Theoretical calculations and simulations power the design of inorganic solid-state electrolytes

Using solid-state electrolytes (SSEs) to build batteries helps improve the safety and lifespan of batteries, making it crucial to deeply understand the fundamental physical and chemical properties of SSEs. Theoretical calculations based on modern quantum chemical methods and molecular simulation techniques can explore the relationship between the structure and performance of SSEs at the atomic and molecular levels. In this review, we first comprehensively introduce theoretical methods used to assess the stability of SSEs, including mechanical, phase, and electrochemical stability, and summarize the significant progress achieved through these methods. Next, we outline the methods for calculating ion diffusion properties and discuss the advantages and limitations of these methods by combining the diffusion behaviors and mechanisms of ions in the bulk phase, grain boundaries, and electrode-solid electrolyte interfaces. Finally, we summarize the latest research progress in the discovery of high-quality SSEs through high-throughput screening and machine learning and discuss the application prospects of a new mode that incorporates machine learning into high-throughput screening. With increasing computational capabilities and ongoing methodological innovations, theoretical calculation and simulations will play a more significant role in the design and development of high-performance energy storage materials.