Theoretical study of highly efficient VS2-based single-atom catalysts for lithium–sulfur batteries

Lithium-sulfur (Li-S) batteries have become a research hotspot due to their high energy density. However, they also have certain disadvantages and limitations. To enhance the performance of Li-S batteries, this study focuses on the utilization of transition metal (TM)-embedded vanadium disulfide (VS₂) materials as cathode catalysts. Using density functional theory (DFT), comprehensive calculations and atomic-level screening of ten TM atoms were conducted to understand the underlying mechanisms and explore the potential of TM@VS₂ catalysts for enhancing battery performance. The computational results indicate that five selected catalysts possess sufficient bonding strength towards high-order lithium polysulfide intermediates by the formation of a significant covalent bond between S atoms in Li₂S_n and TM atoms, thereby effectively suppressing the shuttle effect. The Ni@VS₂ catalyst can effectively decrease the decomposition energy barrier of Li₂S in the charge reaction and can have an optimal Gibbs free energy at the rate-determining step among TM@VS₂ catalysts for the discharge reaction. This study elucidates the mechanism of VS₂-based transition-metal single-atom catalysts and provides an effective reference for the anchoring of TM atoms on other materials.