Layered vanadate cathodes hold promise for aqueous zinc-ion batteries (AZIBs) owing to their multiple redox reactions as well as large interlayer space for Zn²⁺ storage. However, they are limited by vanadium dissolution during cycling, in association with severe capacity fade and unsatisfactory cyclic life. To address this challenge, we herein report a pre-inserted dual-cation vanadate (Na_xZn_yV₃O₈·nH₂O) cathode, which combines the Zn²⁺-reinforced cathode structure with the Na⁺-enlarged lattice distance for fast and stable Zn²⁺ migration. Multiple ex situ analysis found that electrochemically active Zn₃(OH)₂V₂O₇·2H₂O was generated after discharging, and this corresponds to the efficient suppression of vanadium dissolution by strong ionic bonding. As a result, a certain Na_xZn_yV₃O₈·nH₂O cathode having a Na⁺ to Zn²⁺ ratio of 2:1 retains 99.6% of capacity after 418 cycles at 0.1 A g⁻¹, 90.5% after 6000 cycles at 1.0 A g⁻¹, and 96.7% after 9499 cycles at 10.0 A g⁻¹. Our method paves a way for researchers to develop robust cathode materials for ultra-stable AZIBs.

中文翻译：

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通过多个离子键合钒酸盐阴极抑制钒溶解的超稳定锌离子电池

层状钒酸盐阴极因其多重氧化还原反应以及用于 Zn ²⁺存储的大层间空间而有望用于水系锌离子电池 (AZIB)。然而，它们受到循环过程中钒溶解的限制，与严重的容量衰减和不令人满意的循环寿命有关。为了应对这一挑战，我们在此报告了一种预插入双阳离子钒酸盐 (Na _x Zn _y V ₃ O ₈ ·nH ₂ O) 阴极，它结合了 Zn ²⁺增强的阴极结构和 Na ⁺扩大的晶格距离用于快速稳定的 Zn ²⁺迁移。多个异地分析发现，放电后产生电化学活性Zn ₃ (OH) ₂ V ₂ O ₇ ·2H ₂ O，这对应于通过强离子键有效抑制钒溶解。结果，具有2:1的Na ⁺与Zn ^{2+比率的特定Na} _x Zn _y V ₃ O ₈ ·nH ₂ O正极在0.1 A g -1下418次循环后保持99.6%的容量，在0.1 A g ^-1下保持90.5%的容量。在 1.0 A g ^{-1下 6000 次循环，在 10.0 A g -1}下 9499 次循环后为 96.7%. 我们的方法为研究人员开发用于超稳定 AZIB 的坚固阴极材料铺平了道路。