Metal and Coordinating Atoms Synergistically Achieve\nHigh Activity and Stability in Single-Atom Catalysts within the Framework\nof TM–N<sub>3</sub>X for the Oxygen Evolution Reaction of Lithium\nPeroxide

A critical challenge in the advancement\nof lithium–oxygen\nbatteries (LOBs) is the difficulty in decomposing lithium peroxide,\nleading to high charge overpotentials and poor cycling stability.\nSingle-atom catalysts (SACs), known for their ultrahigh catalytic\nactivity in various electrochemical reactions, are expected to enhance\nthe kinetics of the oxygen evolution reaction (OER) for LOBs. Herein,\n24 SACs within the framework of TM–N<sub>3</sub>X have been\ndesigned and optimized for the OER of lithium peroxide. First-principles\ncalculations reveal that the doped non-metal atom (X = B, C, O, or\nP) significantly contributes to the structural stability of the SACs\nwhile the metal atom (TM = Ru, Os, Rh, Ir, Pd, or Pt) significantly\ninfluences the catalytic activity of the SACs. Upon evaluation of\ntheir stability and catalytic activity, the Pt–N<sub>3</sub>B and Pd–N<sub>3</sub>B catalysts have been identified as\npromising candidates for the OER of lithium peroxide, with theoretical\ncharge overpotentials of 0.19 and 0.18 V, respectively. This work\nprovides new guidance for the design of efficient SACs for LOBs and\ninspires a fundamental understanding of the underlying structure–activity\nrelationship.