Codependent failure mechanisms between cathode and anode in solid state lithium metal batteries: mediated by uneven ion flux

Yue Zheng; Shu Zhang; Jun Ma; Fu Sun; Markus Osenberg; André Hilger; Henning Markötter; Fabian Wilde; Ingo Manke; Zhongbo Hu; Guanglei Cui

doi:10.1016/j.scib.2023.03.021

Codependent failure mechanisms between cathode and anode in solid state lithium metal batteries: mediated by uneven ion flux

Sci Bull (Beijing). 2023 Apr 30;68(8):813-825. doi: 10.1016/j.scib.2023.03.021. Epub 2023 Mar 13.

Authors

Yue Zheng¹, Shu Zhang², Jun Ma³, Fu Sun⁴, Markus Osenberg⁵, André Hilger⁵, Henning Markötter⁶, Fabian Wilde⁷, Ingo Manke⁵, Zhongbo Hu⁸, Guanglei Cui⁹

Affiliations

¹ Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China; College of Materials Science and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 100049, China.
² Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China.
³ Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China; Shandong Energy Institute, Qingdao 266101, China. Electronic address: majun@qibebt.ac.cn.
⁴ Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China. Electronic address: sunfu@qibebt.ac.cn.
⁵ Institute of Applied Materials, Helmholtz-Zentrum Berlin für Materialien und Energie, Berlin 14109, Germany.
⁶ Department of Non-Destructive Testing, Bundesanstalt für Materialforschung und -Prüfung, Berlin 12205, Germany.
⁷ Institute of Materials Physics, Helmholtz-Zentrum Hereon, Geesthacht 21502, Germany.
⁸ College of Materials Science and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 100049, China.
⁹ Qingdao Industrial Energy Storage Research Institute, Qingdao Institute of Bioenergy and Bioprocess Technology, Chinese Academy of Sciences, Qingdao 266101, China; College of Materials Science and Opto-Electronic Technology, University of Chinese Academy of Sciences, Beijing 100049, China; Shandong Energy Institute, Qingdao 266101, China. Electronic address: cuigl@qibebt.ac.cn.

PMID: 36967270
DOI: 10.1016/j.scib.2023.03.021

Abstract

An in-depth understanding of the degradation mechanisms is a prerequisite for developing the next-generation all solid-state lithium metal battery (ASSLMB) technology. Herein, synchrotron X-ray computed tomography (SXCT) together with other probing tools and simulation method were employed to rediscover the decaying mechanisms of LiNi_0.8Co_0.1Mn_0.1O₂ (NCM)|Li₆PS₅Cl (LPSCl)|Li ASSLMB. It reveals that the detachment and isolation of NCM particles cause the current focusing on the remaining active regions of cathode. The extent of Li stripping and the likelihood of Li⁺ plating into LPSCl facing the active NCM particles becomes higher. Besides, the homogeneity of Li stripping/plating is improved by homogenizing the electrochemical reactions at the cathode side by LiZr₂(PO₄)₃ (LZP) coating. These results suggest a codependent failure mechanism between cathode and anode that is mediated by uneven Li ion flux. This work contributes to a holistic understanding of the degradation mechanisms in ASSLMBs and opens new opportunities for their further optimization and development.

Keywords: Cathode deactivation; Codependent failure mechanism; Current density distribution; Lithium ion flux; Solid-state lithium metal batteries.