Mesoscale Elucidation of Electrodeposition in All-Solid-State Lithium Batteries

Lithium metal anodes, owing to their theoretical promise have been considered decisive towards the development of next-generation battery systems with higher power and energy densities. Compared to the liquid counterparts, solid electrolytes proffer enhanced safety and dendrite suppression features due to the non-flammability and mechanical stiffness. However, the electrodeposition dynamics at a solid-solid interface is quite intricate, involving coupled transport, mechanical and kinetic processes, which are closely related to the interfacial heterogeneities. Furthermore, the mechanical properties of the solid electrolyte, lithium metal and externally applied pressure influence the mechano-electrochemical interaction and hence the interfacial stability. In this work, a mechanistic understanding of the mesoscale underpinnings in the electrodeposition stability at solid-solid interfaces for all-solid-state lithium batteries will be presented.