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 LiNiCoMnO (NCM)|LiPSCl (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 LiZr(PO) (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.
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