Superaerophilic/Superaerophobic NiFe-LDHs Electrode for Enhancing Overall Water Splitting in Alkaline Media.

Overall water splitting, as a critical approach to producing green hydrogen, is greatly impeded by the mass transfer of gaseous bubbles and dissolved gas molecules. Herein, a bifunctional superaerophilic/superaerophobic (SAL/SAB) NiFe layered-double-hydroxides (LDHs) electrode has been developed, which can drive H2 and O2 bubbles out of the reaction system by asymmetric Laplace pressure and accelerate dissolved gases diffusion through reducing their diffusion distance. Consequently, the SAL/SAB NiFe-LDHs electrode exhibits excellent HER activity with an overpotential of -76 mV at -10 mA cm-2 and outstanding oxygen evolution reaction activity with an overpotential of 253 mV at 100 mA cm-2. The bifunctional SAL/SAB NiFe-LDHs electrode is further utilized in overall water splitting, which can achieve 10 mA cm-2 with a cell voltage of 1.54 V. This work provides an efficient strategy to improve the efficiency of overall water splitting and can stimulate new electrode design in various gas-involved processes.

Unidirectional Moisture Delivery via a Janus Photothermal Interface for Indoor Dehumidification: A Smart Roof.

Rational control of the humidity in specific environments plays an important role in green building, equipment protection, etc. A smart apparatus that can actively expel inner moisture and largely prevent outer liquid penetration can be highly desirable. Through the integration of the Janus interface with unidirectional liquid manipulation and the solar evaporating layer, here, a Janus solar dehumidifying interface (JSDI) is designed for the switchable moisture management of an indoor environment. By covering with the JSDI roof, the continuous elimination of inner water is achieved via outward condensate delivery and solar evaporation on sunny days. On rainy days, JSDI with a hydrophobic lower surface can largely hamper inward liquid leakage and then spontaneously drain the accumulated water via a siphoning structure. The real-world water evaporation rate via the JSDI is ≈0.38 kg m-2 h-1 on an autumn day, showing a promising function of in situ moisture expelling. In addition, the JSDI is made of natural materials that are easy to scale up with a cost of four dollars per square meter. It is envisioned that the JSDI may meet the wide requirements of indoor dehumidification and update the understanding of the integration of Janus interfaces and solar steam generation.

Bioinspired Underwater Superoleophilic Two-Dimensional Surface with Asymmetric Oleophobic Barriers for Unidirectional and Long-Distance Oil Transport.

Unidirectional and long-distance liquid transport is critically important to a range of practical applications, e.g., water harvesting, microfluidics, and chemical reactions. Great efforts have been made on liquid manipulation; most of which, however, are limited in the air environment. It is still a great challenge to achieve unidirectional and long-distance oil transport in an aqueous environment. Herein, we have successfully fabricated an underwater superoleophilic two-dimensional surface (USTS) with asymmetric oleophobic barriers to arbitrarily manipulate oil in aqueous medium. The behavior of oil on USTS was carefully investigated, of which the unidirectional spreading capability was originated from the anisotropic spreading resistance resulted from the asymmetric oleophobic barriers. Accordingly, an underwater oil/water separation device has been developed, which can achieve continuous and efficient oil/water separation and further prevent the secondary pollution caused by oil volatilization.

Light-Powered Ion Pumping in a Cation-Selective Conducting Polymer Membrane.

The simulation of the ion pumping against a proton gradient energized by light in photosynthesis is of significant importance for the energy conversion in a non-biological environment. Herein, we report light-powered ion pumping in a polystyrene sulfonate anion (PSS) doped polypyrrole (PPy) conducting polymer membrane (PSS-PPy) with a symmetric geometry. This PSS-PPy conducting polymer membrane exhibits a cationic selectivity and a light-responsive surface-charge-governed ion transport attributed to the negatively charged PSS groups. An asymmetric visible irradiation on one side of the PSS-PPy membrane induces a built-in electric field across the membrane due to the intrinsic photoelectronic property of PPy, which drives the cationic transport against the concentration gradient, demonstrating an ion-pumping effect. This work is a prototype that uses a geometry-symmetric conducting polymer membrane as a light-powered artificial ion pump for active ion transport, which exhibits potential applications in nanofluidic energy conversion.

Liquid-Assisted Single-Layer Janus Membrane for Efficient Unidirectional Liquid Penetration.

Unidirectional liquid penetration plays an important role in many fields, such as microfluidic devices, biological medical, liquid printing, and oil/water separation. Although there are some progresses in the liquid unidirectional penetration using a variety of Janus membranes with anisotropic wettability, it still remains a great difficulty for single-layer Janus membranes with straight pore to balance spontaneous liquid penetration in positive direction and superior liquid resistance in the reverse direction. Herein, a liquid-assisted strategy for single-layer Janus membrane is developed, which can efficiently decrease the critical breakthrough pressure from superhydrophobic side to hydrophilic side and show little influence on that in the reverse direction. Consequently, unidirectional water penetration with high hydraulic pressure difference can be achieved. The Laplace pressure change along the thickness of the single-layer Janus membranes is further discussed, and the mechanism by which the auxiliary liquid decreases the critical breakthrough pressure is revealed. Furthermore, this Janus membrane with unidirectional water penetration "diode" performance can be used to prevent liquid backflow in intravenous transfusion. It is believed that this work can open an avenue for people to design single-layer Janus membrane with high pressure difference and find wide applications in unidirectional liquid transport.

Molecular-Structure-Induced Under-Liquid Dual Superlyophobic Surfaces.

Surfaces with under-water superoleophobicity or under-oil superhydrophobicity have attractive features due to their widespread applications. However, it is difficult to achieve under-liquid dual superlyophobic surfaces, that is, under-oil superhydrophobicity and under-water superoleophobicity coexistence, due to the thermodynamic contradiction. Herein, we report an approach to obtain the under-liquid dual superlyophobic surface through conformational transitions of surface self-assembled molecules. Preferential exposure of either hydrophobic or hydrophilic moieties of the hydroxythiol (HS(CH2)nOH, where n is the number of methylene groups) self-assembled monolayers to the surrounding solvent (water or oil) can be used to manipulate macroscopic wettability. In water, the surfaces modified with different hydroxythiols exhibit under-water superoleophobicity because of the exposure of hydroxyl groups. In contrast, surface wettability to water is affected by molecular orientation in oil, and the surface transits from under-oil superhydrophilicity to superhydrophobicity when n ≥ 4. This surface design can amplify the molecular-level conformational transition to the change of macroscopic surface wettability. Furthermore, on-demand oil/water separation relying on the under-liquid dual superlyophobicity is successfully demonstrated. This work may be useful in developing the materials with opposite superwettability.

Fabrication of Elastic Macroporous Polymers with Enhanced Oil Absorbability and Antiwaxing Performance.

Porous polymers are of great interest in potential energy storage and environmental remediation applications. However, traditional fabrication methods are either time-consuming or energy-consuming and deteriorate the mechanical strength of polymer materials. In this study, polymerization-induced phase separation was used to realize the template-free fabrication of superflexible macroporous polymers. Since the solvent is also used as a porogen, this method can be widely used to synthesize several porous polymers by carefully choosing the solvent and monomer. Compared to nonstructured polymers, the prepared macroporous polymers exhibited enhanced mechanical strength, superflexibility, multicompressibility, and bending properties. Along with hydrophobicity/oleophilicity and macroporous structures, the as-prepared porous polymers demonstrated controllable oil absorbability and release; furthermore, after infusing with lubrication liquid, these materials can be used as antiwaxing materials. The elastic porous polymers prepared using this simple and universal method show great potential for various applications, including controlled drug release, antiwaxing, and lubrication.

Multifunctional Magnetocontrollable Superwettable-Microcilia Surface for Directional Droplet Manipulation.

In nature, fluid manipulations are ubiquitous in organisms, and they are crucial for many of their vital activities. Therefore, this process has also attracted widescale research attention. However, despite significant advances in fluid transportation research over the past few decades, it is still hugely challenging to achieve efficient and nondestructive droplet transportation owing to contamination effects and controllability problems in liquid transportation applications. To this end, inspired by the motile microcilia of micro-organisms, the superhydrophobicity of lotus leaves, the underwater superoleophobicity of filefish skin, and pigeons' migration behavior, a novel manipulation strategy is developed for droplets motion. Specifically, herein, a superwettable magnetic microcilia array surface with a structure that is switchable by an external magnetic field is constructed for droplet manipulation. It is found that under external magnetic fields, the superhydrophobic magnetic microcilia array surface can continuously and directionally manipulate the water droplets in air and that the underwater superoleophobic magnetic microcilia array surface can control the oil droplets underwater. This work demonstrates that the nondestructive droplet transportation mechanism can be used for liquid transportation, droplet reactions, and micropipeline transmission, thus opening up an avenue for practical applications of droplet manipulation using intelligent microstructure surfaces.

Diffusion-Freezing-Induced Microphase Separation for Constructing Large-Area Multiscale Structures on Hydrogel Surfaces.

Hydrogels with multiscale structured surface have attracted significant attention for their valuable applications in diverse areas. However, current strategies for the design and fabrication of structured hydrogel surfaces, which suffer from complicated manufacturing processes and specific material modeling, are not efficient to produce structured hydrogel surfaces in large area, and therefore restrict their practical applications. To address this problem, a general and reliable method is reported, which relies on the interplay between polymer chain diffusion and the subsequent freezing-induced gelation and microphase separation processes. The basic idea is systematically analyzed and further exploited to manufacture gel surfaces with gradient structures and patterns through the introduction of temperature gradient and shape control of the contact area. Moreover, the formed micro/nanostructured surfaces are exemplified to work as capillary systems and thus can uplift the liquid spontaneously indicating the potential application for anti-dehydration. It is believed that the proposed facile and large-area fabrication method can inspire the design of materials with various functionalized surfaces.

An Integrated Janus Mesh: Underwater Bubble Antibuoyancy Unidirectional Penetration.

Gas bubbles are a powerful tool with applications in particle visualization, spacers, actuation pistons, and pressure sensors. Controlling the transportation of bubbles in the liquid phase is a challenge that needs to be solved in many industrial processes, such as in the pipe transportation of fluids, the corrosion of ocean vessels, and the control of foaming processes. There are few existing materials capable of the antibuoyancy unidirectional transportation of bubbles. Here, a Janus superwetting mesh is fabricated by integrating aerophilic (AL) and superaerophobic (SAB) surfaces. The resulting composite mesh achieves underwater bubble antibuoyancy unidirectional penetration. In aqueous solution, bubbles pass through the mesh from the SAB side to the AL side, but are blocked from passing through in the opposite direction. This Janus mesh can be considered to be a bubble diode, so is convenient for use in underwater bubble unidirectional transportation. This work may promote the development of advanced materials for gas bubble directional transportation and separation in aqueous media.

Friction of Droplets Sliding on Microstructured Superhydrophobic Surfaces.

Liquid transport is a fundamental process relevant to a wide range of applications, for example, heat transfer, anti-icing, self-cleaning, drag reduction, and microfluidic systems. For these applications, a deeper understanding of the sliding behavior of water droplets on solid surfaces is of particular importance. In this study, the frictional behavior of water droplets sliding on superhydrophobic surfaces decorated with micropillar arrays was studied using a nanotribometer. Our experiments show that surfaces with a higher solid area fraction generally exhibited larger friction, although friction might drop when the solid area fraction was close to unity. More interestingly, we found that the sliding friction of droplets was enhanced when the dimension of the microstructures increased, showing a distinct size effect. The nonmonotonic dependence of friction force on solid area fraction and the apparent size effect can be qualitatively explained by the evolution of two governing factors, that is, the true length of the contact line and the coordination degree of the depinning events. The mechanisms are expected to be generally applicable for other liquid transport processes involving the dynamic motion of a three-phase contact line, which may provide a new means of tuning liquid-transfer behavior through surface microstructures.

Direct Imaging of Superwetting Behavior on Solid-Liquid-Vapor Triphase Interfaces.

A solid-liquid-vapor interface dominated by a three-phase contact line usually serves as an active area for interfacial reactions and provides a vital clue to surface behavior. Recently, direct imaging of the triphase interface of superwetting interfaces on the microscale/nanoscale has attracted broad scientific attention for both theoretical research and practical applications, and has gradually become an efficient and intuitive approach to explore the wetting behaviors of various multiphase interfaces. Here, recent progress on characterizing the solid-liquid-vapor triphase interface on the microscale/nanoscale with diverse types of imaging apparatus is summarized. Moreover, the accurate, visible, and quantitative information that can be obtained shows the real interfacial morphology of the wetting behaviors of multiphase interfaces. On the basis of fundamental research, technical innovations in imaging and complicated multiphase interfaces of the superwetting surface are also briefly presented.

Desert Beetle-Inspired Superwettable Patterned Surfaces for Water Harvesting.

With the impacts of climate change and impending crisis of clean drinking water, designing functional materials for water harvesting from fog with large water capacity has received much attention in recent years. Nature has evolved different strategies for surviving dry, arid, and xeric conditions. Nature is a school for human beings. In this contribution, inspired by the Stenocara beetle, superhydrophilic/superhydrophobic patterned surfaces are fabricated on the silica poly(dimethylsiloxane) (PDMS)-coated superhydrophobic surfaces using a pulsed laser deposition approach with masks. The resultant samples with patterned wettability demonstrate water-harvesting efficiency in comparison with the silica PDMS-coated superhydrophobic surface and the Pt nanoparticles-coated superhydrophilic surface. The maximum water-harvesting efficiency can reach about 5.3 g cm-2 h-1 . Both the size and the percentage of the Pt-coated superhydrophilic square regions on the patterned surface affect the condensation and coalescence of the water droplet, as well as the final water-harvesting efficiency. The present water-harvesting strategy should provide an avenue to alleviate the water crisis facing mankind in certain arid regions of the world.

Unidirectional Wetting Properties on Multi-Bioinspired Magnetocontrollable Slippery Microcilia.

Here, a smart fluid-controlled surface is designed, via the rational integration of the unique properties of three natural examples, i.e., the unidirectional wetting behaviors of butterfly's wing, liquid-infused "slippery" surface of the pitcher plant, and the motile microcilia of micro-organisms. Anisotropic wettability, lubricated surfaces, and magnetoresponsive microstructures are assembled into one unified system. The as-prepared surface covered by tilted microcilia achieves significant unidirectional droplet adhesion and sliding. Regulating by external magnet field, the directionality of ferromagnetic microcilia can be synergistically switched, which facilitates a continuous and omnidirectional-controllable water delivery. This work opens an avenue for applications of anisotropic wetting surfaces, such as complex-flow distribution and liquid delivery, and extend the design approach of multi-bioinspiration integration.

Direct insight into the three-dimensional internal morphology of solid-liquid-vapor interfaces at microscale.

Solid-liquid-vapor interfaces dominated by the three-phase contact line, usually performing as the active center in reactions, are important in biological and industrial processes. In this contribution, we provide direct three-dimensional (3D) experimental evidence for the inside morphology of interfaces with either Cassie or Wenzel states at micron level using X-ray micro-computed tomography, which allows us to accurately "see inside" the morphological structures and quantitatively visualize their internal 3D fine structures and phases in intact samples. Furthermore, the in-depth measurements revealed that the liquid randomly and partly located on the top of protrusions on the natural and artificial superhydrophobic surfaces in Cassie regime, resulting from thermodynamically optimal minimization of the surface energy. These new findings are useful for the optimization of classical wetting theories and models, which should promote the surface scientific and technological developments.

Fly-eye inspired superhydrophobic anti-fogging inorganic nanostructures.

Fly-eye bio-inspired inorganic nanostructures are synthesized via a two-step self-assembly approach, which have low contact angle hysteresis and excellent anti-fogging properties, and are promising candidates for anti-freezing/fogging materials to be applied in extreme and hazardous environments.

Peanut leaf inspired multifunctional surfaces.

Nature has long served as a source of inspiration for scientists and engineers to design and construct multifunctional artificial materials. The lotus and the peanut are two typical plants living in the aquatic and the arid (or semiarid) habitats, respectively, which have evolved different optimized solutions to survive. For the lotus leaf, an air layer is formed between its surface and water, exhibiting a discontinuous three-phase contact line, which resulted in the low adhesive superhydrophobic self-cleaning effect to avoid the leaf decomposition. In contrast to the lotus leaf, the peanut leaf shows high-adhesive superhydrophobicity, arising from the formation of the quasi-continuous and discontinuous three-phase contact line at the microscale and nanoscale, respectively, which provides a new avenue for the fabrication of high adhesive superhydrophobic materials. Further, this high adhesive and superhydrophobic peanut leaf is proved to be efficient in fog capture. Inspired by the peanut leaf, multifunctional surfaces with structural similarity to the natural peanut leaf are prepared, exhibiting simultaneous superhydrophobicity and high adhesion towards water.

Superhydrophobicity-mediated electrochemical reaction along the solid-liquid-gas triphase interface: edge-growth of gold architectures.

A superhydrophobic pillar-structured electrode leads to uncommon electrochemical behavior. The anti-wetting reaction surface restricts the contact between electrolyte and electrode to the pillar tops, as a result of trapped air pockets in the gaps between pillars. The electrochemical reaction occurs mainly at the solid/liquid/gas triphase interface, instead of the traditional solid/liquid diphase surface, yielding unique edge-growth structures - for example gold microflowers - on the top of each pillar.