Mesoscale Analysis of Interfacial Stability in Solid-State Batteries

Abstract

The utilization of lithium metal anodes along with inorganic solid electrolytes holds the potential to enhance the energy density, power density and safety of conventional lithium-ion batteries. Despite the theoretical promise of solid electrolytes, the morphological instability of lithium metal anodes during electrochemical operation continues to pose major challenges for the advancement of solid-state batteries. Electrodeposition stability at the solid-solid interface is governed by a wide range of factors including the surface roughness, microstructural arrangement, transport and mechanical properties, relevant to the solid electrolyte and lithium metal. In addition, the competing kinetics of vacancy diffusion and electrochemical reaction alters the metal morphology during discharge and governs the interfacial contact. In this work, a mechanistic understanding of the electrochemical-mechanical interactions underlying the electrodeposition and dissolution stability of lithium metal anodes during fast charge and discharge operation of solid-state batteries will be presented.