Thanks to low costs and the abundance of the resources, sodium‐ion (SIBs) and potassium‐ion batteries (PIBs) have emerged as leading candidates for next‐generation energy storage devices. So far, only few materials can serve as the host for both Na+ and K+ ions. Herein, a cubic phase CuSe with crystal‐pillar‐like morphology (CPL‐CuSe) assembled by the nanosheets are synthesized and its dual functionality in SIBs and PIBs is comprehensively studied. The electrochemical measurements demonstrate that CPL‐CuSe enables fast Na+ and K+ storage as well as the sufficiently long duration. Specifically, the anode delivers a specific capacity of 295 mA h g−1 at current density of 10 A g−1 in SIBs, while 280 mA h g−1 at 5 A g−1 in PIBs, as well as the high capacity retention of nearly 100% over 1200 cycles and 340 cycles, respectively. Remarkably, CPL‐CuSe exhibits a high initial coulombic efficiency of 91.0% (SIBs) and 92.4% (PIBs), superior to most existing selenide anodes. A combination of in situ X‐ray diffraction and ex situ transmission electron microscopy tests fundamentally reveal the structural transition and phase evolution of CuSe, which shows a reversible conversion reaction for both cells, while the intermediate products are different due to the sluggish K+ insertion reaction.

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Aqueous‐ion batteries have received much attention owing to the merits of high safety, low cost, and environmental friendliness. Among potential cathode candidates, transition metal sulfides drew little attention since they suffer from low capacity, low working potential, and fast capacity fading. Here, advantage is taken of the chemical instability of VS2 in aqueous electrolyte to in situ fabricate a heterostructural VS2/VOx material. Benefiting from the internal electric field at heterointerfaces, high conductivity of vanadium sulfide and high chemical stability of vanadium oxides, heterostructural VS2/VOx delivers an enhanced working potential by 0.25 V, superior rate capability with specific capacity of 156 mA h g−1 at 10 A g−1, and long‐term stability over 3000 cycles as Zn2+ storage electrode. In addition, heterostructural VS2/VOx is employed as the cathode for aqueous NH4+ ion storage with high reversible capacity over 150 mA h g−1 and long lifespan over 1000 cycles, surpassing the state‐of‐the‐art materials. VS2/VOx is proved to demonstrate a (de)intercalation process for Zn2+ storage, while a conversion reaction accompanied by insertion is responsible for nonmetal NH4+. The strong insight obtained in this study sheds light on a new methodology of exploring the potential of transition metal sulfides‐based cathode materials for aqueous ion batteries.

Aqueous zinc‐ion batteries are receiving increasing attention; however, the development of high‐voltage cathodes is limited by the narrow voltage window of conventional aqueous electrolytes. Herein, it is reported that Na3V2(PO4)2O1.6F1.4 exhibits the excellent performance, optimal to date, among polyanion cathode materials in a novel neutral water‐in‐bisalts electrolyte of 25 m ZnCl2 + 5 m NH4Cl. It delivers a reversible capacity of 155 mAh g−1 at 50 mA g−1, a high average operating potential of ≈1.46 V, and stable cyclability of 7000 cycles at 2 A g−1.

Anion storage in cathode of dual-ion batteries provides leeway for new battery chemistries. For high energy density and better safety, it is desirable but challenging to reversibly intercalate chloride in a graphite cathode because either the oxygen or chlorine evolution reaction can prevail over chloride insertion. The primary barrier is the lack of suitable aqueous electrolytes that suppress these parasitic reactions. Herein, we report an aqueous deep eutectic solvent gel electrolyte that allows reversible chloride storage for graphite based on a chloride-based electrolyte via the formation of iodine–chloride interhalogens. The results suggest three reversible steps: iodine plating on the host surface, oxidation to form I-Cl interhalides, and then intercalation into graphite. As a result, the graphite cathode delivers a high reversible capacity of 291 mAh g–1 with stable cycling performance. Facilitated by the same mechanism, a porous graphenic carbon delivered a record-high capacity of over 1100 mAh g–1.