State Key Laboratory of Advanced Technology For Materials Synthesis and Processing

Photocatalytic water splitting represents a promising strategy for clean, low-cost, and environmental-friendly production of H2 by utilizing solar energy. There are three crucial steps for the photocatalytic water splitting reaction: solar light harvesting, charge separation and transportation, and the catalytic H2 and O2 evolution reactions. While significant achievement has been made in optimizing the first two steps in the photocatalytic process, much less efforts have been put into improving the efficiency of the third step, which demands the utilization of cocatalysts. To date, cocatalysts based on rare and expensive noble metals are still required for achieving reasonable activity in most semiconductor-based photocatalytic systems, which seriously restricts their large-scale application. Therefore, seeking cheap, earth-abundant and high-performance cocatalysts is indispensable to achieve cost-effective and highly efficient photocatalytic water splitting. This review for the first time summarizes all the developed earth-abundant cocatalysts for photocatalytic H2- and O2-production half reactions as well as overall water splitting. The roles and functional mechanism of the cocatalysts are discussed in detail. Finally, this review is concluded with a summary, and remarks on some challenges and perspectives in this emerging area of research.

Recent progress and strategies toward solar water splitting over heterogeneous semiconductors are reviewed and the challenges and future perspectives are suggested.

As a green and sustainable technology, semiconductor-based heterogeneous photocatalysis has received much attention in the last few decades because it has potential to solve both energy and environmental problems. To achieve efficient photocatalysts, various hierarchical semiconductors have been designed and fabricated at the micro/nanometer scale in recent years. This review presents a critical appraisal of fabrication methods, growth mechanisms and applications of advanced hierarchical photocatalysts. Especially, the different synthesis strategies such as two-step templating, in situ template-sacrificial dissolution, self-templating method, in situ template-free assembly, chemically induced self-transformation and post-synthesis treatment are highlighted. Finally, some important applications including photocatalytic degradation of pollutants, photocatalytic H2 production and photocatalytic CO2 reduction are reviewed. A thorough assessment of the progress made in photocatalysis may open new opportunities in designing highly effective hierarchical photocatalysts for advanced applications ranging from thermal catalysis, separation and purification processes to solar cells.

Over the last decade, significant effort has been devoted to the applications of hierarchically structured porous materials owing to their outstanding properties such as high surface area, excellent accessibility to active sites, and enhanced mass transport and diffusion. The hierarchy of porosity, structural, morphological and component levels in these materials is key for their high performance in all kinds of applications. The introduction of hierarchical porosity into materials has led to a significant improvement in the performance of materials. Herein, recent progress in the applications of hierarchically structured porous materials from energy conversion and storage, catalysis, photocatalysis, adsorption, separation, and sensing to biomedicine is reviewed. Their potential future applications are also highlighted. We particularly dwell on the relationship between hierarchically porous structures and properties, with examples of each type of hierarchically structured porous material according to its chemical composition and physical characteristics. The present review aims to open up a new avenue to guide the readers to quickly obtain in-depth knowledge of applications of hierarchically porous materials and to have a good idea about selecting and designing suitable hierarchically porous materials for a specific application. In addition to focusing on the applications of hierarchically porous materials, this comprehensive review could stimulate researchers to synthesize new advanced hierarchically porous solids.

Owing to their immense potential in energy conversion and storage, catalysis, photocatalysis, adsorption, separation and life science applications, significant interest has been devoted to the design and synthesis of hierarchically porous materials. The hierarchy of materials on porosity, structural, morphological, and component levels is key for high performance in all kinds of applications. Synthesis and applications of hierarchically structured porous materials have become a rapidly evolving field of current interest. A large series of synthesis methods have been developed. This review addresses recent advances made in studies of this topic. After identifying the advantages and problems of natural hierarchically porous materials, synthetic hierarchically porous materials are presented. The synthesis strategies used to prepare hierarchically porous materials are first introduced and the features of synthesis and the resulting structures are presented using a series of examples. These involve templating methods (surfactant templating, nanocasting, macroporous polymer templating, colloidal crystal templating and bioinspired process, i.e. biotemplating), conventional techniques (supercritical fluids, emulsion, freeze-drying, breath figures, selective leaching, phase separation, zeolitization process, and replication) and basic methods (sol-gel controlling and post-treatment), as well as self-formation phenomenon of porous hierarchy. A series of detailed examples are given to show methods for the synthesis of hierarchically porous structures with various chemical compositions (dual porosities: micro-micropores, micro-mesopores, micro-macropores, meso-mesopores, meso-macropores, multiple porosities: micro-meso-macropores and meso-meso-macropores). We hope that this review will be helpful for those entering the field and also for those in the field who want quick access to helpful reference information about the synthesis of new hierarchically porous materials and methods to control their structure and morphology.

Novel catalytic materials are highly demanded to perform a variety of catalytic organic reactions. MOFs combine the benefits of heterogeneous catalysis like easy post reaction separation, catalyst reusability, high stability and homogeneous catalysis such as high efficiency, selectivity, controllability and mild reaction conditions. The possible organization of active centers like metallic nodes, organic linkers, and their chemical synthetic functionalization on the nanoscale shows potential to build up MOFs particularly modified for catalytic challenges. In this review, we have summarized the recent research progress in heterogeneous catalysis by MOFs and their catalytic behavior in various organic reactions, highlighting the key features of MOFs as catalysts based on the active sites in the framework. Examples of their post functionalization, inclusion of active guest species and metal nanoparticles have been discussed. Finally, the use of MOFs as catalysts for asymmetric heterogeneous catalysis and stability of MOFs has been presented as separate sections.

Silicon oxides have been recognized as a promising family of anode materials for high-energy lithium-ion batteries (LIBs) owing to their abundant reserve, low cost, environmental friendliness, easy synthesis, and high theoretical capacity. However, the extended application of silicon oxides is severely hampered by the intrinsically low conductivity, large volume change, and low initial coulombic efficiency. Significant efforts have been dedicated to tackling these challenges towards practical applications. This Review focuses on the recent advances in the synthesis and lithium storage properties of silicon oxide-based anode materials. To present the progress in a systematic manner, this review is categorized as follows: (i) SiO-based anode materials, (ii) SiO2-based anode materials, (iii) non-stoichiometric SiOx-based anode materials, and (iv) Si-O-C-based anode materials. Finally, future outlook and our personal perspectives on silicon oxide-based anode materials are presented.

A novel Zn/Co zeolitic imidazolate framework (ZIF) has been constructed which demonstrates better gas adsorption (CO₂, CH₄ and N₂) and catalytic (CO₂ conversion) properties compared with ZIF-8 and ZIF-67.

Heterogeneous catalysis is one of the most important chemical processes of various industries performed on catalyst nanoparticles with different sizes or/and shapes. In the past two decades, the catalytic performances of different catalytic reactions on nanoparticles of metals and oxides with well controlled sizes or shapes have been extensively studied thanks to the spectacular advances in syntheses of nanomaterials of metals and oxides. This review discussed the size and shape effects of catalyst particles on catalytic activity and selectivity of reactions performed at solid-gas or solid-liquid interfaces with a purpose of establishing correlations of size- and shape-dependent chemical and structural factors of surface of a catalyst with the corresponding catalytic performances toward understanding of catalysis at a molecular level.

This work demonstrates the development of hierarchical ultra-thin g-C₃N₄ nanosheets with enhanced photocatalytic CO₂ reduction activity.

Hybrid organic-inorganic perovskite photovoltaics (PSCs) have attracted significant attention during the past decade. Despite the stellar rise of laboratory-scale PSC devices, which have reached a certified efficiency over 25% to date, there is still a large efficiency gap when transiting from small-area devices to large-area solar modules. Efficiency losses would inevitably arise from the great challenges of homogeneous coating of large-area high quality perovskite films. To address this problem, we provide an in-depth understanding of the perovskite nucleation and crystal growth kinetics, including the LaMer and Ostwald ripening models, which advises us that fast nucleation and slow crystallization are essential factors in forming high-quality perovskite films. Based on these cognitions, a variety of thin film engineering approaches will be introduced, including the anti-solvent, gas-assisted and solvent annealing treatments, Lewis acid-base adduct incorporation, etc., which are able to regulate the nucleation and crystallization steps. Upscaling the photovoltaic devices is the following step. We summarize the currently developed scalable deposition technologies, including spray coating, slot-die coating, doctor blading, inkjet printing and vapour-assisted deposition. These are more appealing approaches for scalable fabrication of perovskite films than the spin coating method, in terms of lower material/solution waste, more homogeneous thin film coating over a large area, and better morphological control of the film. The working principles of these techniques will be provided, which direct us that the physical properties of the precursor solutions and surface characteristics/temperature of the substrate are both dominating factors influencing the film morphology. Optimization of the perovskite crystallization and film formation process will be subsequently summarized from these aspects. Additionally, we also highlight the significance of perovskite stability, as it is the last puzzle to realize the practical applications of PSCs. Recent efforts towards improving the stability of PSC devices to environmental factors are discussed in this part. In general, this review, comprising the mechanistic analysis of perovskite film formation, thin film engineering, scalable deposition technologies and device stability, provides a comprehensive overview of the current challenges and opportunities in the field of PSCs, aiming to promote the future development of cost-effective up-scale fabrication of highly efficient and ultra-stable PSCs for practical applications.

Ferroelectric polymer nanocomposites with boron nitride nanosheets exhibit greatly improved energy densities and higher charge–discharge efficiencies.

Light, as an external stimulus, is capable of driving the motion of micro/nanomotors (MNMs) with the advantages of reversible, wireless and remote manoeuvre on demand with excellent spatial and temporal resolution. This review focuses on the state-of-the-art light-driven MNMs, which are able to move in liquids or on a substrate surface by converting light energy into mechanical work. The general design strategies for constructing asymmetric fields around light-driven MNMs to propel themselves are introduced as well as the photoactive materials for light-driven MNMs, including photocatalytic materials, photothermal materials and photochromic materials. Then, the propulsion mechanisms and motion behaviors of the so far developed light-driven MNMs are illustrated in detail involving light-induced phoretic propulsion, bubble recoil and interfacial tension gradient, followed by recent progress in the light-driven movement of liquid crystalline elastomers based on light-induced deformation. An outlook is further presented on the future development of light-driven MNMs towards overcoming key challenges after summarizing the potential applications in biomedical, environmental and micro/nanoengineering fields.

We report a melt spinning technique followed by a quick spark plasma sintering procedure to fabricate high-performance p-type Bi0.52Sb1.48Te3 bulk material with unique microstructures. The microstructures consist of nanocrystalline domains embedded in amorphous matrix and 5–15 nm nanocrystals with coherent grain boundary. The significantly reduced thermal conductivity leads to a state-of-the-art dimensionless figure of merit ZT∼1.56 at 300 K, more than 50% improvement of that of the commercial Bi2Te3 ingot materials.

This review summarizes the influences of water molecules during the energy storage process from the perspectives of the electrolyte, Zn anode, and cathode materials, including the basic theory, modification methods, and practical applications.

Nanoscale Bi-based photocatalysts are promising candidates for visible-light-driven photocatalytic environmental remediation and energy conversion. However, the performance of bulk bismuthal semiconductors is unsatisfactory. Increasing efforts have been focused on enhancing the performance of this photocatalyst family. Many studies have reported on component adjustment, morphology control, heterojunction construction, and surface modification. Herein, recent topics in these fields, including doping, changing stoichiometry, solid solutions, ultrathin nanosheets, hierarchical and hollow architectures, conventional heterojunctions, direct Z-scheme junctions, and surface modification of conductive materials and semiconductors, are reviewed. The progress in the enhancement mechanism involving light absorption, band structure tailoring, and separation and utilization of excited carriers, is also introduced. The challenges and tendencies in the studies of nanoscale Bi-based photocatalysts are discussed and summarized.

A novel potassium-containing quadruple-cation absorber realizes over 20% efficiency and hysteresis elimination for planar perovskite solar cells.

Metal-organic frameworks (MOFs) as a new kind of porous crystalline materials have attracted much interest in many applications due to their high porosity, diverse structures, and controllable chemical structures. However, the specific geometrical morphologies, limited functions and unsatisfactory performances of pure MOFs hinder their further applications. In recent years, an efficient approach to synthesize new composites to overcome the above issues has been achieved, by integrating MOF coatings with other functional materials, which have synergistic advantages in many potential applications, including batteries, supercapacitors, catalysis, gas storage and separation, sensors, drug delivery/cytoprotection and so on. Nevertheless, the systemic synthesis strategies and the relationships between their structures and application performances have not been reviewed comprehensively yet. This review emphasizes the recent advances in versatile synthesis strategies and broad applications of MOF coatings. A comprehensive discussion of the fundamental chemistry, classifications and functions of MOF coatings is provided first. Next, by modulating the different states (e.g. solid, liquid, and gas) of metal ion sources and organic ligands, the synthesis methods for MOF coatings on functional materials are systematically summarized. Then, many potential applications of MOF coatings are highlighted and their structure-property correlations are discussed. Finally, the opportunities and challenges for the future research of MOF coatings are proposed. This review on the deep understanding of MOF coatings will bring better directions into the rational design of high-performance MOF-based materials and open up new opportunities for MOF applications.

A series of noble metal diphosphides (IrP₂@NC, RhP₂@NC and Pd₅P₂@NC) have been designed and fabricated, and among which IrP₂@NC exhibits ultrahigh hydrogen evolution reaction performance.

In this review, we have portrayed the structure, synthesis and applications of a variety of biomimetic MOFs from an unprecedented angle. Synthetic MOF analogues of five distinct enzymes: phosphotriesterase, hydrogenase, cytochrome P450, chymotrypsin and carbonic anhydrase, have been discussed with their skeletal comparison to actual enzymatic active sites as reference, and an explanation of catalytic pathways from the mechanistic cycle of the corresponding enzymes is depicted. We demonstrated critically each of the five discrete situations by assimilating available benchmark researches in an attempt to provide a concise literature source on the ingenious design strategies and versatile biomimetic applications of this domain of materials.