Volume 21, Issue 14 2412647
Research Article

A Pre-Oxidation Strategy to Establish Stable Oxide Cathode/Halide Solid-State Electrolyte Interfaces for High Energy all Solid-State Batteries

Hanzhou Liu

Hanzhou Liu

School of Metallurgy and Environment, Central South University, Changsha, 410083 P. R. China

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Yang Lu

Corresponding Author

Yang Lu

School of Metallurgy and Environment, Central South University, Changsha, 410083 P. R. China

E-mail: [email protected]; [email protected]

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Yanchen Liu

Yanchen Liu

School of Metallurgy and Environment, Central South University, Changsha, 410083 P. R. China

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Shenghao Jing

Shenghao Jing

School of Metallurgy and Environment, Central South University, Changsha, 410083 P. R. China

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Zongliang Zhang

Zongliang Zhang

National Energy Metal Resources and New Materials Key Laboratory, Central South University, Changsha, 410083 P. R. China

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Siliang Liu

Siliang Liu

Hunan Provincial Key Laboratory of Nonferrous Value-added Metallurgy, Changsha, 410083 P. R. China

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Yang Liu

Yang Liu

Hunan Energy Frontiers New Materials Technology Co., Ltd., Changsha, 410083 P. R. China

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Yongle Chen

Yongle Chen

Hunan Energy Frontiers New Materials Technology Co., Ltd., Changsha, 410083 P. R. China

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Kun Zhang

Kun Zhang

GEM Co., Ltd, Shenzhen, 518100 P. R. China

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Shuo Yin

Shuo Yin

CNGR Advanced Material Co., Ltd, Tongren, 554300 P. R. China

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Fanqun Li

Fanqun Li

Wanxiang One two Three Co., Ltd., Hangzhou, 311200 P. R. China

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Fangyang Liu

Corresponding Author

Fangyang Liu

School of Metallurgy and Environment, Central South University, Changsha, 410083 P. R. China

E-mail: [email protected]; [email protected]

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First published: 28 February 2025

Abstract

All-solid-state lithium metal batteries (ASSLBs) are promising for high energy and safety. Halide-based solid-state electrolytes, characterized by high ionic conductivity and a notably wide electrochemical window exceeding 4.3 V, hold significant promise for compatibility with high-energy cathodes. However, oxygen in cathodes exhibits a strong tendency to interact with the central metal cation in halide solid-state electrolyte, forming an unstable cathode-electrolyte interface (CEI) and leading to cathodic degradations. Herein, a pre-oxidation strategy is proposed for Y based halide solid-state electrolytes, leveraging oxygen to pre-establish robust Y─O bonds within the halide electrolyte structure Li2YCl2.5Br1.5O0.5 (2LO-0.5). The robust Y─O bonds in 2LO-0.5 effectively hinder uncontrolled oxygen interactions with Y3⁺, which would otherwise lead to the formation of oxidizable YOCl. This stabilization promotes the formation of a thin, stable Y₂O₃-based CEI against LiNi0.83Co0.11Mn0.06O2 (NCM83). Therefore, the ASSLB assembled with 2LO-0.5 and NCM83 demonstrates an initial discharge-specific capacity of 208 mAh g−1 and retained 80.6% of its capacity after 1000 cycles, attributed to stable CEI film derived from pre-oxidized strategy. This work offers new insights for regulating the non-redox reaction between halide solid-state electrolytes and oxide cathodes, promoting the rational design of high-performance halide solid-state electrolytes.

Conflict of Interest

The authors declare no conflict of interest.

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

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