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Aqueous sodium-ion batteries (ASIBs) represent a promising battery technology for stationary energy storage, due to their attractive merits of low cost, high abundance, and inherent safety. Recently, a variety of advanced cathode, anode, and electrolyte materials have been developed for ASIBs, which not only enhance our fundamental understanding of the Na insertion mechanism, but also facilitate the research and development of practical ASIB systems. Among these electrode materials, iron-based materials are of particular importance because of the high abundance, low price, and low toxicity of Fe elements. However, to our knowledge, there are no review papers that specifically discuss the properties of Fe-based materials for ASIBs yet. In this review, we present the recent research progress on Fe-based cathode/anode materials, which include polyanionic compounds, Prussian blue, oxides, carbides, and selenides. We also discuss the research efforts to build Fe-based ASIB full cells. Lastly, we share our perspectives on the key challenges that need to be addressed and suggest alternative directions for aqueous Na-ion batteries. We hope this review paper can promote more research efforts on the development of low-cost and low-toxicity materials for aqueous battery applications. 

The solid–solid electrode–electrolyte interface represents an important component in solid‐state batteries (SSBs), as ionic diffusion, reaction, transformation, and restructuring could all take place. As these processes strongly influence the battery performance, studying the evolution of the solid–solid interfaces, particularly in situ during battery operation, can provide insights to establish the structure–property relationship for SSBs. Synchrotron X‐ray techniques, owing to their unique penetration power and diverse approaches, are suitable to investigate the buried interfaces and examine structural, compositional, and morphological changes. In this review, we will discuss various surface‐sensitive synchrotron‐based scattering, spectroscopy, and imaging methods for the in situ characterization of solid–solid interfaces and how this information can be correlated to the electrochemical properties of SSBs. The goal is to overview the advantages and disadvantages of each technique by highlighting representative examples, so that similar strategies can be applied by battery researchers and beyond to study similar solid‐solid interface systems.

 

The safety issue represents a long‐standing obstacle that retards large‐scale applications of high‐energy lithium batteries. Among different causes, thermal runaway is the most prominent one. To date, various approaches have been proposed to inhibit thermal runaway; however, they suffer from some intrinsic drawbacks, either being irreversible (one‐time protection), using volatile and flammable electrolytes, or delayed thermal protection (140–150 °C). Herein, this work exploits a non‐volatile, non‐flammable, and thermo‐reversible polymer/ionic liquid gel electrolyte as a built‐in safety switch, which provides highly precise and reversible thermal protection for lithium batteries. At high temperature, the gel electrolyte experiences phase separation and deposits polymer on the electrode surfaces/separators, which blocks Li⁺insertion reactions and thus prevents thermal runaway. When the temperature decreases, the gel electrolyte restores its original properties and battery performance resumes. Notably, the optimal protection effect is achieved at 110 °C, which is the critical temperature right before thermal runaway. More importantly, such a thermal‐protection process can repeat multiple times without compromising the battery performance, indicating extraordinary thermal reversibility. To the authors' knowledge, such a precise and reversible protection effect has never been reported in any electrolyte systems, and this work opens an exciting avenue for safe operation of high‐energy Li batteries.