Advanced computational methods in lithium-sulfur batteries

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. (© 2024 Wiley‐VCH GmbH)