Hierarchical copper silicate hydrate hollow spheres-reduced graphene oxide (RGO) composite is successfully fabricated by a facile hydrothermal method using silica as in situ sacrificing template. The electrochemical performance of the composite as lithium-ion battery anode was studied for the first time. Benefiting from the synergistic effect of the hierarchical hollow structure and conductive RGO matrix, the composite exhibits excellent long-life performance and rate capability. A capacity of 890 mAh/g is achieved after 200 cycles at 200 mA/g and a capacity of 429 mAh/g is retained after 800 cycles at 1000 mA/g. The results indicate that the strategy of combining hierarchical hollow structures with conductive RGO holds the potential in addressing the volume expansion issue of high capacity anode materials.

Copper Silicate Hydrate Hollow Spheres Constructed by Nanotubes Encapsulated in Reduced Graphene Oxide as Long-Life Lithium-Ion Battery Anode

Sodium-ion batteries (SIBs) are a viable alternative to meet the requirements of future large-scale energy storage systems due to the uniform distribution and abundant sodium resources. Among the various cathode materials for SIBs, phosphate-based polyanionic compounds exhibit excellent sodium-storage properties, such as high operation voltage, remarkable structural stability, and superior safety. However, their undesirable electronic conductivities and specific capacities limited their application in large-scale energy storage systems. Herein, the development history and recent progress of phosphate-based polyanionic cathodes are first overviewed. Subsequently, the effective modification strategies of phosphate-based polyanionic cathodes are summarized toward high-performance SIBs, including surface coating, morphological control, ion doping, and electrolyte optimization. Besides, the electrochemical performance, cost, and industrialization analysis of phosphate-based polyanionic cathodes for SIBs are discussed for accelerating commercialization development. Finally, the future directions of phosphate-based polyanionic cathodes are comprehensively concluded.  We believe that this review can provide instructive insight into developing practical phosphate-based polyanionic cathodes for SIBs. This article is protected by copyright. All rights reserved.

The Distance Between Phosphate-Based Polyanionic Compounds and Their Practical Application For Sodium-Ion Batteries.

Magnesium Ion Doping and Micro‐Structural Engineering Assist NH4V4O10 as a High‐Performance Aqueous Zinc Ion Battery Cathode

Recent progress in rational structural regulation for high-efficiency potassium-ion batteries is reviewed. 

Recent advances in rational design for high-performance potassium-ion batteries

The low cost and intrinsic safety of rechargeable aqueous zinc‐ion batteries (ZIBs) contribute to their significant potential in grid‐level energy storage systems. However, the limited cathode options still hinder the development of ZIBs, which always delivers poor rate capacities and cycling stability. Herein, Monoclinic phase H3.78V6O13 microspheres with a stable internal framework and intrinsic metallic properties as a high‐performance cathode for ZIBs are proposed and utilized. The reversible Zn2+insertion/de‐insertion mechanism in H3.78V6O13through ex situ X‐ray diffraction, X‐ray absorption near‐edge structure, and in situ Raman involves the enlargement/shrink of interplanar distance, the decrease/increase of the V valance, and the open/recombine of V─O/V─V bonds. Further, experiments and theoretical calculations elucidate the superior electrochemical performance and extraordinary reaction kinetics in H3.78V6O13. The as‐prepared H3.78V6O13 cathode delivers high specific capacity of 406 mAh g–1 at 0.1 A g–1, excellent structure stability with 100% manifested after 120 cycles at 0.5 A g–1, 72.9% retained after 15 000 cycles at 10 A g–1. This research offers distinctive perspectives on the development of high‐performance cathode materials for ZIBs and enhances the understanding of the electrochemical reaction mechanisms of vanadium oxides.

Unveiling the X‐Ray Absorption Chemistry of H3.78V6O13 Cathode for Aqueous Zinc‐Ion Batteries

Vanadium oxides with multioxidation states and various crystalline structures offer unique electrical, optical, optoelectronic and magnetic properties, which could be manipulated for various applications. For the past 30 years, significant efforts have been made to study the fundamental science and explore the potential for vanadium oxide materials in ion batteries, water splitting, smart windows, supercapacitors, sensors, and so on. This review focuses on the most recent progress in synthesis methods and applications of some thermodynamically stable and metastable vanadium oxides, including but not limited to V2O3, V3O5, VO2, V3O7, V2O5, V2O2, V6O13, and V4O9. We begin with a tutorial on the phase diagram of the V–O system. The second part is a detailed review covering the crystal structure, the synthesis protocols, and the applications of each vanadium oxide, especially in batteries, catalysts, smart windows, and supercapacitors. We conclude with a brief perspective on how material and device improvements can address current deficiencies. This comprehensive review could accelerate the development of novel vanadium oxide structures in related applications.

https://doi.org/10.1021/acs.chemrev.2c00546

Vanadium Oxide: Phase Diagrams, Structures, Synthesis, and Applications

Na superionic conductor (NASICON) structured cathode materials with robust structural stability and large Na+ diffusion channels have aroused great interest in sodium-ion batteries (SIBs). However, most of NASICON-type cathode materials exhibit redox reactions of no more than three electrons per formula, which strictly limits capacity and energy density. Herein, a series of NASICON-type Na3+xMnTi1-xV x (PO4)3 cathode materials are designed, which demonstrate not only a multi-electron reaction but also high voltage platform. With five redox couples from V5+/4+ (~4.1 V), Mn4+/3+ (~4.0 V), Mn3+/2+ (~3.6 V), V4+/3+ (3.4 V), and Ti4+/3+ (~2.1 V), the optimized material, Na3.2MnTi0.8V0.2(PO4)3, realizes a reversible 3.2-electron redox reaction, enabling a high discharge capacity (172.5 mAh g-1) and an ultrahigh energy density (527.2 Wh kg-1). This work sheds light on the rational construction of NASICON-type cathode materials with multi-electron redox reactions for high-energy SIBs.

A High-Energy NASICON-Type Na3.2MnTi0.8V0.2(PO4)3 Cathode Material with Reversible 3.2-Electron Redox Reaction for Sodium-Ion Batteries.

Revealing excess Al3+ preinsertion on altering diffusion paths of aluminum vanadate for zinc-ion batteries

To enhance the energy density of batteries and explore intrinsic charge storage mechanism of the active materials, it is important to reduce or eliminate the use of non‐active materials in electrodes, such as binder and conductive additives. Herein, free‐standing Na4MnV(PO4)3@C (F‐NMVP@C) fiber membrane is fabricated and directly used as a sodium‐ion battery (SIB) cathode. In situ X‐ray diffraction reveals that the V3+/V4+ redox reaction occurs through a solid‐solution reaction while a two‐phase Mn2+/Mn3+ redox reaction is identified, and both are highly reversible. Meanwhile, ex situ electrochemical impedance spectroscopy reveals that both the ion diffusion coefficient and charge transfer resistance of F‐NMVP@C change reversibly during the Na+ intercalation/de‐intercalation. Battery full cells are assembled based on the free‐standing F‐NMVP@C cathodes and F‐Sb@C anodes, which manifests a high energy density (293 Wh kg−1) and good cyclability (87.5% after 100 cycles at 1 C). The high‐performance free‐standing cathodes and anodes shed light on the development of flexible SIBs.

Sodium Ion Storage in Na4MnV(PO4)3@C Free‐Standing Electrode

Introducing anionic redox in layered oxides is an effective approach to breaking the capacity limit of conventional cationic redox. However, the anionic redox reaction generally suffers from excessive oxidation of lattice oxygen to O2 and O2 release, resulting in local structural deterioration and rapid capacity/voltage decay. Here, a Na0.71Li0.22Al0.05Mn0.73O2 (NLAM) cathode material is developed by introducing Al3+ into the transition metal (TM) sites. Thanks to the strong Al–O bonding strength and small Al3+ radius, the TMO2 skeleton and the holistic TM–O bonds in NLAM are comprehensively strengthened, which inhibits the excessive lattice oxygen oxidation. The obtained NLAM exhibits a high reversible capacity of 194.4 mAh g‐1 at 20 mA g‐1 and decent cyclability with 98.6% capacity retention over 200 cycles at 200 mA g−1. In situ characterizations reveal that the NLAM experiences phase transitions with an intermediate OP4 phase during the charge–discharge. Theoretical calculations further confirm that the Al substitution strategy is beneficial for improving the overlap between Mn 3d and O 2p orbitals. This finding sheds light on the design of layered oxide cathodes with highly reversible anionic redox for sodium storage.

Comprehensively Strengthened Metal‐Oxygen Bonds for Reversible Anionic Redox Reaction

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