Two-Dimensional Germanium Sulfide Nanosheets as an Ultra-Stable and High Capacity Anode for Lithium Ion Batteries

Lithium ion batteries (LIBs) at present still suffer from low rate capability and poor cycle life during fast ion insertion/extraction processes. Searching for high-capacity and stable anode materials is still an ongoing challenge. Herein, a facile strategy for the synthesis of ultrathin GeS₂ nanosheets with the thickness of 1.1 nm is reported. When used as anodes for LIBs, the two-dimensional (2D) structure can effectively increase the electrode/electrolyte interface area, facilitate the ion transport, and buffer the volume expansion. Benefiting from these merits, the as-synthesized GeS₂ nanosheets deliver high specific capacity (1335 mAh g⁻¹ at 0.15 A g⁻¹), extraordinary rate performance (337 mAh g⁻¹ at 15 A g⁻¹) and stable cycling performance (974 mAh g⁻¹ after 200 cycles at 0.5 A g⁻¹). Importantly, our fabricated Li-ion full cells manifest an impressive specific capacity of 577 mAh g⁻¹ after 50 cycles at 0.1 A g⁻¹ and a high energy density of 361 Wh kg⁻¹ at a power density of 346 W kg⁻¹. Furthermore, the electrochemical reaction mechanism is investigated by the means of ex-situ high-resolution transmission electron microscopy. These results suggest that GeS₂ can use to be an alternative anode material and encourage more efforts to develop other high-performance LIBs anodes.     

Molybdenum Disulfide Based Nanomaterials for Rechargeable Batteries

The rapid development of electrochemical energy storage systems requires new electrode materials with high performance. As a two-dimensional material, molybdenum disulfide (MoS₂) has attracted increasing interest in energy storage applications due to its layered structure, tunable physical and chemical properties, and high capacity. In this review, the atomic structures and properties of different phases of MoS₂ are first introduced. Then, typical synthetic methods for MoS₂ and MoS₂-based composites are presented. Furthermore, the recent progress in the design of diverse MoS₂-based micro/nanostructures for rechargeable batteries, including lithium-ion, lithium-sulfur, sodium-ion, potassium-ion, and multivalent-ion batteries, is overviewed. Additionally, the roles of advanced in situ/operando techniques and theoretical calculations in elucidating fundamental insights into the structural and electrochemical processes taking place in these materials during battery operation are illustrated. Finally, a perspective is given on how the properties of MoS₂-based electrode materials are further improved and how they can find widespread application in the next-generation electrochemical energy-storage systems.     

N-Doped Graphdiyne Coating for Dendrite-Free Lithium Metal Batteries

Nonuniform nucleation is one of the major reasons for the dendric growth of metallic lithium, which leads to intractable problems in the efficiency, reversibility, and safety in Li-based batteries. To improve the deposition of metallic Li on Cu substrates, herein, a freestanding current collector (NGDY@CuNW) is formed by coating pyridinic nitrogen-doped graphdiyne (NGDY) nanofilms on 3D Cu nanowires (CuNWs). Theoretical predictions reveal that the introduction of nitrogen atoms in the 2D GDY can enhance the binding energy between the Li atom and GDY, therefore improving the lithiophilicity on the surface for uniform lithium nucleation and deposition. Accordingly, the deposited metallic Li on the NGDY@CuNW electrode exhibits a dendrite-free morphology, resulting in significant improvements in terms of the reversibility with a high coulombic efficiency (CE) and a long lifespan at high current density. Our research provides an efficient method to control the surface property of Cu, which also will be instructive for other metal batteries.     

MXene-Based Nanocomposites for Energy Conversion and Storage Applications

Novel nanomaterials and advanced nanotechnology continuously push forward the rapid development of sustainable energy conversion and storage equipment. An emerging family of two-dimensional transition-metal carbides, nitrides and carbonitrides, also known as MXenes, have attracted increasing attention and in depth investigation. Benefitting from their unique intrinsic properties, MXenes have attracted significant attention and they have been considered as promising candidate materials for the development of environmentally friendly energy resources. A large number of studies show that MXenes have great potential in energy conversion and storage fields. Despite of their exceptional properties, MXenes also have some inherent characteristics, such as low capacities and unstable retention performances, which severely hinder their prospect applications in energy conversion and storage fields. In this Minireview, the latest progress on MXenes and their hybrid composites with small molecules, polymers, carbon or metal ions, and their applications in energy conversion and storage fields is highlighted, including their use in different types of batteries, supercapacitors, hydrogen/oxygen evolution reactions, electromagnetic interference absorption/shielding and solar steam generation. In addition, the critical challenges and further development prospects of MXene-based materials are also introduced.     

Engineering Bifunctional Host Materials of Sulfur and Lithium-Metal Based on Nitrogen-Enriched Polyacrylonitrile for Li–S Batteries

Lithium–sulfur batteries (LSBs) still suffer from the shuttle effect on the cathode and the lithium dendrite on the anode. Herein, polyacrylonitrile (PAN) is developed into a bifunctional host material to simultaneously address the challenges faced on both the sulfur cathode and lithium anode in LSBs. For the sulfur cathode, PAN is bonded with sulfur to produce sulfurized PAN (SPAN) to avoid the shuttle effect. The SPAN is accommodated into a conductive 3D CNTs-wrapped carbon foam to prepare a self-supporting cathode, which improves the electronic and ionic conductivity, and buffers the volume expansion. Thereby, it delivers reversible capacity, superb rate capability, and outstanding cycling stability. For the Li-metal anode, PAN aerogel is carbonized to give macroporous N-doped cross-linked carbon nanofiber that behaves as a lithiophilic host to regulate Li plating and suppress the growth of Li dendrite. Combining the improvements for both the cathode and anode realizes a remarkable long-term cyclability (765 mAh g⁻¹ after 300 cycles) in a full cell. It provides new opportunity to propel the practical application of advanced LSBs.     

Toward Understanding the Enhanced Pseudocapacitive Storage in 3D SnS/MXene Architectures Enabled by Engineered Surface Reactions

The optimization of three-dimensional (3D) MXene-based electrodes with desired electrochemical performances is highly demanded. Here, a precursor-guided strategy is reported for fabricating the 3D SnS/MXene architecture with tiny SnS nanocrystals (≈5 nm in size) covalently decorated on the wrinkled Ti₃C₂T_x nanosheets through Ti−S bonds (denoted as SnS/Ti₃C₂T_x-O). The formation of Ti−S bonds between SnS and Ti₃C₂T_x was confirmed by extended X-ray absorption fine structure (EXAFS). Rather than bulky SnS plates decorated on Ti₃C₂T_x (SnS/Ti₃C₂T_x-H) by one-step hydrothermal sulfidation followed by post annealing, this SnS/Ti₃C₂T_x-O presents size-dependent structural and dynamic properties. The as-formed 3D hierarchical structure can provide short ion-diffusion pathways and electron transport distances because of the more accessible surface sites. In addition, benefiting from the tiny SnS nanocrystals that can effectively improve Na⁺ diffusion and suppress structural variation upon charge/discharge processes, the as-obtained SnS/Ti₃C₂T_x-O can generate pseudocapacitance-dominated storage behavior enabled by engineered surface reactions. As predicted, this electrode exhibits an enhanced Na storage capacity of 565 mAh g⁻¹ at 0.1 A g⁻¹ after 75 cycles, outperforming SnS/Ti₃C₂T_x-H (336 mAh g⁻¹), SnS (212 mAh g⁻¹), and Ti₃C₂T_x (104 mAh g⁻¹) electrodes.     

Atomic-Scale Dispersed Fe-Based Catalysts Confined on Nitrogen-Doped Graphene for Li-S Batteries: Polysulfides with Enhanced Conversion Efficiency

Lithium-sulfur batteries have been considered as potential electrochemical energy-storage devices owing to their satisfactory theoretical energy density. Nonetheless, the inferior conversion efficiency of polysulfides in essence leads to fast capacity decay during the discharge/charge cycle. In this work, it is successfully demonstrated that the conversion efficiency of lithium polysulfides is remarkably enhanced by employing a well-distributed atomic-scale Fe-based catalyst immobilized on nitrogen-doped graphene (Fe@NG) as a coating of separator in lithium-sulfur batteries. The quantitative electrocatalytic efficiency of the conversion of lithium polysulfides is determined through cyclic voltammetry. It is also proven that the Fe-N_X configuration with highly catalytic activity is quite beneficial for the conversion of lithium polysulfides. In addition, the adsorption and permeation experiments distinctly indicate that the strong anchoring effect, originated from the charge redistribution of N doping into the graphene matrix, inhibits the movement of lithium polysulfides. Thanks to these advantages, if the as-prepared Fe@NG catalyst is combined with polypropylene and applied as a separator (Fe@NG/PP) in Li-S batteries, a high initial capacity (1616 mA h g⁻¹ at 0.1 C), excellent capacity retention (93 % at 0.2 C, 70 % at 2 C), and superb rate performance (820 mA h g⁻¹ at 2 C) are achieved.     

Fe3O4@C Nanotubes Grown on Carbon Fabric as a Free-Standing Anode for High-Performance Li-Ion Batteries

Recently, Li-ion batteries (LIBs) have attracted extensive attention owing to their wide applications in portable and flexible electronic devices. Such a huge market for LIBs has caused an ever-increasing demand for excellent mechanical flexibility, outstanding cycling life, and electrodes with superior rate capability. Herein, an anode of self-supported Fe₃O₄@C nanotubes grown on carbon fabric cloth (CFC) is designed rationally and fabricated through an in situ etching and deposition route combined with an annealing process. These carbon-coated nanotube structured Fe₃O₄ arrays with large surface area and enough void space can not only moderate the volume variation during repeated Li⁺ insertion/extraction, but also facilitate Li⁺/electrons transportation and electrolyte penetration. This novel structure endows the Fe₃O₄@C nanotube arrays stable cycle performance (a large reversible capacity of 900 mA h g⁻¹ up to 100 cycles at 0.5 A g⁻¹) and outstanding rate capability (reversible capacities of 1030, 985, 908, and 755 mA h g⁻¹ at 0.15, 0.3, 0.75, and 1.5 A g⁻¹, respectively). Fe₃O₄@C nanotube arrays still achieve a capacity of 665 mA h g⁻¹ after 50 cycles at 0.1 A g⁻¹ in Fe₃O₄@C//LiCoO₂ full cells.     

Understanding cathode materials in aqueous zinc–organic batteries

Organic electrode materials (OEMs) are being investigated as promising candidates for aqueous zinc-ion batteries (AZIBs) owing to their environmental friendliness, cost-effectiveness, and structural diversity, and tunability. Understanding the correlation between structural regulation of OEMs and their electrochemical property in AZIBs is vital to rational design of OEMs. Herein, we first discuss the fundamentals of the energy storage mechanism of OEMs. Then, strategies to improve the electrochemical performance, including the specific capacity, voltage, rate capability, and cycling stability, are elaborated from the perspective of molecular engineering. Finally, we share our views on the remaining challenges and prospects of OEMs in AZIBs.     

Recent Advances of Freestanding Cathodes for Li-S Batteries

Lithium-sulfur batteries (LSBs) with high energy density and low cost have been recognized as one of the most promising next-generation energy storage systems. Although it has taken decades of development, the practical application of LSBs has been hindered by several inherent obstacles, particularly the severe shuttle effect and sluggish reaction kinetics in the sulfur cathode. Various strategies have been proposed to address these problems via rational design of electrode materials and configurations. Freestanding sulfur cathode could be a promising strategy to improve the sulfur mass loading at the cathode level and energy density of LSBs. This minireview will briefly summary the recent advances in freestanding cathodes for LSBs. The advantages and disadvantages of various freestanding cathodes are discussed and the prospects for the development of flexible cathodes are envisioned.