Metal and Coordinating Atoms Synergistically Achieve High Activity and Stability in Single-Atom Catalysts within the Framework of TM–N₃X for the Oxygen Evolution Reaction of Lithium Peroxide

A critical challenge in the advancement of lithium-oxygen batteries (LOBs) is the difficulty in decomposing lithium peroxide, leading to high charge overpotentials and poor cycling stability. Single-atom catalysts (SACs), known for their ultrahigh catalytic activity in various electrochemical reactions, are expected to enhance the kinetics of the oxygen evolution reaction (OER) for LOBs. Herein, 24 SACs within the framework of TM-N₃X have been designed and optimized for the OER of lithium peroxide. First-principles calculations reveal that the doped non-metal atom (X = B, C, O, or P) significantly contributes to the structural stability of the SACs while the metal atom (TM = Ru, Os, Rh, Ir, Pd, or Pt) significantly influences the catalytic activity of the SACs. Upon evaluation of their stability and catalytic activity, the Pt-N₃B and Pd-N₃B catalysts have been identified as promising candidates for the OER of lithium peroxide, with theoretical charge overpotentials of 0.19 and 0.18 V, respectively. This work provides new guidance for the design of efficient SACs for LOBs and inspires a fundamental understanding of the underlying structure-activity relationship.