Stability and surface diffusion at lithium-electrolyte interphases with connections to dendrite suppression

TL;DR

This paper investigates the fundamental surface diffusion mechanisms at lithium-electrolyte interfaces using ab initio methods, revealing insights into dendrite suppression strategies for stable lithium metal batteries.

Contribution

It provides the first ab initio analysis of surface diffusion barriers and surface energies at lithium-electrolyte interfaces, linking these to dendrite suppression techniques.

Findings

Surface diffusion plays a key role in dendrite suppression.

Lithium-halide passivating layers reduce dendrite formation.

New pathways for mitigating lithium dendrites are identified.

Abstract

This work presents an ab initio exploration of fundamental mechanisms with direct relevance to dendrite formation at lithium-electrolyte interfaces. Specifically, we explore surface diffusion barriers and solvated surface energies of typical solid-electrolyte interphase layers of lithium metal electrodes. Our results indicate that surface diffusion is an important mechanism for understanding the recently observed dendrite suppression from lithium-halide passivating layers, which were motivated by our previous work. Our results uncover possible mechanisms underlying a new pathway for mitigating dendridic electrodeposition of lithium on metal and thereby contribute to the ongoing efforts to develop stable lithium metal anodes for rechargeable battery systems.