The solid-solid contact interface is crucial for the reliability of solid-state energy storage systems. The contact condition becomes more complicated when lithium (Li) metal is used as the anode. The contact between solid electrolyte (SE) and Li metal is inferior compared to the liquid/solid interface in conventional Li-ion batteries. Experimental evidence has shown that improper operating conditions of solid-state batteries can lead to electro-chemo-mechanical failures at the Li/SE interface, including the formation of voids and the penetration of Li. In this study, a unified phase-field model is developed to investigate these two mechanisms. The model considers the coupled electro-chemo-mechanical processes including void diffusion, lattice annihilation, stripping and plating reactions, and plastic deformation of Li metal. The study begins with a revisit of the deformation-mechanism map for Li metal under a wide range of temperatures, stress, and deformation rates. This map serves as the basis for the mechanical characterization in the phase-field model. The large inelastic deformation of Li is considered by introducing an advection term into the Allen-Cahn equation, which is used to describe the dynamic evolution of the Li and void phases. The effects of current density and stack pressure on void evolution and Li penetration are studied based on the model predictions. By combining the simulation results with the experimental data from publications, we obtain the stable operation zone of stack pressure and applied current density. In this zone, the Li/SE interface can enable stable stripping and plating of Li metal. The same phase-field modeling framework is transferred to investigate the Li-Mg alloy/SE interface considering Li-Mg alloy is also used as the anode. The fundamental difference between Li/SE and Li-Mg/SE is analyzed accordingly. This study provides a useful tool for the design, manufacturing, and management of next-generation batteries by providing important scientific insights into the electro-chemo-mechanical processes of different anode materials under various operational conditions.
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