Problems at the Electrolyte-Electrode Interfaces in All-Solid-State Li-Ion Batteries : Insight from First-Principles Computation

All-solid-state batteries using solid electrolyte materials provide intrinsic safety and high energy density. Problems at the interfaces between the electrode and electrolyte materials, such as high interfacial resistance and interfacial degradation, are limiting the development of all-solid-state batteries. Computational modeling based on first principles methods can provide valuable insights into the fundamental mechanisms regarding both thermodynamics and kinetics at the solid interfaces. In this talk, I will present our recent computational study about the solid-solid interfaces in all-solid-state Li-ion batteries. Our first-principles modeling study reveals the compatibility issues of the electrolyte and electrode which lead to the failure of sulfide and oxide solid electrolyte materials. We will also discuss how to resolves these interfacial problems using the insights from first-principles computation.