Computational studies on ion and electron transfer across the electrode - solid electrolyte interfaces in all-solid-state batteries

Abstract

We have been studying the atomic-scale interface science of Li-ion batteries as well as all-solid-state batteries by DFT first-principles calculations. For the latter target, we have developed a novel method for efficient sampling of heterogeneous interface structures, and applied it to several interfaces between positive electrodes and solid electrolytes. Those applications elucidated the presence of unstable sites for Li around the interfaces, its connection with the dynamical formation of the Li depletion layer as well as the electrolyte oxidation. We have also suggested a useful approach to the annealed state and a universal picture of the standard electrochemical potential of the Li+ ion based on the DFT calculation framework. These findings may give novel insights into the future of battery science and technology.