Intercalation-type layered oxides have been widely explored as cathode materials for aqueous zinc-ion batteries (ZIBs). Although high-rate capability has been achieved based on the pillar effect of various intercalants for widening interlayer space, an in-depth understanding of atomic orbital variations induced by intercalants is still unknown. Herein, we design an NH 4 + -intercalated vanadium oxide (NH 4 + -V 2 O 5 ) for high-rate ZIBs, together with deeply investigating the role of the intercalant in terms of atomic orbital. Besides extended layer spacing, our X-ray spectroscopies reveal that the insertion of NH 4 + could promote electron transition to 3 d xy state of V t 2 g orbital in V 2 O 5 , which significantly accelerates the electron transfer and Zn-ion migration, further verified by DFT calculations. As results, the NH 4 + -V 2 O 5 electrode delivers a high capacity of 430.0 mA h g −1 at 0.1 A g −1 , especially excellent rate capability (101.0 mA h g −1 at 200 C), enabling fast charging within 18 s. Moreover, the reversible V t 2 g orbital and lattice space variation during cycling are found via ex-situ soft X-ray absorption spectrum and in-situ synchrotron radiation X-ray diffraction, respectively. This work provides an insight at orbital level in advanced cathode materials.

中文翻译：

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插层剂诱导的 V t 2 g 轨道占据氧化钒阴极用于快速充电水性锌离子电池

插层型层状氧化物作为水系锌离子电池（ZIB）的正极材料已被广泛探索。尽管基于各种插层剂的柱效应扩大层间空间已经实现了高速率能力，但对插层剂引起的原子轨道变化的深入理解仍然未知。在这里，我们设计了一个NH4 +-插层氧化钒（NH4 +-V2氧5）用于高速率 ZIB，并深入研究插层剂在原子轨道方面的作用。除了扩展层间距之外，我们的 X 射线光谱显示 NH 的插入4 +可以促进电子跃迁到3dXY V状态t 2 G V 轨道2氧5，显着加速了电子转移和锌离子迁移，并通过 DFT 计算进一步验证。结果，NH4 +-V2氧5电极提供 430.0 mA hg 的高容量−10.1 A g 时−1，特别出色的倍率性能（101.0 mA hg−1200℃），可在18秒内快速充电。此外，可逆Vt 2 G 分别通过异位软X射线吸收光谱和原位同步加速器辐射X射线衍射发现循环过程中轨道和晶格空间的变化。这项工作提供了先进阴极材料轨道水平的见解。