Rechargeable aqueous Zn-ion batteries (ZiBs) have received significant attention owing to their low cost and environmental friendliness. The charge storage mechanism of ZiBs generally depends on the cationic redox conversion. The anodic redox conversion is still rare due to the lack of suitable cathode materials and electrolytes, which may impede the ZiB performance. The present investigation focuses on enhancing the ZiB performance through in situ involvement of disulfide redox chemistry from a patronite Mn-doped VS₄ crystal in a 1 M Zn(OTf)₂ water/acetonitrile (ACN) hybrid electrolyte. Simultaneous involvement of cationic and anionic redox conversion during the charging/discharging process enhances the specific capacity as high as ∼547 mA h g^–1 at 0.2 A g^–1 current density. The water/ACN hybrid solvent effectively improves the working voltage and suppresses Zn dendrite formation, resulting in superior cycling performance. The conversion of the VS₄ crystal phase and intercalation of H⁺/Zn²⁺ in the cathode have been investigated through ex situ X-ray diffraction, field emission scanning electron microscopy, X-ray photoelectron spectroscopy, and Raman studies.

中文翻译：

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通过硫化钒阴极的结构改性在混合电解质锌离子电池中实现可逆阳极氧化策略

可充电水性锌离子电池（ZiBs）由于其低成本和环境友好性而受到广泛关注。ZiBs 的电荷存储机制通常取决于阳离子氧化还原转化。由于缺乏合适的正极材料和电解质，阳极氧化还原转化仍然很少见，这可能会阻碍 ZiB 的性能。本研究的重点是通过在1 M Zn(OTf) ₂水/乙腈 (ACN) 混合电解质中原位参与二硫化物氧化还原化学反应来提高 ZiB 性能，该化学反应来自掺杂 Mn 的 VS ₄晶体。在充电/放电过程中同时参与阳离子和阴离子氧化还原转化可将比容量提高至~547 mA hg ^–1在 0.2 A g ^–1电流密度下。水/乙腈混合溶剂有效地提高了工作电压并抑制了锌枝晶的形成，从而获得了优异的循环性能。通过非原位X射线衍射、场发射扫描电子显微镜、X射线光电子能谱和拉曼研究，已经研究了VS ₄晶相的转化和H ⁺ /Zn ²⁺在阴极中的嵌入。