Advanced Computational Methods in Lithium–Sulfur Batteries

Abstract Lithium–sulfur (Li–S) batteries, as one of the most promising “post‐Li‐ion” energy storage devices, encounter several intrinsic challenges: polysulfide dissolution and shuttle effect, poor sulfur utilization, lithiation‐induced sulfur expansion, and lithium dendritic growth. These challenges must be resolved, and the associated mechanisms must be completely understood before the practical applications of Li–S batteries. Despite significant progress in enhancing battery capacities, experimental studies on the working mechanisms of Li–S batteries remain challenging. Alternatively, computational methods are proven useful for understanding Li–S electrochemistry and designing high‐performance Li–S batteries. This review presents recent advances in computational methods (density functional theory, molecular dynamics simulations, and finite element analysis) for Li–S batteries, compares their advantages, and summarizes their favorable applications in addressing the challenges of Li–S batteries. Computational methods should find more applications in the development of Li–S batteries.