State Key Laboratory of Materials-Oriented Chemical Engineering

Graphene is a well-known two-dimensional material that exhibits preeminent electrical, mechanical and thermal properties owing to its unique one-atom-thick structure. Graphene and its derivatives (e.g., graphene oxide) have become emerging nano-building blocks for separation membranes featuring distinct laminar structures and tunable physicochemical properties. Extraordinary molecular separation properties for purifying water and gases have been demonstrated by graphene-based membranes, which have attracted a huge surge of interest during the past few years. This tutorial review aims to present the latest groundbreaking advances in both the theoretical and experimental chemical science and engineering of graphene-based membranes, including their design, fabrication and application. Special attention will be given to the progresses in processing graphene and its derivatives into separation membranes with three distinct forms: a porous graphene layer, assembled graphene laminates and graphene-based composites. Moreover, critical views on separation mechanisms within graphene-based membranes will be provided based on discussing the effect of inter-layer nanochannels, defects/pores and functional groups on molecular transport. Furthermore, the separation performance of graphene-based membranes applied in pressure filtration, pervaporation and gas separation will be summarized. This article is expected to provide a compact source of relevant and timely information and will be of great interest to all chemists, physicists, materials scientists, engineers and students entering or already working in the field of graphene-based membranes and functional films.

Meeting the growing global energy demand is one of the important challenges of the 21st century. Currently over 80% of the world's energy requirements are supplied by the combustion of fossil fuels, which promotes global warming and has deleterious effects on our environment. Moreover, fossil fuels are non-renewable energy and will eventually be exhausted due to the high consumption rate. A new type of alternative energy that is clean, renewable and inexpensive is urgently needed. Several candidates are currently available such as hydraulic power, wind force and nuclear power. Solar energy is particularly attractive because it is essentially clean and inexhaustible. A year's worth of sunlight would provide more than 100 times the energy of the world's entire known fossil fuel reserves. Photocatalysis and photovoltaics are two of the most important routes for the utilization of solar energy. However, environmental protection is also critical to realize a sustainable future, and water pollution is a serious problem of current society. Photocatalysis is also an essential route for the degradation of organic dyes in wastewater. A type of compound with the defined structure of perovskite (ABX3) was observed to play important roles in photocatalysis and photovoltaics. These materials can be used as photocatalysts for water splitting reaction for hydrogen production and photo-degradation of organic dyes in wastewater as well as for photoanodes in dye-sensitized solar cells and light absorbers in perovskite-based solar cells for electricity generation. In this review paper, the recent progress of perovskites for applications in these fields is comprehensively summarized. A description of the basic principles of the water splitting reaction, photo-degradation of organic dyes and solar cells as well as the requirements for efficient photocatalysts is first provided. Then, emphasis is placed on the designation and strategies for perovskite catalysts to improve their photocatalytic activity and/or light adsorption capability. Comments on current and future challenges are also provided. The main purpose of this review paper is to provide a current summary of recent progress in perovskite materials for use in these important areas and to provide some useful guidelines for future development in these hot research areas.

Recent years have witnessed an upsurge in the development of non-precious catalysts (NPCs) for alkaline water electrolysis (AWE), especially with the strides made in experimental and computational techniques. In this contribution, the most recent advances in NPCs for AWE were systematically reviewed, emphasizing the application of in situ/operando experimental methods and density functional theory (DFT) calculations in their understanding and development. First, we briefly introduced the fundamentals of the anode and cathode reaction for AWE, i.e., the oxygen evolution reaction (OER) and the hydrogen evolution reaction (HER), respectively. Next, the most popular in situ/operando approaches for characterizing AWE catalysts, including hard and soft XAS, ambient-pressure XPS, liquid and identical location TEM, electrochemical mass spectrometry, and Raman spectroscopy were thoroughly summarized. Subsequently, we carefully discussed the principles, computational methods, applications, and combinations of DFT with machine learning for modeling NPCs and predicting the alkaline OER and HER. With the improved understanding of the structure-property-performance relationship of NPCs for AWE, we proceeded to overview their current development, summarising state-of-the-art design strategies to boost their activity. In addition, advances in various extensively investigated NPCs for AWE were evaluated. By conveying these methods, progress, insights, and perspectives, this review will contribute to a better understanding and rational development of non-precious AWE electrocatalysts for hydrogen production.

Recent research progresses on high performance anode materials for high-energy sodium-ion batteries are comprehensively summarized.

Metal oxide-based materials are emerging as a promising family of hydrogen evolution reaction (HER) electrocatalysts.

Key challenges include rational design of flexible cell components, exploration of novel configurations, and optimization of operation management.

Ionic liquids (ILs) and deep eutectic solvents (DESs) have been suggested as eco-friendly alternatives to organic solvents. A trace amount of water is often unavoidable as impurity, and water is also added on purpose to reduce their problematically high viscosity and lower their high price. Understanding the distinct effects of water on the properties of ILs/DESs is highly important. In this review, we collect published experimental and theoretical results for IL/DES-H2O systems at varied water concentrations and analyze them. Results from mechanistic studies, thermodynamic modelling and advanced experiments are collected and critically discussed. Six commonly studied IL/DES-H2O systems were selected to map experimental observations onto microscopic results obtained in mechanistic studies. A great variety of distinct contours of the excess properties can be observed over the entire compositional range, indicating that the properties of IL/DES-H2O systems are highly unpredictable. Mechanistic studies clearly demonstrate that the added H2O rapidly changes the heterogeneous 3D structures of pure ILs/DESs, leading to very different properties and behaviour. There are similarities between aqueous electrolytes and IL/DES solutions but the bulky and asymmetric organic cations in ILs/DESs do not conform to the standard salt dissolution and hydration concepts. Thermodynamic modelling previously assumes ILs/DESs to be either a neutral ion-pair or completely dissociated ions, neglecting specific ion hydration effects. A new conceptual framework is suggested for thermodynamic modelling of IL/DES-H2O binary systems to enable new technologies for their practical applications.

This review summarizes the advances in non-enzymatic glucose sensors based on different metal oxides (ZnO, CuO/Cu₂O, NiO,<italic>etc.</italic>) and their composites.

This review provides a comprehensive survey and critical comments on the development of photocatalysts with a focus on the metal-free materials.

Mesoporous solid bases are extremely desirable in green catalytic processes, due to their advantages of accelerated mass transport, negligible corrosion, and easy separation. Great progress has been made in mesoporous solid bases in the last decade. In addition to their wide applications in the catalytic synthesis of organics and fine chemicals, mesoporous solid bases have also been used in the field of energy and environmental catalysis. Development of mesoporous solid bases is therefore of significant importance from both academic and practical points of view. In this review, we provide an overview of the recent advances in mesoporous solid bases, which is basically grouped by the support type and each category is illustrated with typical examples. Cooperative catalysts derived from the incorporation of additional functionalities (i.e. acid and metal) into mesoporous solid bases are also included. The fundamental principles of how to design and fabricate basic materials with mesostructure are highlighted. The mechanism of the formation of basic sites in different mesoporous systems is discussed as well.

Steel slag has been used as supplementary cementitious materials or aggregates in concrete. However, the substitution levels of steel slag for Portland cement or natural aggregates were limited due to its low hydraulic property or latent volume instability. In this study, 60% of steel slag powders containing high free-CaO content, 20% of Portland cement and up to 20% of reactive magnesia and lime were mixed to prepare the binding blends. The binding blends were then used to cast concrete, in which up to 100% of natural aggregates (limestone and river sands) were replaced with steel slag aggregates. The concrete was exposed to carbonation curing with a concentration of 99.9% CO2 and a pressure of 0.10 MPa for different durations (1d, 3d, and 14d). The carbonation front, carbonate products, compressive strength, microstructure, and volume stability of the concrete were investigated. Results show that the compressive strength of the steel slag concrete after CO2 curing was significantly increased. The compressive strengths of concrete subjected to CO2 curing for 14d were up to five-fold greater than that of the corresponding concrete under conventional moist curing for 28d. This is attributed to the formation of calcium carbonates, leading to a microstructure densification of the concrete. Replacement of limestone and sand aggregates with steel slag aggregates also increased the compressive strengths of the concrete subjected to CO2 curing. In addition, the concrete pre-exposed to CO2 curing produced less expansion than the concrete pre-exposed to moist curing during the subsequent accelerated curing in 60 °C water. This study provides a potential approach to prepare concrete with low-carbon emissions via the accelerated carbonation of steel slag.

We summarize recent developments of Ruddlesden–Popper perovskites as intriguing and high-performing electrocatalysts for key reactions relevant to energy conversion and storage at both low and high temperatures.

2-Phenylimidazoline based porous hypercrosslinked ionic polymers afforded high yields in the cycloaddition of epoxides with ambient or diluted CO₂ (0.15 bar CO₂ and 0.85 bar N₂) under low or room temperature.

A comprehensive review of current developments in artificial buffer layer-modified electrode–electrolyte interfaces for solid-state Li-ion batteries.

Meso-macroporous hierarchical poly(ionic liquid)s are ionothermally synthesized through self-polymerization of the new divinylimidazole IL, exhibiting enhanced CO₂ capture and excellent activity in the cycloaddition of CO₂ to epoxides.

Based on an organic ligand involving both carboxylate and tetrazole groups, a chemically stable Zn(II) metal-organic framework has been rationally synthesized and behaves as a fluorescence chemosensor for the highly selective and sensitive detection of picric acid, an extremely hazardous and strong explosive.

We synthesized luminescent CsPbBr₃ nanocrystals with a high quantum yield and realized patterning and color-purity light-emitting diode applications.

In this study, we report a promising rGO-CNT hybrid nanofiltration (NF) membrane that was fabricated by loading reduced graphene oxide that was intercalated with carbon nanotubes (rGO-CNTs) onto an anodic aluminum oxide (AAO) microfiltration membrane via a facile vacuum-assisted filtration process. To create this NF membrane, the CNTs were first dispersed using block copolymers (BCPs); the effects of the types and contents of BCPs used on the dispersion of CNTs have been investigated. The as-prepared rGO-CNT hybrid NF membranes were then used for drinking water purification to retain the nanoparticles, dyes, proteins, organophosphates, sugars, and particularly humic acid. Experimentally, it is shown that the rGO-CNT hybrid NF membranes have high retention efficiency, good permeability and good anti-fouling properties. The retention was above 97.3% even for methyl orange (327 Da); for other objects, the retention was above 99%. The membrane's permeability was found to be as high as 20-30 L m(-2) h(-1) bar(-1). Based on these results, we can conclude that (i) the use of BCPs as a surfactant can enhance steric repulsion and thus disperse CNTs effectively; (ii) placing well-dispersed 1D CNTs within 2D graphene sheets allows an uniform network to form, which can provide many mass transfer channels through the continuous 3D nanostructure, resulting in the high permeability and separation performance of the rGO-CNT hybrid NF membranes.

Polyoxometalates (POMs) are a unique class of molecular metal oxides with a tunable structure at the atomic level. They have demonstrated various potential applications in various fields. In particular, POMs have been widely used as catalysts, due to their facilely modified acid–base properties and redox potential through molecular designing. Normally, POMs can be utilized as both homogeneous and heterogeneous catalysts, where the former favors high activity, while the latter benefits facile separation of the catalysts. Faced with the requirement for sustainable development, significant effort has been made in the preparation of POM-based heterogeneous catalysts. This review focuses on the recent developments in heterogeneous strategies of POM-based catalysts and their applications in liquid organic reactions.

<italic>b</italic>- and<italic>c</italic>-oriented ZIF-<italic>L</italic>membranes were synthesized by controlling ZIF-<italic>L</italic>orientational growth, and they showed orientation-dependent gas permeation properties.