Chemical Identification of Catalytically Active Sites on Oxygen-doped Carbon Nanosheet to Decipher the High Activity...

Electrochemical production of hydrogen peroxide (H₂ O₂ ) through two-electron (2 e^- ) oxygen reduction reaction (ORR) is an on-site and clean route. Oxygen-doped carbon materials with high ORR activity and H₂ O₂ selectivity have been considered as the promising catalysts, however, there is still a lack of direct experimental evidence to identify true active sites at the complex carbon surface. Herein, we propose a chemical titration strategy to decipher the oxygen-doped carbon nanosheet (OCNS₉₀₀ ) catalyst for 2 e^- ORR. The OCNS₉₀₀ exhibits outstanding 2 e^- ORR performances with onset potential of 0.825 V (vs. RHE), mass activity of 14.5 A g^-1 at 0.75 V (vs. RHE) and H₂ O₂ production rate of 770 mmol g^-1  h^-1 in flow cell, surpassing most reported carbon catalysts. Through selective chemical titration of C=O, C-OH, and COOH groups, we found that C=O species contributed to the most electrocatalytic activity and were the most active sites for 2 e^- ORR, which were corroborated by theoretical calculations.