Theoretical study of superionic phase transition in Li2S

Abstract

Abstract We have studied temperature-induced superionic phase transition in Li2S, which is one of the most promising Li-S battery cathode material. Concentration of ionic carriers at low and high temperature was evaluated from thermodynamics of defects (using density functional theory) and detailed balance condition (using ab initio molecular dynamics (AIMD)), respectively. Diffusion coefficients were also obtained using AIMD simulations. Calculated ionic conductivity shows that superionic phase transition occurs at T = 900 K, which is in agreement with reported experimental values. The superionic behavior of Li2S is found to be due to thermodynamic reason (i.e. a large concentration of disordered defects).