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  1. 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. 
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  3. Abstract

    Iron ion batteries using Fe2+as a charge carrier have yet to be widely explored, and they lack high‐performing Fe2+hosting cathode materials to couple with the iron metal anode. Here, it is demonstrated that VOPO4∙2H2O can reversibly host Fe2+with a high specific capacity of 100 mAh g−1and stable cycling performance, where 68% of the initial capacity is retained over 800 cycles. In sharp contrast, VOPO4∙2H2O's capacity of hosting Zn2+fades precipitously over tens of cycles. VOPO4∙2H2O stores Fe2+with a unique mechanism, where upon contacting the electrolyte by the VOPO4∙2H2O electrode, Fe2+ions from the electrolyte get oxidized to Fe3+ions that are inserted and trapped in the VOPO4∙2H2O structure in an electroless redox reaction. The trapped Fe3+ions, thus, bolt the layered structure of VOPO4∙2H2O, which prevents it from dissolution into the electrolyte during (de)insertion of Fe2+. The findings offer a new strategy to use a redox‐active ion charge carrier to stabilize the layered electrode materials.

     
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  4. Abstract

    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.

     
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  5. Abstract

    A non‐aqueous proton electrolyte is devised by dissolving H3PO4into acetonitrile. The electrolyte exhibits unique vibrational signatures from stimulated Raman spectroscopy. Such an electrolyte exhibits unique characteristics compared to aqueous acidic electrolytes: 1) higher (de)protonation potential for a lower desolvation energy of protons, 2) better cycling stability by dissolution suppression, and 3) higher Coulombic efficiency owing to the lack of oxygen evolution reaction. Two non‐aqueous proton full cells exhibit better cycling stability, higher Coulombic efficiency, and less self‐discharge compared to the aqueous counterpart.

     
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  6. Abstract

    A non‐aqueous proton electrolyte is devised by dissolving H3PO4into acetonitrile. The electrolyte exhibits unique vibrational signatures from stimulated Raman spectroscopy. Such an electrolyte exhibits unique characteristics compared to aqueous acidic electrolytes: 1) higher (de)protonation potential for a lower desolvation energy of protons, 2) better cycling stability by dissolution suppression, and 3) higher Coulombic efficiency owing to the lack of oxygen evolution reaction. Two non‐aqueous proton full cells exhibit better cycling stability, higher Coulombic efficiency, and less self‐discharge compared to the aqueous counterpart.

     
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