Lithium-Ion Transport through Complex Interphases in Lithium Metal Batteries

Lithium metal is one of the best anode candidates for next-generation batteries. However, there are still many unknowns regarding the structure and properties of the solid electrolyte interphase (SEI) formed due to electron transfer reactions between the Li metal surface and the electrolyte. In addition, because of the difficulties to study amorphous and dynamic phases and interphases, there are many questions about the ion diffusion mechanism through complex multicomponent materials and interphases. In this study, using first-principles theory and computation, we focus on developing a better understanding of the ion motion mechanisms in the vicinity of a SEI formed when a seed Li₂O or LiOH cluster nucleates on the Li metal surface. We study the role of charge transfer at the interface between charged surfaces and the electrolyte, and we investigate the evolution of inhomogeneous Li metal deposits present in the neighborhood of the SEI nuclei, aiming to fundamentally understand how these events modify the ion transport through complex electrochemically active materials.