Lithium Metal Anodes: Advancing our Mechanistic Understanding of Cycling Phenomena in Liquid and Solid Electrolytes.

Lithium metal anodes have the potential to be a disruptive technology for next-generation batteries with high energy densities, but their electrochemical performance is limited by a lack of fundamental understanding into the mechanistic origins that underpin their poor reversibility, morphological evolution (including dendrite growth), and interfacial instability. The goal of this perspective is to summarize the current state-of-the-art understanding of these phenomena, and highlight knowledge gaps where additional research is needed. The various stages of cycling are described sequentially, including nucleation, growth, open-circuit rest periods, and electrodissolution (stripping). A direct comparison of lessons learned from liquid and solid-state electrolyte systems is made throughout the discussion, providing cross-cutting insights between these research communities. Major themes of the discussion include electro-chemo-mechanical coupling, insights from in situ/operando analysis, and the interplay between experimental observations and computational modeling. Finally, a series of fundamental research questions are proposed to identify critical knowledge gaps and inform future research directions.