Boosting Oxygen Reduction for High-Efficiency H₂ O₂ Electrosynthesis on Oxygen-Coordinated CoNC Catalysts

Atomically dispersed CoNC is a promising material for H₂ O₂ selective electrosynthesis via a two-electron oxygen reduction reaction. However, the performance of typical CoNC materials with routine CoN₄ active center is insufficient and needs to be improved further. This can be done by fine-tuning its atomic coordination configuration. Here, a single-atom electrocatalyst (Co/NC) is reported that comprises a specifically penta-coordinated CoNC configuration (OCoN₂ C₂ ) with Co center coordinated by two nitrogen atoms, two carbon atoms, and one oxygen atom. Using a combination of theoretical predictions and experiments, it is confirmed that the unique atomic structure slightly increases the charge state of the cobalt center. This optimizes the adsorption energy towards *OOH intermediate, and therefore favors the two-electron ORR relevant for H₂ O₂ electrosynthesis. In neutral solution, the as-synthesized Co/NC exhibits a selectivity of over 90% over a potential ranging from 0.36 to 0.8 V, with a turnover frequency value of 11.48 s^-1 ; thus outperforming the state-of-the-art carbon-based catalysts.