Revealing unprecedented cathode interface behavior in all-solid-state batteries with oxychloride solid electrolytes

Feipeng Zhao; Shumin Zhang; Shuo Wang; Carmen M. Andrei; Hui Yuan; Jigang Zhou; Jian Wang; Zengqing Zhuo; Yu Zhong; Han Su; Jung Tae Kim; Ruizhi Yu; Yingjie Gao; Jinghua Guo; Tsun-Kong Sham; Yifei Mo; Xueliang Sun

doi:10.1039/D4EE00750F

Revealing unprecedented cathode interface behavior in all-solid-state batteries with oxychloride solid electrolytes†

Feipeng Zhao,

‡^a Shumin Zhang,‡^a Shuo Wang,^c Carmen M. Andrei,^d Hui Yuan,^de Jigang Zhou,

^f Jian Wang,^f Zengqing Zhuo,

^g Yu Zhong,^h Han Su,^h Jung Tae Kim,

^a Ruizhi Yu,^a Yingjie Gao,^a Jinghua Guo,

^g Tsun-Kong Sham,ⁱ Yifei Mo

^c and Xueliang Sun

*^ab

Author affiliations

* Corresponding authors

^a Department of Mechanical and Materials Engineering, Western University, London, ON, Canada
E-mail: xsun9@uwo.ca

^b Eastern Institute for Advanced Study, Eastern Institute of Technology, Ningbo, Zhejiang 3150200, P. R. China

^c Department of Materials Science and Engineering, University of Maryland, College Park, MD 20742, USA

^d Canadian Centre for Electron Microscopy, McMaster University, Hamilton, ON, Canada

^e Department of Materials Science and Engineering, McMaster University, Hamilton, ON, Canada

^f Canadian Light Source Inc., University of Saskatchewan, Saskatoon, SK, Canada

^g Advanced Light Source, Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA

^h State Key Laboratory of Silicon Materials, Key Laboratory of Advanced Materials and Applications for Batteries of Zhejiang Province, School of Materials Science & Engineering, Zhejiang University, Hangzhou 310027, China

ⁱ Department of Chemistry, Western University, London, ON, Canada

Abstract

All-solid-state lithium batteries (ASSLBs) are highly desirable for their sustainability, enhanced safety, and increased energy densities. The compatibility between cathodes and solid electrolytes (SEs) is critical for ASSLB electrochemical performance. While the conventional LiCoO₂ (LCO) cathode shows structural stability, limitations in the energy density and materials cost prompt exploration of Ni-rich, Co-poor cathodes like lithium nickel cobalt manganese oxide (NCM). However, Ni-rich NCM faces challenges with typical solid electrolytes (e.g., sulfides or oxides), hindering high-energy-density ASSLBs. Our study reveals a unique cathode/electrolyte interface behavior with lithium tantalum oxychloride (LTOC) superionic conductors, favoring Co-less, Ni-rich NCM over LCO. The Ta/Co interaction is identified as a failure mechanism for LTOC/LCO, while a kinetically stabilized interface is achieved with lean-Co cathodes. Beyond the cathode material composition, our study also establishes a correlation between the temperature used for battery testing and both interface reactivity and cell performance. This research provides crucial insights into the innovative design of high-performance ASSLBs based on the promising LTOC oxychloride SEs.

Energy & Environmental Science

Revealing unprecedented cathode interface behavior in all-solid-state batteries with oxychloride solid electrolytes†

Abstract

Supplementary files

Article information

Download Citation

Permissions

Revealing unprecedented cathode interface behavior in all-solid-state batteries with oxychloride solid electrolytes

Social activity

Search articles by author

Spotlight

Advertisements