Hierarchical Structured Multifunctional Self‐Cleaning Material with Durable Superhydrophobicity and Photocatalytic Functionalities

Self‐cleaning materials, which are inspired and derived from natural phenomena, have gained significant scientific and commercial interest in the past decades as they are energy‐ and labor‐saving and environmentally friendly. Several technologies are developed to obtain self‐cleaning materials. The combination of superhydrophobic and photocatalytic properties enables the efficient removal of solid particles and organic contaminations, which could reduce or damage the superhydrophobicity. However, the fragility of the nanoscale roughness of the superhydrophobic surface limits its practical application. Here, a hierarchical structure approach combining micro‐ and nanoscale architectures is created to protect the nanoscale surface roughness from mechanical damage. Glass beads of 75 µm are partially embedded into a low‐density polyethylene film. This composite surface is coated with silicone nanofilaments (SNFs) via the droplet‐assisted growth and shaping approach, providing the nanoscale surface roughness as well as the support for the photocatalyst with enlarged surface area. TiO₂ nanoparticles, which serve as the photocatalyst, are synthesized in situ on SNFs through a hydrothermal reaction. The self‐cleaning effect is proved using wettability measurements for various liquids, degradation of organic contamination under UV light, and antibacterial tests. The enhanced mechanical durability of the hierarchical structure of the composite material is verified with an abrasion test.     

Earthworm‐Inspired Rough Polymer Coatings with Self‐Replenishing Lubrication for Adaptive Friction‐Reduction and Antifouling Surfaces

Earthworms are able to pass through sticky soil without inducing stains through a self‐forming thick lubricating layer on their rough skins. To mimic this earthworm‐like lubricating capability, an attempt to create a textured structure on the surface of liquid‐releasable polymer coatings by a “breath figure” process is described herein. The resulting coatings exhibit fast and site‐specific release behavior under external triggers such as solid‐based friction. The released oil is then stabilized by the surface texture to form thick lubricating layers, reducing friction and enhancing wear resistance. Moreover, the coatings also exhibit excellent antifouling property in a sticky soil environment. Because the lubricating layer can be regenerated after consumption, the potential of this self‐replenished lubricating mechanism in preparing friction‐reduction, antiwear, and antifouling coatings used in solid‐based environments is therefore envisioned.     

Secondary‐Component Incorporated Hollow MOFs and Derivatives for Catalytic and Energy‐Related Applications

Their highly functional nature has endowed metal–organic frameworks (MOFs) with diverse applications. On this basis, a higher demand has been proposed for the preparation of novel‐structured MOFs. Hollow MOFs have been intensively studied and exhibited versatile properties, and among the various methods, secondary‐component incorporation has been proved promising in the design and preparation of complex structures with requisite properties. Herein, the synthesis and applications of secondary component incorporated MOFs and their derivatives are systematically reviewed. Two main methodologies, preincorporation and postmodification, are discussed in detail, and the role of the secondary component is demonstrated. Based on these introductions, the applications of those materials, including chemical catalysis, electrocatalysis, and energy storage applications, are summarized. Finally, a personal outlook for the future opportunities and challenges in this field is given.     

Multifunctional Inverted Nanocone Arrays for Non‐Wetting,Self‐Cleaning Transparent Surface with High Mechanical Robustness

A multifunctional surface that enables control of wetting, optical reflectivity and mechanical damage of nanostructured interfaces is presented. Our approach is based on imprinting a periodic array of nanosized cones into a UV‐curable polyurethane acrylate (PUA), resulting in a self‐reinforcing egg‐crate topography evenly distributed over large areas up to several cm² in size. The resulting surfaces can be either superhydrophilic or superhydrophobic (through subsequent application of an appropriate chemical coating), they minimize optical reflection losses over a broad range of wavelengths and a wide range of angles of incidence, and they also have enhanced mechanical resilience due to greatly improved redistribution of the normal and shearing mechanical loads. The transmissivity and wetting characteristics of the nanoscale egg‐crate structure, as well as its resistance to mechanical deformation are analyzed theoretically. Experiments show that the optical performance together with self‐cleaning or anti‐fogging behavior of the inverted nanocone topography is comparable to earlier designs that have used periodic arrays of nanocones to control reflection and wetting. However the egg‐crate structures are far superior in terms of mechanical robustness, and the ability to replicate this topography through several generations is promising for large‐scale commercial applications where multifunctionality is important.     

Toward Wearable Self‐Charging Power Systems: The Integration of Energy‐Harvesting and Storage Devices

One major challenge for wearable electronics is that the state‐of‐the‐art batteries are inadequate to provide sufficient energy for long‐term operations, leading to inconvenient battery replacement or frequent recharging. Other than the pursuit of high energy density of secondary batteries, an alternative approach recently drawing intensive attention from the research community, is to integrate energy‐generation and energy‐storage devices into self‐charging power systems (SCPSs), so that the scavenged energy can be simultaneously stored for sustainable power supply. This paper reviews recent developments in SCPSs with the integration of various energy‐harvesting devices (including piezoelectric nanogenerators, triboelectric nanogenerators, solar cells, and thermoelectric nanogenerators) and energy‐storage devices, such as batteries and supercapacitors. SCPSs with multiple energy‐harvesting devices are also included. Emphasis is placed on integrated flexible or wearable SCPSs. Remaining challenges and perspectives are also examined to suggest how to bring the appealing SCPSs into practical applications in the near future.     

Underwater Self‐Cleaning PEDOT‐PSS Hydrogel Mesh for Effective Separation of Corrosive and Hot Oil/Water Mixtures

Oil‐polluted water is a worldwide problem due to the increasing industry oily wastewater and the frequent oil‐spill pollution. Here, PEDOT‐PSS hydrogel meshes are successfully prepared by using in‐situ chemical polymerization on Ti mesh substrate, which are composed of hierarchical porous structures and present superhydrophilicity in air and superoleophobicity underwater. And PEDOT‐PSS hydrogel meshes exhibit excellent environmental stability under a series of harsh conditions, which are used for the separation of the mixtures of oil and various corrosive and active aqueous solutions, including strong acidic, alkaline, or salt aqueous solutions, even hot‐water. The hydrogel meshes offer high separation efficiency of up to 99.9%. Importantly, the mesh still reveals 99.5% separation efficiency even after 50 times separation operation, demonstrating its excellent durability that shows attractive potential for practical oil‐water separation in industry and everyday life.     

Hierarchical TiO2/SnO2 Hollow Spheres Coated with Graphitized Carbon for High‐Performance Electrochemical Li‐Ion Storage

A self‐templated strategy is developed to fabricate hierarchical TiO₂/SnO₂ hollow spheres coated with graphitized carbon (HTSO/GC‐HSs) by combined sol–gel processes with hydrothermal treatment and calcination. The as‐prepared mesoporous HTSO/GC‐HSs present an approximate yolk‐double–shell structure, with high specific area and small nanocrystals of TiO₂ and SnO₂, and thus exhibit superior electrochemical reactivity and stability when used as anode materials for Li‐ion batteries. A high reversible specific capacity of about 310 mAh g^?1 at a high current density of 5 A g^?1 can be achieved over 500 cycles indicating very good cycle stability and rate performance.     

Self‐Correction Strategy for Precise,Massive, and Parallel Macroscopic Supramolecular Assembly

Macroscopic supramolecular assembly (MSA) represents a new advancement in supramolecular chemistry involving building blocks with sizes beyond tens of micrometers associating through noncovalent interactions. MSA is established as a unique method to fabricate supramolecularly assembled materials by shortening the length scale between bulk materials and building blocks. However, improving the precise alignment during assembly to form orderly assembled structures remains a challenge. Although the pretreatment of building blocks can ameliorate order to a certain degree, defects or mismatching still exists, which limits the practical applications of MSA. Therefore, an iterative poststrategy is proposed, where self‐correction based on dynamic assembly/disassembly is applied to achieve precise, massive, and parallel assembly. The self‐correction process consists of two key steps: the identification of poorly ordered structures and the selective correction of these structures. This study develops a diffusion‐kinetics‐dependent disassembly to well identify the poorly aligned structures and correct these structures through iterations of disassembly/reassembly in a programmed fashion. Finally, a massive and parallel assembly of 100 precise dimers over eight iteration cycles is achieved, thus providing a powerful solution to the problem of processing insensitivity to errors in self‐assembly‐related methods.     

Hollow Carbon Nanospheres with Tunable Hierarchical Pores for Drug,Gene, and Photothermal Synergistic Treatment

Design and synthesis of porous and hollow carbon spheres have attracted considerable interest in the past decade due to their superior physicochemical properties and widespread applications. However, it is still a big challenge to achieve controllable synthesis of hollow carbon nanospheres with center‐radial large mesopores in the shells and inner surface roughness. Herein, porous hollow carbon nanospheres (PHCNs) are successfully synthesized with tunable center‐radial mesopore channels in the shells and crater‐like inner surfaces by employing dendrimer‐like mesoporous silica nanospheres (DMSNs) as hard templates. Compared with conventional mesoporous nanospheres, DMSN templates not only result in the formation of center‐radial large mesopores in the shells, but also produce a crater‐like inner surface. PHCNs can be tuned from open center‐radial mesoporous shells to relatively closed microporous shells. After functionalization with polyethyleneimine (PEI) and poly(ethylene glycol) (PEG), PHCNs not only have negligible cytotoxicity, excellent photothermal property, and high coloading capacity of 482 µg of doxorubicin and 44 µg of siRNA per mg, but can also efficiently deliver these substances into cells, thus displaying enhanced cancer cell killing capacity by triple‐combination therapy.