrionalis skin arises from


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the oriented hook-like spines arranged on the surface of the fish skin. These asymmetric microtextures impel anisotropic fluid motion in a head-to-tail direction which allow the fish to remain clean in oil-contaminated aquatic environments.6 Anisotropic surfaces can be artificially achieved through imposing gradients in the chemical and structural features of a surface to account for differences in the energy barrier of wetting on patterned surfaces. For example, chemical heterogeneity of the surface induces a self-running motion of water from the hydrophobic region to the hydrophilic region without any other forces applied.82 In addition, changing periods, width, and spacing of surface structural features affect the transportation of liquid droplets. For artificial materials, liquid-impregnated surfaces generated from the anisotropic arrangement of micro-/nanostructures are ideal substrates for controlling movement of liquid droplets through high contact angles and low contact angle hysteresis. It has been verified that anisotropic micro-grooved organogel surfaces infused with silicon oil display excellent anisotropic sliding properties using water droplets (Figure 11).83 Moreover, recently, stimulus-responsive anisotropic slippery surfaces were developed by using paraffin, a thermoresponsive phase-transition material, as a lubricating fluid and directional porous polystyrene (PS) films as the substrate.84 The smart driven anisotropic system offers unusual control of anisotropic sliding motion for several liquid droplets (Figure 12).


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Figure 11. Anisotropic sliding of water droplets on the elastomeric micro-grooved organogel surfaces. a) Water droplets can easily slide from the stretched end to the un-stretched end in one direction with a low sliding angle ca. 10, b) but cannot slide from the un-stretched end to the stretched end at the same sliding angle. Reprinted with permission from ref 83. Copyright 2014, WILEY-VCH.


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Figure 12. Temperature-responsive SLIPS produced by incorporating paraffin, a thermoresponsive phase-transition material, into an anisotropic porous polystyrene (PS) fibrous matrix. At room temperature, the paraffin solidified on the surface of PS film results in pinning the liquid droplet on the surface in the parallel (//) and perpendicular direction (⊥) to the fiber arrangements. At higher temperatures, paraffin becomes a slippery liquid, and the droplets easily slide on the composite surface in two directions. Reprinted with permission from ref 84. Copyright 2018, American Chemical Society.


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EMERGING APPLICATIONS

Liquid-infused materials are expected to show superior, special wettability properties to fulfill the fundamental and practical application requirements for self-cleaning,85,86 omniphobicity,16,54,87 separations, increasing heat transfer,88,53,89 and fluid-flow drag reduction.9094

Some successful examples are liquid repellency for a wide range of liquids, immiscible liquid

separation,95-98 solid repellency such as ice, insects, and dust, anti-bioadhesion, and droplet manipulation and collection. To meet the growing requirements in real-world applications, appropriate combinations of surface slipperiness and specific desired physicochemical functionality such as stimuli-responsivenes,99 self-healing,47,100 and optical tunability are highly desired. Table 2 summarizes some examples of liquid infused system design parameters and the field of applications.


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Table 2. Examples of liquid infused system design parameters and the field of applications; 1) Adapted with permission from ref 101. Copyright 2018, American Chemical Society. 2) Adapted with permission from ref 102. Copyright 2017, American Chemical Society. 3) Adapted with permission from ref 103. Copyright 216, WILEY-VCH. 4) Adapted with permission from ref 104. Copyright 2017, WILEY-VCH. 5) Adapted with permission from ref 105. Copyright 2015, Royal Society of Chemistry. 6) Adapted with permission from ref 106. Copyright 2013, American Chemical Society. LIS 1

Underlying Substrate Random electrospun nanoporous fiber networks made of PVDF-HFP containing SiO2 NPs

Liquid Layer Silicone oil

Application As a transparent antifouling coating for endoscope lens

2

Porous microstructure glass substrate fabricated using the hydrothermal method

Perfluoropoly ether (PFPE)

Antibiofouling surfaces for marine optical instruments

102

3

porous polymer multilayers fabricated on the inner surfaces of catheter tubes

Silicone oil

Prevent surface fouling and proliferation of common bacterial pathogens and mammalian cell line

103

4

Organogel prepared by swelling the crosslinked poly(dimethylsiloxane) (PDMS) with molten alkanes of different carbon numbers

Regenerable alkane surface layers

Easy removal of undesired foreign materials such as anti-graffiti, antifouling, and antiicing

107


Ref 101

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5

6

Poly carbonate track etched (PCTE) membrane

Wax-elastic copolymer (polystyrene– (ethylene– butylene)– polystyrene, SEBS)

Thermally-gated nanochannel as a heat-sensor

105

The 5 μm tall square silicon microposts with different interpillar spacings obtained by photolithography

Perfluorinated oil (Krytox1506)

Anti-frosting

106

Liquid Repellency/Separation

The surface topography not only contributes to anisotropic pinning/rolling properties of the LIS, but also plays a critically important role in maintaining a lubricating liquid in place. It is worth noting that the liquid-lubricated layer is the primary factor that determines the surface free energy and thus has a profound influence on liquid-repellency features of the surface. Liquid infused systems can be designed by impregnating 3D porous solids with low-surface-tension perfluorinated liquids. The homogeneous and nearly molecularly smooth surfaces not only repel pure liquids such as water, but also complex fluids such as crude oil, blood, and dairy liquids that normally stain most conventional superhydrophobic surfaces (Figure 13).16,86,108-110


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Figure 13. Superior repellency properties of SLIPS for complex fluids. a) Crude oil on a SLIPS, a superhydrophobic Teflon™ porous membrane, and a hydrophobic surface. b) Blood on a SLIPS, a superhydrophobic Teflon™ porous membrane, and a flat hydrophilic glass surface. Reprinted with permission from ref 16. Copyright 2011, Springer Nature.

Currently, there is a considerable demand for materials that can efficiently separate immiscible mixtures, especially oil/water either in the form of free mixtures or emulsions. In general, two types of special wetting materials are suitable for oil/water filtration: hydrophobic/oleophilic materials, called “oil-removing” materials that separate oil phase from oil/water mixtures by selective oil permeation, and hydrophilic/oleophobic materials known as “water-removing” materials that separate water phase from oil/water mixture by allowing water to penetrate through them while repelling oil.


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Conventional oil-removing membranes which are hydrophobic/oleophilic face limitations for separating oil/water mixtures. First, these materials can be easily fouled and clogged by oil due to their intrinsic oleophilic nature, which greatly restrict their application in filtration due to a remarkable reduction in permeation flux. Secondly, water normally has a higher density than most of oils, which tends to settle below the oil due to gravity and form a barrier layer above the materials. This water layer directly affects oil permeation by blocking all filtration. Thirdly, these materials show poor recoverability for reuse. In most cases, the adhered oil is hard to remove leading to secondary contamination in the environment. So far, only a few hydro-responsive materials have been reported based on hydrophilic and oleophobic polymeric components.111-113

Although, hydrophilic/oleophobic materials can overcome these issues, due to low surface tension of most oils, the design and fabrication of materials that simultaneously display hydrophilicity and oleophobicity is theoretically very challenging. However, fully wettable water-lubricated anisotropic membrane is an effective approach to remove only one phase from the oil/water mixture owing to extreme opposing affinities towards water and oil.114 During the separation process, the infused water layer, having no affinity for oil drops, prevents the materials from fouling by oils, while it allows the water phase to pass through. In fact, as shown previously the capillary-stabilized liquid in pore structures can form a reconfigurable doorway which selectively allow liquids to pass through the membrane. This so-called gating mechanism enables LIS to coordinate multiphase transport and suppresses fouling, in a highly selective approach without facing pore clogging problems.115,69 A superhydrophilic and underwater superoleophobic hydrogel-coated mesh showed high separation efficiency and ultralow fouling for even crude oil. Stainless steel meshes were used as the substrates and polyacrylamide (PAM)


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was selected as the hydrogel coating layer because of its excellent water-absorbing and waterholding capacities (Figure 14).116


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Figure 14. SEM images of a polyacrylamide (PAM) hydrogel-coated mesh: a) Uncoated stainless-steel mesh. b) PAM hydrogel-coated stainless-steel mesh. c) Magnification of a single pore of the PAM hydrogel-coated stainless-steel mesh. d) The nanostructured papillae on a single wire on hydrogel-coated stainless-steel mesh. e, f) Underwater superoleophobic and slippery characteristics of the as-prepared PAM hydrogel-coated mesh. g, h) Ultra-low oil-adhesion properties of the coated mesh in oil/water/solid system. i, j) Oil-water separation performance of the liquid infused stainless steel mesh; water selectively penetrates through the mesh, while crude oil remained on top. Reprinted with permission from ref 116. Copyright 2011, WILEYVCH.


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Solid Repellency

Slippery liquid incorporated surfaces have the potential to significantly reduce solid adhesion arising from ice, insects, and dust.48,117-119 The failure of an ant to hold on to SLIPS when the surface is tilted has been captured, though the ant can travel uphill on hydrophobic surfaces such as Teflon.16 In another attempt to study the slippery behavior of textured solids filled with silicon oil, the drying patterns left by coffee drops after evaporation, on a non-liquid-impregnated surface (textured or not) and on a slippery pre-impregnated material, were observed. In Figure 15, on the non-slippery surface, coffee particles distributed in a ring shape that arises from the pinning of the initial contact line whereas, on the slippery surface, and low hysteresis of these materials stop pinning of the line. Thus, the ring does not form to leave only a round chunk of coffee particles that can be easily removed. The photograph also illustrates the self-cleaning properties of LIS; specifically, a water drop moving down and cleaning the surface (previously sprinkled with silica particles) along its path.54


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Figure 15. Slippery characteristics of liquid-infused materials. a) A water droplet carries away the silica particles on a textured substrate pre-impregnated with a silicon oil. b) Patterns left by coffee drops (initial diameter of 5mm) after evaporation on a non-SLIPS (left) and on a slippery pre-infused substrate (right). Reprinted with permission from ref 54. Copyright 2011, EPLA.

Most of the desirable characteristics of anti-icing surfaces, comprising low surface energy and contact angle hysteresis, is conventionally obtained by introducing micro- or nanoscale roughness in superhydrophobic surface to reduce the actual ice-contacting area:120-125 however, their practical performance, on impinging droplets, is still largely limited under harsh


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environmental conditions, particularly high humidity. Alternatively, surfaces with a smooth and stable lubricant interfaces eliminate moisture condensation rapidly because of a reduction in the number of possible nucleation sites.126,106 Further, high mobility of droplets arising from low CAH of the lubricating film suppress frost/ice formation even under humid conditions. Additionally, the lubricant film shows high stability performance under high droplet impact pressures, whereas the voids between surface features of superhydrophobic surfaces encounter physical and mechanical defects under pressure. On this subject, extraordinarily low ice adhesion has been demonstrated using lubricant-infused systems.55,127,49,128-130

Anti-bioadhesion

The accumulation of biomolecules such as proteins and cells, marine organisms, and bacteria and diatoms on surfaces is a great challenge in a variety of applications ranging from food storage and water purification systems to biomedical devices such as artificial blood vessels, surgical and camera-guided instruments, implants and marine and industrial equipment.131-133 Although the fouling species and the type of interaction they make which varies from one kind to another add to the complexity of the problem, but one approach to develop anti-fouling surfaces, is creating a platform that limits the initial attachment of fouling organisms.134-137

During the fouling processes of a new surface, several steps take place including adsorption of species, formation of a conditioning layer, primary colonization, and finally formation of biofouling community. Fouling organisms mostly use their superficial biological molecules such


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as proteins to make the first contact with a synthetic substrate.138 One of the key strategies to combat biofoulants from attaching is making solid interfaces less available by employing of lowadhesion liquid infused surfaces onto which most organisms have low affinity to settle onto. If we look at the human body, inner and some outer surfaces are infused with liquid. For instance, eyeballs are wet with transparent defect-free tears liquid layer that shields the surface from contamination by microbes and other foreign objects. 108,139-143 Several studies explored the interaction of physiological fluids like blood, artificial saliva and urine, bovine serum albumin, and DNA solutions with liquid infused surfaces. One of the challenges of designing LIS for medical applications is biocompatibility obligations. Medically relevant oil lubricating liquid like canola, coconut, olive, almond, sesame, and medical-grade silicone oils have been used so far (Figure 16).143,144


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Figure 16. Images showing samples of complex fluids sliding down a glass slide coated with silicone oil-infused; acidic and alkaline water, unfiltered lake water, serum containing cellculture medium, glycerol, and ketchup. Table shows wetting behaviors (advancing contact angles and contact angle hysteresis) and sliding velocities of droplets of water (20 µL) on multilayers infused with silicone, canola, coconut, and olive oils (tilt angle ≈10°). Reprinted with permission from ref 144. Copyright 2015, WILEY-VCH.

Porous polytetrafluoroethylene (PTFE) substrate and microstructured fluorosilanized Si wafers have been reported to inhibit 99.6% of attachment of Pseudomonas aeruginosa over a 7-day period. Further experiments confirmed the effectiveness of LIS strategy for other clinically relevant pathogens, including Staphylococcus aureus (97.2%) and Escherichia coli (96%). These nontoxic, antibiofilm surfaces demonstrate stability under water and harsh conditions, including extreme pH, salinity, and UV exposure.52 Promising early results showed initial applications of LIS in vivo for preventing implant infection. A comprehensive review paper on liquid infused surfaces for medical applications provide a more in-depth information on the subject.143


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Moreover, marine organisms such as sharks, mussels, and crabs have natural antifouling defenses which rely on a combination of surface chemistry, physical attributes, and responses to outside stimuli. Inspired by these criteria, superior anti-biofouling slippery surfaces have been developed.37,138,145-148 Glass slides coated with lubricant infused PDMS were incubated in culture containing the green alga Botryococcus braunii. After 12 days, the attachment of the algae biofilm clearly prohibited to the treated glass was observed.149 Mussels, for example, are a living system that are the worst perpetrators of fouling. The US Navy alone spends $1BB/year on antifouling efforts to overcome their actions. A recent report found that lubricant infused surfaces prevented mussel adhesion. The work suggested that the surfaces “softness” was not favorable for mussel adhesive thread release. Although the study indicated that sprays could be formulated to achieve the lubricating effect, it remains to be seen how such materials can adhere satisfactorily to solid surfaces under various temperatures and pressures and how those factors influence biofouling.150

Microfluidic Droplet Handling

Droplet-based, microfluidic liquid-infused systems are attractive for performing chemical reactions and controlling droplet motion in reactors, collectors, and sensors on a miniaturescale.58,81,85,109,151-153 The lower surface tension, non-polarity and high viscosity of oil/organic droplets as compared to aqueous droplets make oil droplet manipulation difficult. To perform oil-droplet-based chemical reactions, underwater superoleophobic tweezers are fabricated by attaching frosted glass plates to the tips of tweezers.154 Tweezers were employed to facilitate the


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dispersion of oil droplets in water. Hydrophilic frosted glass plates trapped water molecules in the gap of their surface microstructures act as a low adhesion oil repulsive slippery layer. Employing these tweezers, oil droplets motion in water was performed as show in Figure 17. A series of miniature organic chemical reactions inside oil droplets was explored. As such, a droplet of bromine tetrachloromethane solution in a dark yellow color to come into contact with a transparent droplet of styrene tetrachloromethane. The two droplets merged into a larger one leading to a miniature chemical reaction as shown by a slow change of the color from dark yellow to transparent. Moreover, due to the ultra-low oil adhesion property of pedestals in water media, reaction products inside coalesced droplets were obtained. Miniature liquid immobilized reaction systems can thus be used for potential lab-on-a-chip applications ranging from microscale components such as biological medicines and toxic chemicals miniature reactors and sensors to high-throughput assays.153-159


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Figure 17. Demonstration of manipulating oil droplets in water to perform a miniature organic reaction. a) A bromine tetrachloromethane droplet was carefully dropped onto a superoleophobic plate, forming a dark yellow spherical shape. b,c) A styrene tetrachloromethane droplet was picked up by a pair of superoleophobic tweezers and placed onto the yellow droplet. d) Two droplets slowly combined. e,f) After 43 seconds, the color of the coalesced droplet slowly changed from dark yellow to transparent, indicating that the reaction was completed. Schematic illustrations of each steps are shown on the right of each image. Reprinted with permission from ref 154. Copyright 2011, Royal Society of Chemistry.


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Inspired by the Namib desert beetle’s back,34 which collects microdroplets of water from fog in the desert atmosphere and guides the droplets down to their mouth, Aizenberg and co-workers160 designed a surface with asymmetric bumps to optimize fast localized droplet condensation. Later, the slippery surface of pitcher plants inspired them to coat the bumps with a molecularly smooth lubricant layer to render them with higher friction. They achieved a surface with enhanced continuous water condensation and shedding performance superior to conventional superhydrophobic surfaces. Promoting dropwise condensation is critical for water-harvesting applications and many phase-change heat-transfer applications requiring reliable rapid droplet growth and transport performance.53,88,161,162

PERSPECTIVES

Recently, the domain of biomimicry of surface wetting has expanded exponentially with respect to scientific community attention as evidence by the number of papers and patents within numerous disciplines in science and engineering. The opportunity to control wetting phenomena at surfaces and interfaces has numerous commercial applications which is one of the many driving factors for work in surface biomimicry. More specifically, the constructs of superhydrophobicity and superhydrophilicity lend themselves to efforts of surface bioengineering using nature as a model to enable a diverse menu of applications including self‐cleaning surfaces, universal surface adhesability through the “Gecko Effect”, condensation of droplets, and anti-fogging amongst numerous others. Therefore, creating surfaces that are


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endowed with any of the latter properties using a vast field of fabrication techniques is of great interest.

The emergence of bio-constructs such as the “Lotus Effect” has given much food for thought with respect to how to achieve supersurface effects such as superhydrophobicity through surface roughness, for example, in addition to Cassie States that rely on air pockets to contribute to the phenomenon. Alternatively, the recent emergence of the understanding of how liquids instead of air can give rise to super surface energetics as exemplified in SLIPS, Slippery Liquid-Infused Porous Surfaces. This concept that was introduced in 2011 is based on the natural phenomenon of infusing a surface with a lubricating liquid for endowing it with super-wettable and super antiwettable properties.

Bio-inspired surfaces infused with a lubricating liquid display a remarkable range of useful properties unlike gas-cushioned surfaces that lose stability and robustness upon damage to the texture under extreme conditions. These properties originate from the ability of the continuous, fouling-resistance, defect-free, nearly molecularly smooth fluid to flow and configure itself around a variety of surfaces from rigid to elastic. Although there is no doubt about the potential of the lubricant-impregnated surfaces, several fundamental questions need to be addressed to carefully design an optimal non-wetting material. For instance, the infused liquid film may drain due to external shear flow. Although an analytical model showed that manipulating the aspect ratio of the surface grooved pattern-to-wick wetting liquids play a role in this regard,58 further investigation on optimization of more complicated topographical length scales is required.


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Moreover, to satisfy practical demand, lubricant depletion and replenishment need to be considered. The overall importance of this consideration cannot be overemphasized with respect to defining industrially relevant systems. As a successful example, a supramolecular polymer-gel matrix consisting of liquid-storage compartments in which self-regulating and self-reporting secretion materials was introduced to address these needs. It may be possible that future advances lie in materials systems that are hygroscopic and are continually replenished by native environmental humidity and evaporative cycles. Additionally, self-lubricating hydrogels/organogels are other promising candidates to provide more sustainable replenishing reservoirs.

Although complete immobilization of texture is among the most desirable features, it restricts the choice of lubricant, and thus it remains a key challenge to gain a deeper understanding of surface functionality and lubricant chemical/physical properties. For example, the role of lubricating liquid viscosity, texture, and the interactions amongst components on droplet shedding behavior is a vital question. It remains to be seen whether they slip or roll on the surface, and thus require much more investigation into their respective roles. The technology of liquid infused systems is likely to dominate the field of biomimetic and functional surfaces in practical scenarios for the foreseeable future.

Indeed, one of the chief arenas of significant interest in which they can and will continue to dominate interest is biofouling. Biofouling is a process in which living organisms secrete adhesive substances or other secretes onto a surface to create a slime or other foulant preventing


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any further exposure of the surface to the ambient conditions. Such a scenario can upset interfacial communication processes, increase drag and load, lead to surface deterioration, and within the biomedical community lead to diseases or steady diminution of function. With respect to naval systems, biofouling is a very common phenomenon. Despite the questions and challenges posed by the lubricating systems espoused in this review, their overall importance and potential to endowing surfaces with super wettability properties is undeniable. Indeed, given that they appear to be relatively economic, practical, and efficient, they portend a new paradigm for interfacial super-activity.

ACKNOWLEDGMENTS

We gratefully acknowledge the support of the Fiber and Polymer Science (FPS) program and the Nonwoven Institute (grant number 525667) at NC State University under whose umbrella ZA was able to pursue the work described and obtain her PhD as of this writing.


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