A scalable Li-Al-Cl stratified structure for stable all-solid-state lithium metal batteries

Han Su, Jingru Li, Yu Zhong (), Yu Liu, Xuhong Gao, Juner Kuang, Minkang Wang, Chunxi Lin, Xiuli Wang and Jiangping Tu ()
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Han Su: School of Materials Science and Engineering, Zhejiang University
Jingru Li: School of Materials Science and Engineering, Zhejiang University
Yu Zhong: School of Materials Science and Engineering, Zhejiang University
Yu Liu: School of Materials Science and Engineering, Zhejiang University
Xuhong Gao: School of Materials Science and Engineering, Zhejiang University
Juner Kuang: School of Materials Science and Engineering, Zhejiang University
Minkang Wang: School of Materials Science and Engineering, Zhejiang University
Chunxi Lin: School of Materials Science and Engineering, Zhejiang University
Xiuli Wang: School of Materials Science and Engineering, Zhejiang University
Jiangping Tu: School of Materials Science and Engineering, Zhejiang University

Nature Communications, 2024, vol. 15, issue 1, 1-10

Abstract: Abstract Sulfides are promising electrolyte materials for all-solid-state Li metal batteries due to their high ionic conductivity and machinability. However, compatibility issues at the negative electrode/sulfide electrolyte interface hinder their practical implementation. Despite previous studies have proposed considerable strategies to improve the negative electrode/sulfide electrolyte interfacial stability, industrial-scale engineering solutions remain elusive. Here, we introduce a scalable Li-Al-Cl stratified structure, formed through the strain-activated separating behavior of thermodynamically unfavorable Li/Li9Al4 and Li/LiCl interfaces, to stabilize the negative electrode/sulfide electrolyte interface. In the Li-Al-Cl stratified structure, Li9Al4 and LiCl are enriched at the surface to serve as a robust solid electrolyte interphase and are diluted in bulk by Li metal to construct a skeleton. Enabled by its unique structural characteristic, the Li-Al-Cl stratified structure significantly enhances the stability of negative electrode/sulfide electrolyte interface. This work reports a strain-activated phase separation phenomenon and proposes a practical pathway for negative electrode/sulfide electrolyte interface engineering.

Date: 2024
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DOI: 10.1038/s41467-024-48585-7

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