Universal‐Descriptors‐Guided Design of Single Atom Catalysts toward Oxidation of Li2S in Lithium–Sulfur Batteries

Abstract The sulfur redox kinetics critically matters to superior lithium–sulfur (Li–S) batteries, for which single atom catalysts (SACs) take effect on promoting Li 2 S redox process and mitigating the shuttle behavior of lithium polysulfide (LiPs). However, conventional trial‐and‐error strategy significantly slows down the development of SACs in Li–S batteries. Here, the Li 2 S oxidation processes over MN 4 @G catalysts are fully explored and energy barrier of Li 2 S decomposition ( E b ) is identified to correlate strongly with three parameters of energy difference between initial and final states of Li 2 S decomposition, reaction energy of Li 2 S oxidation and LiS bond strength. These three parameters can serve as efficient descriptors by which two excellent SACs of MoN 4 @G and WN 4 @G are screened which give rise to E b values of 0.58 and 0.55 eV, respectively, outperforming other analogues in adsorbing LiPs and accelerating the redox kinetics of Li 2 S. This method can be extended to a wider range of SACs by coupling MN 4 moiety with heterostructures and heteroatoms beyond N where WN 4 @G/TiS 2 heterointerface is predicted to exhibit enhanced catalytic performance for Li 2 S decomposition with E b of 0.40 eV. This work will help accelerate the process of designing a wider range of efficient catalysts in Li–S batteries and even beyond, e.g. alkali‐ion‐Chalcogen batteries.