Progress in Theoretical Calculation and Simulation of Sulfide Solid Electrolytes and Their Application in All-Solid-State Batteries

Along with the development of electric vehicles and electronic devices, all-solid-state batteries (ASSBs) have become the next-generation energy storage batteries, owing to their safety and chemical stability. Sulfide Solid Electrolytes (SSEs) are deemed to be crucial materials for ASSBs because of their ultrahigh ionic conductivity (10−3–10−2 S cm−1), but are still plagued by the narrow electrochemical window and poor interfacial stability. In this paper, we summarize our systematic research progress on sulfide SSEs from the view of how theoretical calculations and simulations play a crucial role in material design. First-principles calculation gives evidence of the structure’s stability and ion migration mechanism for electrolytes, MD and AIMD simulations provide insights for the dynamic diffusion behavior and the interface reaction mechanism. High-throughput screening and machine learning have accelerated new electrolyte designs. Scientists discovered Li10GeP2S12 and explored ion dynamics in a crystal lattice of that material. There are also material interface phenomena such as space charge layers and chemical breakdown. These problems can be managed by developing and tuning appropriate computational models to steer material doping and protective layer design. In this paper, we demonstrate that the combination of computer simulations and real experiments is valuable.