One‐Dimensional Hybrid Nanostructures for Heterogeneous Photocatalysis and Photoelectrocatalysis

Semiconductor‐based photocatalysis and photoelectrocatalysis have received considerable attention as alternative approaches for solar energy harvesting and storage. The photocatalytic or photoelectrocatalytic performance of a semiconductor is closely related to the design of the semiconductor at the nanoscale. Among various nanostructures, one‐dimensional (1D) nanostructured photocatalysts and photoelectrodes have attracted increasing interest owing to their unique optical, structural, and electronic advantages. In this article, a comprehensive review of the current research efforts towards the development of 1D semiconductor nanomaterials for heterogeneous photocatalysis and photoelectrocatalysis is provided and, in particular, a discussion of how to overcome the challenges for achieving full potential of 1D nanostructures is presented. It is anticipated that this review will afford enriched information on the rational exploration of the structural and electronic properties of 1D semiconductor nanostructures for achieving more efficient 1D nanostructure‐based photocatalysts and photoelectrodes for high‐efficiency solar energy conversion.     

Multifunctional Cellular Materials Based on 2D Nanomaterials: Prospects and Challenges

Recent advances in emerging 2D nanomaterial‐based cellular materials (2D‐CMs) open up new opportunities for the development of next generation cellular solids with exceptional properties. Herein, an overview of the current research status of 2D‐CMs is provided and their future opportunities are highlighted. First, the unique features of 2D nanomaterials are introduced to illustrate why these nanoscale building blocks are promising for the development of novel cellular materials and what the new features of 2D nanoscale building blocks can offer when compared to their 0D and 1D counterparts. An in‐depth discussion on the structure–property relationships of 2D‐CMs is then provided, and the remarkable functions that can be achieved by engineering their cellular architecture are highlighted. Additionally, the use of 2D‐CMs to tackle key challenges in different practical applications is demonstrated. In conclusion, a personal perspective on the challenges and future research directions of 2D‐CMs is given.     

A High‐Performance Lithium‐Ion Capacitor Based on 2D Nanosheet Materials

Lithium‐ion capacitors (LICs) are promising electrical energy storage systems for mid‐to‐large‐scale applications due to the high energy and large power output without sacrificing long cycle stability. However, due to the different energy storage mechanisms between anode and cathode, the energy densities of LICs often degrade noticeably at high power density, because of the sluggish kinetics limitation at the battery‐type anode side. Herein, a high‐performance LIC by well‐defined ZnMn₂O₄‐graphene hybrid nanosheets anode and N‐doped carbon nanosheets cathode is presented. The 2D nanomaterials offer high specific surface areas in favor of a fast ion transport and storage with shortened ion diffusion length, enabling fast charge and discharge. The fabricated LIC delivers a high specific energy of 202.8 Wh kg^?1 at specific power of 180 W kg^?1, and the specific energy remains 98 Wh kg^?1 even when the specific power achieves as high as 21 kW kg^?1.     

25th Anniversary Article: Hybrid Nanostructures Based on Two‐Dimensional Nanomaterials

Two‐dimensional (2D) nanomaterials, such as graphene and transition metal dichalcogenides (TMDs), receive a lot of attention, because of their intriguing properties and wide applications in catalysis, energy‐storage devices, electronics, optoelectronics, and so on. To further enhance the performance of their application, these 2D nanomaterials are hybridized with other functional nanostructures. In this review, the latest studies of 2D nanomaterial‐based hybrid nanostructures are discussed, focusing on their preparation methods, properties, and applications.     

2D V‐V Binary Materials: Status and Challenges

2D phosphorene, arsenene, antimonene, and bismuthene, as a fast‐growing family of 2D monoelemental materials, have attracted enormous interest in the scientific community owing to their intriguing structures and extraordinary electronic properties. Tuning the monoelemental crystals into bielemental ones between group‐VA elements is able to preserve their advantages of unique structures, modulate their properties, and further expand their multifunctional applications. Herein, a review of the historical work is provided for both theoretical predictions and experimental advances of 2D V‐V binary materials. Their various intriguing electronic properties are discussed, including band structure, carrier mobility, Rashba effect, and topological state. An emphasis is also given to their progress in fabricated approaches and potential applications. Finally, a detailed presentation on the opportunities and challenges in the future development of 2D V‐V binary materials is given.     

3D Direct Laser Writing of Nano‐ and Microstructured Hierarchical Gecko‐Mimicking Surfaces

Applying 3D direct laser writing, artificial hierarchical gecko‐type structures are designed and fabricated down to nanometer dimensions. In this way, the elastic modulus and the length scale of the gecko's setae are very closely matched. Direct laser writing is a very flexible rapid prototyping method allowing the fabrication of arbitrary nanostructures. Since the parameters of the structures can be easily changed, this technique is perfect for design studies of dry adhesives. Measuring the adhesional forces by atomic force microscopy, the influence of several design parameters like density, aspect ratio, and tip‐shape on dry adhesion performance are systematically examined. In this way, it is revealed that hierarchy is favorable for artificial gecko‐inspired dry adhesives made of stiff materials on the nanometer scale.     

Fractal‐Theory‐Based Control of the Shape and Quality of CVD‐Grown 2D Materials

The precise control of the shape and quality of 2D materials during chemical vapor deposition (CVD) processes remains a challenging task, due to a lack of understanding of their underlying growth mechanisms. The existence of a fractal‐growth‐based mechanism in the CVD synthesis of several 2D materials is revealed, to which a modified traditional fractal theory is applied in order to build a 2D diffusion‐limited aggregation (2D‐DLA) model based on an atomic‐scale growth mechanism. The strength of this model is validated by the perfect correlation between theoretically simulated data, predicted by 2D‐DLA, and experimental results obtained from the CVD synthesis of graphene, hexagonal boron nitride, and transition metal dichalcogenides. By applying the 2D‐DLA model, it is also discovered that the single‐domain net growth rate (SD‐NGR) plays a crucial factor in governing the shape and quality of 2D‐material crystals. By carefully tuning SD‐NGR, various fractal‐morphology high‐quality single‐crystal 2D materials are synthesized, achieving, for the first time, the precise control of 2D‐material CVD growth. This work lays the theoretical foundation for the precise adjustment of the morphologies and physical properties of 2D materials, which is essential to the use of fractal‐shaped nanomaterials for the fabrication of new‐generation neural‐network nanodevices.     

Wafer‐Scale Fabrication of High‐Performance n‐Type Polymer Monolayer Transistors Using a Multi‐Level Self‐Assembly Strategy

Wafer‐scale fabrication of high‐performance uniform organic electronic materials is of great challenge and has rarely been realized before. Previous large‐scale fabrication methods always lead to different layer thickness and thereby poor film and device uniformity. Herein, the first demonstration of 4 in. wafer‐scale, uniform, and high‐performance n‐type polymer monolayer films is reported, enabled by controlling the multi‐level self‐assembly process of conjugated polymers in solution. Since the self‐assembly process happened in solution, the uniform 2D polymer monolayers can be facilely deposited on various substrates, and theoretically without size limitations. Polymer monolayer transistors exhibit high electron mobilities of up to 1.88 cm² V^?1 s^?1, which is among the highest in n‐type monolayer organic transistors. This method allows to easily fabricate n‐type conjugated polymers with wafer‐scale, high uniformity, low contact resistance, and excellent transistor performance (better than the traditional spin‐coating method). This work provides an effective strategy to prepare large‐scale and uniform 2D polymer monolayers, which could enable the application of conjugated polymers for wafer‐scale sophisticated electronics.     

Self‐Assembled Hybrid Materials Based on Organic Nanocrystals and Carbon Nanotubes

Organic crystalline materials are used as dyes/pigments, pharmaceuticals, and active components of photonic and electronic devices. There is great interest in integrating organic crystals with inorganic and carbon nanomaterials to create nanocomposites with enhanced properties. Such efforts are hampered by the difficulties in interfacing organic crystals with dissimilar materials. Here, an approach that employs organic nanocrystallization is presented to fabricate solution‐processed organic nanocrystal/carbon nanotube (ONC/CNT) hybrid materials based on readily available organic dyes (perylene diimides (PDIs)) and carbon nanotubes. The hybrids are prepared by self‐assembly in aqueous media to afford free‐standing films with tunable CNT content. These exhibit excellent conductivities (as high as 5.78 ± 0.56 S m^?1), and high thermal stability that are superior to common polymer/CNT hybrids. The color of the hybrids can be tuned by adding various PDI derivatives. ONC/CNT hybrids represent a novel class of nanocomposites, applicable as optoelectronic and conductive colorant materials.