Single-atom tailored transition metal oxide enhances d-p hybridization in catalytic conversion for lithium-oxygen batteries

Although the incorporation of d-block single atoms (d-SAs) into TMO is an effective strategy to regulate the intrinsic catalytic function, the comprehensive understanding of the electronic structure of the catalyst and the interaction mechanism with the reaction intermediates is still unclear, making it difficult to design the optimal active site. In this contribution, we establish a clear relationship between the active centers, electronic structure, and oxygen adsorption behavior of the active site. The Nb-SA induce an increase in the energy levels of dx²-y² and effectively activate the redox activity of dx²-y² at Co site, which dramatically optimized the adsorption behavior of key intermediate. Thereby the strong adsorption between the active cations and intermediates promotes uniform nucleation of discharge products, and significantly improve the energy storage performance of Nb-SA@Co₃O₄/h-PANI. The assembled Nb-SA@Co₃O₄-based LOB can operate with low overpotential and long-term cycle stability. Our findings provide insight into electronic structure regulation and activity promotion of efficient catalysts for LOBs.