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

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 LiNi0.8Co0.1Mn0.1O2 (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.