A major challenge for the commercialization of solid-state batteries with Li-metal anodes is the propagation of Li filaments at high current densities. This work utilizes operando video microscopy to study the dynamic evolution of Li penetration within ceramic solid electrolytes. Four morphology types are identified and studied under a range of battery-relevant conditions. Morphology evolution is linked to electrochemical signatures by synchronizing video microscopy with the voltage response of the cells, providing an avenue for on-board diagnostics. A key observation is the reversible plating and stripping of Li filaments before short-circuiting occurs, indicating that if Li propagation is identified through voltage analysis, catastrophic failure modes could be avoided. These findings represent an important step toward understanding and overcoming the challenge of Li penetration and enabling high-rate-capability Li-metal solid-state batteries for applications such as electric vehicles.
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Kazyak, E., R. Garcia-Mendez, W. S. LePage, A. Sharafi, A. L. Davis, A. J. Sanchez, K.-H. Chen, C. Haslam, J. Sakamoto, N. P. Dasgupta. Li penetration in ceramic solid electrolytes: Operando microscopy analysis of morphology, propagation, and reversibility. Matter 2(4): 1025-48 (2020).