Mechanical failure of garnet electrolytes during Li electrodeposition observed by in-operando microscopy

Metallic Li anodes are key to reaching high energy densities in next-generation solid-state batteries, however, major problems are the non-uniform deposition of Li at the interface and the penetrative power of Li metal during operation, which cause failure of the ceramic electrolyte, internal short-circuits and a premature end of battery life. In this work, we explore the anode-electrolyte interface instability of a Li metal-garnet electrolyte system during Li electrodeposition, and its implications for mechanical fracture, Li metal propagation, and electrolyte failure. The degradation mechanism was followed step-by-step during in-operando electrochemical cycling using optical and scanning electron microscopy. High amounts of Li electrodeposition in a localized zone of the interface lead to ceramic fracture followed by an electrode-to-electrode electrical connection via a conductor Li metal filament. This work enables deeper understanding of battery failure modes in all-solid-state batteries containing a ceramic electrolyte membrane.