Mesoscale Interfacial Interactions in All-Solid-State Lithium Batteries

Abstract

All-solid-state batteries comprising of a lithium metal anode are promising next-generation energy storage systems, capable of providing enhanced safety and delivering high power and energy densities. Despite the inherent mechanical rigidity of solid electrolytes, the irregular nature of electrodeposition at the metal anode remains unresolved and thereby necessitates a detailed description of the mechanisms underlying the interfacial instability. The morphological evolution of the metal anode is influenced by various factors including the mechanical properties of lithium and solid electrolyte, presence of interfacial roughness, grain boundaries in the solid electrolyte microstructure and external operating conditions. In this work, the fundamental electrochemical-mechanical interactions governing the electrodeposition stability at the solid-solid interface, especially the role of grain boundaries will be examined in detail.