Mesoscopic Modelling of Li Deposition in Sulfide-Based Solid Electrolyte Using Two-Dimensional Artificial Polycrystal Structure

Abstract Understanding Li nucleation and growth mechanism during charging in solid electrolytes (SEs) is essential in development of all-solid-state batteries with metallic Li, because the Li dendrite could cause internal short-circuit by penetration of SE. However, it is still under debate how the factors including degradation of SE layer, the stacking pressure, and the microstructure affect the Li nucleation and growth in SE. In this study, the coupled current-deposition-stress models using the two-dimensional artificial SE structures have been developed by combination of finite element method and Monte Carlo simulations. The model assumed that Li flux on the SE grain induces an eigen strain in the deposited Li region, and Li grows into the SE layer by breaking grain boundary (GB). Degradation of SE was modelled as the decrease of fracture strength of GB using a coefficient. The effects of these microstructure and operation factors on GB fracture and Li deposition have been evaluated and discussed.