Computation-aided design of oxygen-ligand-steered single-atom catalysts: Sewing unzipped carbon nanotubes

Single-atom catalysts (SACs), among which nitrogen-doped graphene-supported SACs are successful models, have been extensively investi-gated for electrocatalysts. Although oxygen is a common impurity in graphene, metal-oxygen-based SACs are unutilized. Here, we devise a new type of oxygen-coordinated SAC (M-O-C) with a computation -aided approach. Theoretical modeling predicts that the metal atoms are strongly immobilized by carbonyl ligands in unzipped carbon nano -tubes, and then the Ni-O-C SAC is synthesized for the oxygen evolution reaction (OER). It shows excellent OER activity with a low overpotential (228/325 mV at 10/100 mA cm -2), small Tafel slope (36 mV per decade), and long-term durability over 150 h. We find that the highly electronegative oxygen ligand deviates from the conventional linear scaling relationship by shifting toward a more reactive region, so the inductive effect of the oxygen ligand leads to superior OER activity. This "theory first followed by experiment"strategy would help in the design of various SACs.