Intrinsic Regularity of Catalytic Cobalt Chalcogenides in Lithium‐Sulfur Battery: Theoretical Study Delivers New Insights

Cobalt chalcogenides CoX2 (X=S, Se, Te) render great performance of lithium‐sulfur batteries based on catalytic capacity to alleviate shuttle effect. Given that S/Se/Te belong to the same main group, the outstanding cycling stability delivered by CoTe2 aroused the curiosity about the uniqueness of CoTe2 and intrinsic laws of cobalt chalcogenide. Herein, comprehensive theoretical study delivers new insights into the intrinsic laws of CoX2: the relative vertical distance of two X atomic layers (rather than atom electronegativity) mainly controls adsorption; CoX2 mainly regulates the charging process (rather than discharging process) thus contributes to great cycling stability. On this basis, the advantages of CoTe2 are three‐fold: moderate polysulfide adsorption, facile ion transport capacity, and surprisingly great promotion of charging process. It is hope the results will facilitate the development of cobalt chalcogenides, especially tellurides as catalytic material in lithium sulfur batteries. Theoretical study delivers new insights into catalytic cobalt chalcogenides CoX2 (X=S, Se, Te) in lithium‐sulfur battery. The polysulfides adsorption is mainly controled by relative vertical distance of two X atomic layers (rather than atom electronegativity). The charging process (rather than discharging process) is mainly regulated to contribute to steady polysulfides conversion.