Correlating the Interfacial Chemistries With Ion Conduction and Lithium Deactivation in Hybrid Solid Electrolytes

作者：Tianyu Wang, Tengfei Xu, Miao Zhang, Ouwei Sheng, Xiang Li, Zheng Zhang, Chengbin Jin · 发表于：Energy & environment materials · 年份：2026 · DOI：10.1002/eem2.70196 · 被引用次数：1 · 研究领域：Advanced Battery Materials and Technologies、Advancements in Battery Materials、Extraction and Separation Processes

Inactive lithium (dead Li) is the key factor leading to the performance degradation of solid‐state Li metal batteries. Such a deactivated material comprises a useless solid–electrolyte interphase and electrically or ionically isolated Li 0 debris. Dead Li exists at both the “extrinsic” Li/electrolyte and intrinsic electrolyte/electrolyte interfaces and is associated with the ion transport behavior at such interfaces. Herein, we evaluate the different interfacial structures and compositions in a prototype poly(ethylene oxide)–Li 4 SnS 4 hybrid electrolyte and clarify its influence on Li deactivation suppression. Cryotransmission electron microscopy reveals that the intrinsic interface between poly(ethylene oxide) and Li 4 SnS 4 is mainly composed of Li 2 S and Li 2 CO 3 . Notably, the extrinsic interface at Li and poly(ethylene oxide)–Li 4 SnS 4 contains extra Li 2 S and reduced Li 2 O compared with poly(ethylene oxide) electrolyte. The increase of low energy barrier Li 2 S (0.13 eV) components significantly accelerates the interfacial ion migration and reduces the content of dead Li (10.6%). The optimized interface enables the Li || Li cell to operate stably for over 3000 h. This work by interface regulation reduces the formation of electron‐ and ion‐isolated dead Li in solid‐state Li metal batteries, which is of reference significance for the design of dead Li suppression or activation strategies in solid‐state Li metal battery systems.