Since the discovery of mechanically exfoliated graphene in 2004, research on ultrathin two-dimensional (2D) nanomaterials has grown exponentially in the fields of condensed matter physics, material science, chemistry, and nanotechnology. Highlighting their compelling physical, chemical, electronic, and optical properties, as well as their various potential applications, in this Review, we summarize the state-of-art progress on the ultrathin 2D nanomaterials with a particular emphasis on their recent advances. First, we introduce the unique advances on ultrathin 2D nanomaterials, followed by the description of their composition and crystal structures. The assortments of their synthetic methods are then summarized, including insights on their advantages and limitations, alongside some recommendations on suitable characterization techniques. We also discuss in detail the utilization of these ultrathin 2D nanomaterials for wide ranges of potential applications among the electronics/optoelectronics, electrocat...

Recent Advances in Ultrathin Two-Dimensional Nanomaterials

Energy production and storage technologies have attracted a great deal of attention for day-to-day applications. In recent decades, advances in lithium-ion battery (LIB) technology have improved living conditions around the globe. LIBs are used in most mobile electronic devices as well as in zero-emission electronic vehicles. However, there are increasing concerns regarding load leveling of renewable energy sources and the smart grid as well as the sustainability of lithium sources due to their limited availability and consequent expected price increase. Therefore, whether LIBs alone can satisfy the rising demand for small- and/or mid-to-large-format energy storage applications remains unclear. To mitigate these issues, recent research has focused on alternative energy storage systems. Sodium-ion batteries (SIBs) are considered as the best candidate power sources because sodium is widely available and exhibits similar chemistry to that of LIBs; therefore, SIBs are promising next-generation alternatives. Recently, sodiated layer transition metal oxides, phosphates and organic compounds have been introduced as cathode materials for SIBs. Simultaneously, recent developments have been facilitated by the use of select carbonaceous materials, transition metal oxides (or sulfides), and intermetallic and organic compounds as anodes for SIBs. Apart from electrode materials, suitable electrolytes, additives, and binders are equally important for the development of practical SIBs. Despite developments in electrode materials and other components, there remain several challenges, including cell design and electrode balancing, in the application of sodium ion cells. In this article, we summarize and discuss current research on materials and propose future directions for SIBs. This will provide important insights into scientific and practical issues in the development of SIBs.

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Sodium-ion batteries: present and future

Metal species with different size (single atoms, nanoclusters, and nanoparticles) show different catalytic behavior for various heterogeneous catalytic reactions. It has been shown in the literature that many factors including the particle size, shape, chemical composition, metal–support interaction, and metal–reactant/solvent interaction can have significant influences on the catalytic properties of metal catalysts. The recent developments of well-controlled synthesis methodologies and advanced characterization tools allow one to correlate the relationships at the molecular level. In this Review, the electronic and geometric structures of single atoms, nanoclusters, and nanoparticles will be discussed. Furthermore, we will summarize the catalytic applications of single atoms, nanoclusters, and nanoparticles for different types of reactions, including CO oxidation, selective oxidation, selective hydrogenation, organic reactions, electrocatalytic, and photocatalytic reactions. We will compare the results o...

Metal Catalysts for Heterogeneous Catalysis: From Single Atoms to Nanoclusters and Nanoparticles.

Electrolytes have been identified as some of the most influential components in the performance of electrochemical supercapacitors (ESs), which include: electrical double-layer capacitors, pseudocapacitors and hybrid supercapacitors. This paper reviews recent progress in the research and development of ES electrolytes. The electrolytes are classified into several categories, including: aqueous, organic, ionic liquids, solid-state or quasi-solid-state, as well as redox-active electrolytes. Effects of electrolyte properties on ES performance are discussed in detail. The principles and methods of designing and optimizing electrolytes for ES performance and application are highlighted through a comprehensive analysis of the literature. Interaction among the electrolytes, electro-active materials and inactive components (current collectors, binders, and separators) is discussed. The challenges in producing high-performing electrolytes are analyzed. Several possible research directions to overcome these challenges are proposed for future efforts, with the main aim of improving ESs' energy density without sacrificing existing advantages (e.g., a high power density and a long cycle-life) (507 references).

A review of electrolyte materials and compositions for electrochemical supercapacitors

Ongoing technological advances in diverse fields including portable electronics, transportation, and green energy are often hindered by the insufficient capability of energy-storage devices By taking advantage of two different electrode materials, asymmetric supercapacitors can extend their operating voltage window beyond the thermodynamic decomposition voltage of electrolytes while enabling a solution to the energy storage limitations of symmetric supercapacitors This review provides comprehensive knowledge to this field We first look at the essential energy-storage mechanisms and performance evaluation criteria for asymmetric supercapacitors to understand the wide-ranging research conducted in this area Then we move to the recent progress made for the design and fabrication of electrode materials and the overall structure of asymmetric supercapacitors in different categories We also highlight several key scientific challenges and present our perspectives on enhancing the electrochemical performance of future asymmetric supercapacitors

Design and Mechanisms of Asymmetric Supercapacitors.

Rechargeable aqueous zinc-ion batteries are promising energy storage devices due to their high safety and low cost. However, they remain in their infancy because of the limited choice of positive electrodes with high capacity and satisfactory cycling performance. Furthermore, their energy storage mechanisms are not well established yet. Here we report a highly reversible zinc/sodium vanadate system, where sodium vanadate hydrate nanobelts serve as positive electrode and zinc sulfate aqueous solution with sodium sulfate additive is used as electrolyte. Different from conventional energy release/storage in zinc-ion batteries with only zinc-ion insertion/extraction, zinc/sodium vanadate hydrate batteries possess a simultaneous proton, and zinc-ion insertion/extraction process that is mainly responsible for their excellent performance, such as a high reversible capacity of 380 mAh g–1 and capacity retention of 82% over 1000 cycles. Moreover, the quasi-solid-state zinc/sodium vanadate hydrate battery is also a good candidate for flexible energy storage device. Rechargeable zinc-ion batteries are promising energy storage devices but suffer from the limited choice of positive electrodes. Here Niu and co-workers show a design with sodium vanadate hydrate as cathode, allowing simultaneous proton and zinc-ion insertion/extraction and enhanced performance.

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Aqueous rechargeable zinc/sodium vanadate batteries with enhanced performance from simultaneous insertion of dual carriers.

For instance, freestanding graphene macroscopic structures have shown unique catalytic, electrochemical, and mechanical properties together with potential applications in chemical fi lters and electrodes for energy storage devices. [ 6–8 , 11 , 30 ] However, in most cases, during the process of assembling nanometerscale building blocks into macroscopic paper-like structures, the large accessible surface area of 2D graphene sheets is lost. The reason for this is that the individual graphene sheets tend to irreversibly aggregate and restack owing to the strong π π stacking and van der Waals force between the planar basal planes of graphene sheets. This reduces the potential applications of graphene materials in electrochemical electrodes, composite materials, and so on. [ 20 ] Therefore, preventing aggregation of graphene sheets in the macroscopic structures, such that the properties of the individual graphene sheets are not compromised, is a critical challenge in constructing functional graphene-based macroscopic structures. Currently, a number of strategies for preventing aggregation have been developed, which include adding spacers (e.g., surfactants, nanoparticles, polymers), [ 27–36 ] template-assisted growth, [ 37 ] and crumpling the graphene sheets. [ 18 , 38 ] Alternatively, several groups have reported the formation of freestanding 3D graphene-based macroscopic structures without the assistance of any spacers or templates. [ 7 , 39,40 ] For instance, Li and coworkers reported the preparation of freestanding multilayered graphene fi lms by vacuum-assisted fi ltration based on the effective prevention of graphene intersheet restacking. [ 7 ] Shi and coworkers demonstrated the formation of a 3D graphene hydrogel by a hydrothermal method. [ 39 ] However, preparing freestanding and fl exible graphene fi lms with large accessible surface area but

A leavening strategy to prepare reduced graphene oxide foams.

The use of well-defined materials in heterogeneous catalysis will open up numerous new opportunities for the development of advanced catalysts to address the global challenges in energy and the environment. This review surveys the roles of nanoparticles and isolated single atom sites in catalytic reactions. In the second section, the effects of size, shape, and metal-support interactions are discussed for nanostructured catalysts. Case studies are summarized to illustrate the dynamics of structure evolution of well-defined nanoparticles under certain reaction conditions. In the third section, we review the syntheses and catalytic applications of isolated single atomic sites anchored on different types of supports. In the final part, we conclude by highlighting the challenges and opportunities of well-defined materials for catalyst development and gaining a fundamental understanding of their active sites.

Well-Defined Materials for Heterogeneous Catalysis: From Nanoparticles to Isolated Single-Atom Sites.

Capping agents are frequently used in colloidal synthesis to inhibit nanoparticle overgrowth and aggregation as well as to control the structural characteristics of the resulted nanoparticles in a precise manner. Study of the effect of the residual capping agents on particle surface has unveiled various adverse and favorable behaviors in catalytic applications. In essence, while the capping agents usually act as a physical barrier to restrict the free access of reactants to catalytic nanoparticles, they can also be utilized to promote catalytic performance of nanocrystals. Due to the complexity of these effects, a general survey of capping agents in nanocatalysis is therefore necessary. This short review starts from a brief introduction of common capping agents in nanoparticle synthesis and their adverse impact on heterogeneous catalysis. Next, representative progresses in capping agent removal and surfactant-free synthesis for obtaining surface-clean nanocatalysts are summarized. Lastly, we discuss the r...

Removal and Utilization of Capping Agents in Nanocatalysis

Rechargeable zinc-ion batteries (ZIBs) are promising for large scale energy storage and portable electronic applications due to their low cost, material abundance, high safety, acceptable energy density and environmental friendliness. This tutorial review presents an introduction to the fundamentals, challenges, recent advances and prospects related to ZIBs. Firstly, the intrinsic chemical properties, challenges and strategies of metallic zinc anodes are underscored. Then, the multiple types of cathode materials are classified and comparatively discussed in terms of their structural and electrochemical properties, issues and remedies. Specific attention is paid to the mechanistic understanding and structural transformation of cathode materials based on Zn ion-(de)intercalation chemistry. After that, the widely investigated electrolytes are elaborated by discussing their effect on Zn plating/stripping behaviours, reaction kinetics, electrode/electrolyte interface chemistries, and cell performances. Finally, the remaining challenges and future perspectives are outlined for the development of ZIBs.

Zhiqiang Niu

Papers

Aqueous rechargeable zinc/sodium vanadate batteries with enhanced performance from simultaneous insertion of dual carriers.

A leavening strategy to prepare reduced graphene oxide foams.

Well-Defined Materials for Heterogeneous Catalysis: From Nanoparticles to Isolated Single-Atom Sites.

Removal and Utilization of Capping Agents in Nanocatalysis

Materials chemistry for rechargeable zinc-ion batteries