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Chemical Identification of Catalytically Active Sites on Oxygen‐doped Carbon Nanosheet to Decipher the High Activity for Electro‐synthesis Hydrogen Peroxide
Author(s) -
Chen Shanyong,
Luo Tao,
Chen Kejun,
Lin Yiyang,
Fu Junwei,
Liu Kang,
Cai Chao,
Wang Qiyou,
Li Huangjingwei,
Li Xiaoqing,
Hu Junhua,
Li Hongmei,
Zhu Mingshan,
Liu Min
Publication year - 2021
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.202104480
Subject(s) - nanosheet , catalysis , hydrogen peroxide , chemistry , inorganic chemistry , titration , oxygen , carbon fibers , electrocatalyst , electrochemistry , selectivity , materials science , organic chemistry , electrode , composite number , composite material
Electrochemical production of hydrogen peroxide (H 2 O 2 ) 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 H 2 O 2 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 (OCNS 900 ) catalyst for 2 e − ORR. The OCNS 900 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 H 2 O 2 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.