Theoretical Calculations Facilitating Catalysis for Advanced Lithium-Sulfur Batteries.

Lithium-sulfur (Li-S) batteries have emerged as one of the most hopeful alternatives for energy storage systems. However, the commercialization of Li-S batteries is still confronted with enormous hurdles. The poor conductivity of sulfur cathodes induces sluggish redox kinetics. The shuttling of polysulfides incurs the heavy failure of electroactive substances. Tremendous efforts in experiments to seek efficient catalysts have achieved significant success. Unfortunately, the understanding of the underlying catalytic mechanisms is not very detailed due to the complicated multistep conversion reactions in Li-S batteries. In this review, we aim to give valuable insights into the connection between the catalyst activities and the structures based on theoretical calculations, which will lead the catalyst design towards high-performance Li-S batteries. This review first introduces the current advances and issues of Li-S batteries. Then we discuss the electronic structure calculations of catalysts. Besides, the relevant calculations of binding energies and Gibbs free energies are presented. Moreover, we discuss lithium-ion diffusion energy barriers and Li