Boosting Oxygen Reduction for High‐Efficiency H<sub>2</sub>O<sub>2</sub> Electrosynthesis on Oxygen‐Coordinated CoNC Catalysts
Hangjia Shen, Nianxiang Qiu, Liu Yang, Xuyun Guo, Kun Zhang, Tiju Thomas, Shiyu Du, Qifu Zheng, J. Paul Attfield, Ye Zhu, Minghui Yang
Abstract
Abstract Atomically dispersed CoNC is a promising material for H 2 O 2 selective electrosynthesis via a two‐electron oxygen reduction reaction. However, the performance of typical CoNC materials with routine CoN 4 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 CoNC configuration (OCoN 2 C 2 ) 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 H 2 O 2 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.