Triggering Reversible Intercalation‐Conversion Combined Chemistry for High‐Energy–Density Lithium Battery Cathodes

• DOI: 10.1002/adma.202407754
• Publication Date: 2024-10-21T07:02:56Z
• Authors: Jaehoon Heo; Sung‐Kyun Jung; Seungju Yu; Sangwook Han; Jaekyun Yoo; Youngsu Kim; Ho‐Young Jang; Kisuk Kang
• Keywords: Energy transformation; Metastability

Abstract Combining intercalation and conversion reactions maximizes the utilization of redox‐active elements in electrodes, providing a means for overcoming current capacity ceiling. However, integrating both mechanisms within single electrode material presents significant challenges owing to their contrasting structural requirements. Intercalation requires well‐defined host structure efficient lithium‐ion diffusion, whereas entail reorganization, which can undermine capabilities. Based on previous study that successfully demonstrated reversible intercalation–conversion chemistry amorphous LiFeSO4F, this aims provide an in‐depth understanding how be enabled. Experimental theoretical investigations model system based tavorite‐structured LiFeSO4F revealed amorphization governs activation reversibility combined reactions. Enhanced is achieved through facile migration transition metals matrix. Unexpectedly, it found also narrowed voltage gap between This voltage‐gap reduction explained by thermodynamic metastability phase. The applicability approach other hosts further demonstrated, showing enables conversion. These findings suggest new strategy leverages full potential reactions, introducing avenues cathode design.