Practical Application of Li-Rich Materials in Halide All-Solid-State Batteries and Interfacial Reactions between Cathodes and Electrolytes

Anbang Zhang; Jing Wang; Ruizhi Yu; Haoxiang Zhuo; Changhong Wang; Zhimin Ren; Jiantao Wang

doi:10.1021/acsami.2c21569

Practical Application of Li-Rich Materials in Halide All-Solid-State Batteries and Interfacial Reactions between Cathodes and Electrolytes

ACS Appl Mater Interfaces. 2023 Feb 15;15(6):8190-8199. doi: 10.1021/acsami.2c21569. Epub 2023 Feb 3.

Authors

Anbang Zhang^{1

2

3}, Jing Wang^{1

2

3}, Ruizhi Yu^{4

5}, Haoxiang Zhuo^{1

2

3}, Changhong Wang⁴, Zhimin Ren^{1

2

3}, Jiantao Wang^{1

2

3}

Affiliations

¹ National Power Battery Innovation Center, GRINM Group Co. Ltd., Beijing 100088, P. R. China.
² China Automotive Battery Research Institute Co., Ltd., Beijing 100088, P. R. China.
³ General Research Institute for Nonferrous Metals, Beijing 100088, P. R. China.
⁴ Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario, N6A 5B9, Canada.
⁵ Institute of Micro/Nano Materials and Devices, Ningbo University of Technology, Ningbo, Zhejiang 315211, China.

PMID: 36734587
DOI: 10.1021/acsami.2c21569

Abstract

Benefiting from the advanced solid-state electrolytes (SSEs), conventional cathodes have been widely applied in all-solid-state lithium batteries (ASSLBs). However, Li-rich Mn-based (LRM) cathodes, which possess enhanced discharge capacities beyond 250 mA h g^-1, have not yet been studied in ASSLBs. In this work, the practical application of LRM cathodes in ASSLBs using a high-voltage-stability halide SSE (Li₃InCl₆, LIC) is reported for the first time. Furthermore, we decipher that the active oxygen released from LRM cathodes at a high operation voltage seriously oxidizes the LIC electrolytes, thus resulting in the large interfacial resistance between cathodes and electrolytes and hindering their industrialized application in ASSLBs. Therefore, surface chemistry engineering of LRM cathodes with an ionic conductive coating material of LiNbO₃ (LNO) is employed to stabilize the LRM/LIC interface. Consequently, the LRM-based ASSLBs deliver a high specific capacity of 221 mA h g^-1 at 0.1 C and a decent cycle life of 100 cycles. This contribution gives insights into studying the interfacial issues between LRM cathodes and halide electrolytes and sheds light on the application of LRM cathode materials in ASSLBs.

Keywords: Li-rich Mn-based cathodes; all-solid-state lithium batteries; cathode/electrolyte interface; interfacial engineering; solid-state halide electrolyte.