Strong Lewis-acid coordinated PEO electrolyte achieves 4.8 V-class all-solid-state batteries over 580 Wh kg−1

作者：Hanwen An, Menglu Li, Qingsong Liu, Yajie Song, Jiaxuan Liu, Zhihang Yu, Xingjiang Liu, Biao Deng, Jiajun Wang · 发表于：Nature Communications · 年份：2024 · DOI：10.1038/s41467-024-53094-8 · 被引用次数：175 · 研究领域：Advancements in Battery Materials、Advanced Battery Materials and Technologies、Advanced battery technologies research

Polyethylene oxide (PEO) based electrolytes critically govern the security and energy density of solid-state batteries, but typically suffer from poor oxidation resistance at high voltages, which limits the energy density of batteries. Here, we report a Lewis-acid coordinated strategy to significantly improve the cyclic stability of 4.8 V-class PEO-based battery. The introduced Mg2+ and Al3+ with strong electron-withdrawing capability weaken the electron density of ether oxygen (EO) chains via chelation in the coordination structure, resulting in a locally limited interaction between the EO chains and the surface of cathodes at high state of charge. The batteries using Lewis-acid coordinated electrolytes and Ni-rich cathodes achieve high voltage stability of 4.8 V over 300 cycles. Further, the realization of industrial-scale electrolyte membranes, and Ah-level pouch cells over 586 Wh kg‒1 with good cyclic stability, suggests the potential of our strategy in practical applications of all-solid-state batteries. This work reports a Lewis-acid coordinated strategy to improve stability of a 4.8 V-class PEO-based battery. The batteries using Lewis-acid coordinated electrolytes and Ni-rich cathodes achieve high voltage stability of 4.8 V over 300 cycles.