When a more electrophilic O atom Table ). Upon altering the coordination environment, a redistribution of electronic density occurs around the Ni center (Fig. ). Introducing Au nanoparticles onto the simulated Ni-N-O-C structure (Fig. ) resulted in Ni center displacement from the N-C plane (0.25 Å) with further elongated Ni-N and Ni-O bonds (Supplementary Table ) and the electron transfers from the Au particles to Ni single atom (Supplementary Table ). Subsequently, the distorted geometric out-of-plane configuration, coupled with electronic interactions, will create a novel electron tug effect around local structure. This effect, in turn, will instigate the refinement of