All-solid-state battery based on Li metal anode is a promising next-generation energy storage system, but is currently limited by low current density and short cycle life. Further research to improve Li metal anode is impeded by the lack of understanding in its failure mechanisms at lithium-solid interfaces, in particular the fundamental atomistic processes responsible for interface failure. Here, using large-scale molecular dynamics simulations, we perform the first atomistic modeling study of lithium stripping and plating on solid electrolyte by explicitly considering key fundamental atomistic processes and interface atomistic structures. In our simulations, we directly observe the interface failure initiated with the formation of nano-sized pores, and how interface structures, lithium diffusion, adhesion energy, and applied pressure affect interface failure during Li cycling. By systematically varying the parameters of solid-state lithium cells in our simulations, we map the parameter space of applied pressures and interfacial adhesion energies that inhibit interface failure during cycling to guide selection of solid-state cells. Our study establishes the atomistic modeling for Li stripping and plating, and predicts optimal solid interfaces and new strategies for the future research and development of solid-state Li-metal batteries.

Understanding interfacial atomistic mechanisms of lithium metal stripping and plating in solid-state batteries

ACS Spring Meeting 2021

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