插层(化学)
材料科学
阴极
锂(药物)
无定形固体
电池(电)
氧化还原
能量转换效率
能量转换
亚稳态
电极
纳米技术
化学工程
化学物理
无机化学
化学
光电子学
物理化学
热力学
结晶学
功率(物理)
有机化学
内分泌学
工程类
冶金
物理
医学
作者
Jaehoon Heo,Sung‐Kyun Jung,Seungju Yu,Sang-Wook Han,Jaekyun Yoo,Youngsu Kim,Ho‐Young Jang,Kisuk Kang
标识
DOI:10.1002/adma.202407754
摘要
Abstract Combining intercalation and conversion reactions maximizes the utilization of redox‐active elements in electrodes, providing a means for overcoming the current capacity ceiling. However, integrating both mechanisms within a single electrode material presents significant challenges owing to their contrasting structural requirements. Intercalation requires a well‐defined host structure for efficient lithium‐ion diffusion, whereas conversion reactions entail structural reorganization, which can undermine intercalation capabilities. Based on the previous study that successfully demonstrated reversible intercalation–conversion chemistry in amorphous LiFeSO4F, this study aims to provide an in‐depth understanding on how this can be enabled. Experimental and theoretical investigations of a model system based on tavorite‐structured LiFeSO4F revealed that amorphization governs the activation and reversibility of the combined reactions. Enhanced reversibility is achieved through the facile migration of transition metals within the amorphous matrix. Unexpectedly, it is found that amorphization also narrowed the voltage gap between the intercalation and conversion reactions. This voltage‐gap reduction is explained by the thermodynamic metastability of the amorphous phase. The applicability of the approach to other intercalation hosts is further demonstrated, showing that amorphization enables reversible intercalation and conversion. These findings suggest a new strategy that leverages the full potential of intercalation and conversion reactions, introducing new avenues for cathode design.
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