Computational Design of Antiperovskite Solid Electrolytes

In the face of the current climate emergency and the performance, safety, and cost limitations current state-of-art Li-ion batteries present, solid-state batteries are widely anticipated to revolutionize energy storage. The heart of this technology lies in the substitution of liquid electrolytes with solid counterparts, resulting in potential critical advantages, such as higher energy density and safety profiles. In recent years, antiperovskites have become one of the most studied solid electrolyte families for solid-state battery applications as a result of their salient advantages, which include high ionic conductivity, structural versatility, low cost, and stability against metal anodes. This Review highlights the latest progress in the computational design of Li- and Na-based antiperovskite solid electrolytes, focusing on critical topics for their development, including high-throughput screening for novel compositions, synthesizability, doping, ion transport mechanisms, grain boundaries, and electrolyte–electrode interfaces. Moreover, we discuss the remaining challenges facing these materials and provide our perspective on their possible future advances and applications.