All-solid-state sodium batteries (ASSBs) have attracted ever-increasing attention due to their enhanced safety, high energy density, and the abundance of raw materials. One of the remaining key issues for the practical ASSB is the lack of good superionic and electrochemical stable solid-state electrolytes (SEs). Design and manufacturing specific functional materials used as high-performance SEs require an in-depth understanding of the transport mechanisms and electrochemical properties of fast sodium-ion conductors on an atomic level. On account of the continuous progress and development of computing and programming techniques, the advanced computational tools provide a powerful and convenient approach to exploit particular functional materials to achieve that aim. Herein, this review primarily focuses on the advanced computational methods and ion migration mechanisms of SEs. Second, we overview the recent progress on state-of-the-art solid sodium-ion conductors, including Na-β-alumina, sulfide-type, NASICON-type, and antiperovskite-type sodium-ion SEs. Finally, we outline the current challenges and future opportunities. Particularly, this review highlights the contributions of the computational studies and their complementarity with experiments in accelerating the study progress of high-performance sodium-ion SEs for ASSBs.
Keywords: ab initio calculations; all-solid-state sodium batteries; computational auxiliary; ion transport mechanisms; molecular dynamics simulations; nanoscale insight; sodium-ion conductor; sodium-ion solid-state electrolytes.