Rechargeable aqueous zinc-ion batteries (AZIBs) are tremendously competitive in terms of cost-economy and safe-operation. However, their development is significantly hampered by the lack of stable cathode materials allowing robust zinc-ion diffusion. Herein, it is firstly reported that a facile synthesis V₅S₈ with tunnel-like crystal structure, even in micron-size form, can be investigated as a superior intercalated cathode material for AZIBs, which delievers a high capacity of 240 mAh g⁻¹ at 0.1 A g⁻¹ and a record capacity retention of 94% (182 mAh g⁻¹) after 1000 cycles at a high current density of 10 A g⁻¹. Density functional theory (DFT) calculations show that V₅S₈ has a strong metallic characteristic and an optimal zinc-ion diffusion path with a low hopping energy barrier, boosting the distinctly fast transport capability of both electrons and ions. Consequently, an unprecedented rate capacity retention of 80.75% was obtained when the current density underwent a hundred-fold change, and the ultrafast ion migration kinetics along with desirable pseudocapacitive behaviors were further confirmed. Moreover, using in-situ synchrotron X-ray diffraction, ex-situ X-ray photoelectron spectroscopy, and DFT calculations, this study provides significant insight into the reaction mechanism of the V₅S₈ cathode with self-adaptive multistage ion storage.

可充电水性锌离子电池 (AZIB) 在成本经济和安全运行方面极具竞争力。然而，由于缺乏稳定的阴极材料，可以实现强大的锌离子扩散，这大大阻碍了它们的发展。在此，首次报道了具有隧道状晶体结构的容易合成的 V ₅ S ₈，即使是微米级的形式，也可以作为 AZIBs 的优质插层正极材料进行研究，其提供 240 mAh g ^-的高容量^{- 1}在 0.1 A g ^-1和 94% (182 mAh g ^-1 )的记录容量保持率在 10 A g ^-1的高电流密度下循环 1000 次后。密度泛函理论 (DFT) 计算表明 V ₅S ₈具有很强的金属特性和最佳的锌离子扩散路径，具有低跳跃能垒，显着提高了电子和离子的快速传输能力。因此，当电流密度发生一百倍变化时，获得了前所未有的 80.75% 的倍率容量保持率，并且进一步证实了超快离子迁移动力学以及理想的赝电容行为。此外，该研究使用原位同步加速器 X 射线衍射、异位X 射线光电子能谱和 DFT 计算，为了解具有自适应多级离子存储的 V ₅ S ₈阴极的反应机理提供了重要见解。