Synergistic dual atomic sites with localized electronic modulation enable high-performance lithium–oxygen batteries

Lithium-oxygen batteries (LOBs) are recognized as promising candidates for next-generation energy storage system technologies due to their high theoretical energy density. Unfortunately, some fundamental issues still constrain the practical implementation of LOBs, including large overpotential, cathode clogging, and poor long-term stability, mainly due to the slow cathodic reaction kinetics. Therefore, the successful construction of rational catalysts becomes an urgent demand for the development of LOBs. Herein, Ni and Mn co-doped MoS₂ (Ni/Mn-MoS₂) is fabricated via a facile one-pot hydrothermal method and employed as an efficient cathode catalyst for LOBs. The electrochemical results show that the as-prepared Ni/Mn-MoS₂ cathode catalyst exhibits low overpotential with a potential gap of 0.78 V, large discharge capacity of 28,195 mAh g⁻¹ at a current density of 100 mA g⁻¹, and enhanced rate capability. The theoretical calculations further reveal that the synergistic effect of Ni and Mn dual atomic sites modulates the electronic structure of catalyst surface, and then enhances the adsorption energy of intermediate product LiO₂ and significantly reduces the overpotential for the formation/decomposition of the amorphous discharge product, thereby accelerating the reaction kinetics. This work may provide inspiration for the rational design of MoS₂-based materials as highly efficient electrocatalysts for LOBs.