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

Hanwen An, Menglu Li, Qingsong Liu, Yajie Song, Jiaxuan Liu, Zhihang Yu, Xingjiang Liu (), Biao Deng and Jiajun Wang ()
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Hanwen An: Harbin Institute of Technology
Menglu Li: Harbin Institute of Technology
Qingsong Liu: Harbin Institute of Technology
Yajie Song: Harbin Institute of Technology
Jiaxuan Liu: Harbin Institute of Technology
Zhihang Yu: Tianjin Institute of Power Sources
Xingjiang Liu: Tianjin Institute of Power Sources
Biao Deng: 239 Zhangheng Road
Jiajun Wang: Harbin Institute of Technology

Nature Communications, 2024, vol. 15, issue 1, 1-12

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41467-024-53094-8

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