Tuning nickel single-atom coordination in ternary N-, P-, and S-doped graphene for improved Li–O2 batteries

Abstract

The precise engineering of heteroatom coordination environments in single-atom catalysts (SACs) is pivotal for enhancing their catalytic activity. However, the mechanistic interplay between the coordination structure and performance in lithium oxygen batteries (LOBs) remains poorly understood. To address this, we developed a porous Ni SAC with an asymmetric N, P, and S tri-doped coordination, synthesized via a one-pot strategy that enabled the precise tailoring of the first coordination shell. By constructing high-coordination asymmetric geometry, this approach optimizes electronic redistribution and active-site accessibility, offering a versatile pathway to amplify the catalytic efficiency of SACs while providing atomistic insights into coordination–environment–performance relationships. The resulting NiNPSG SAC demonstrated remarkable bifunctional activity, as indicated by its elevated discharge/charge capacities and prolonged cycle stability. This study enhances the rational design of asymmetric SACs via multi-heteroatom coordination and establishes a scalable synthesis method for next-generation catalysts, providing a transformative solution to the ongoing issues of energy efficiency and durability in metal–air battery systems.