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Spectroscopic Identification of Active Sites of Oxygen‐Doped Carbon for Selective Oxygen Reduction to Hydrogen Peroxide

2023; Wiley; Volume: 62; Issue: 21 Linguagem: Inglês

10.1002/anie.202303525

1521-3773

Longxiang Liu, Liqun Kang, Arunabhiram Chutia, Jianrui Feng, Martyna Michalska, Pilar Ferrer, David C. Grinter, Georg Held, Yeshu Tan, Fangjia Zhao, Fei Guo, David G. Hopkinson, Christopher S. Allen, Yanbei Hou, Junwen Gu, Ioannis Papakonstantinou, Paul R. Shearing, Dan J. L. Brett, Ivan P. Parkin, Guanjie He,

CO2 Reduction Techniques and Catalysts

Abstract The electrochemical synthesis of hydrogen peroxide (H 2 O 2 ) via a two‐electron (2 e − ) oxygen reduction reaction (ORR) process provides a promising alternative to replace the energy‐intensive anthraquinone process. Herein, we develop a facile template‐protected strategy to synthesize a highly active quinone‐rich porous carbon catalyst for H 2 O 2 electrochemical production. The optimized PCC 900 material exhibits remarkable activity and selectivity, of which the onset potential reaches 0.83 V vs. reversible hydrogen electrode in 0.1 M KOH and the H 2 O 2 selectivity is over 95 % in a wide potential range. Comprehensive synchrotron‐based near‐edge X‐ray absorption fine structure (NEXAFS) spectroscopy combined with electrocatalytic characterizations reveals the positive correlation between quinone content and 2 e − ORR performance. The effectiveness of chair‐form quinone groups as the most efficient active sites is highlighted by the molecule‐mimic strategy and theoretical analysis.