Spectroscopic identification of active sites of oxygen-doped carbon for selective oxygen reduction to hydrogen peroxide

Journal article

The electrochemical synthesis of hydrogen peroxide (H₂O₂) 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 H₂O₂ electrochemical production. The optimized PCC₉₀₀ 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 H₂O₂ 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.

Authors: Liu, L; Kang, L; Chutia, A; Feng, J; Michalska, M

• Publication status: Published
• Peer review status: Peer reviewed
• Publisher: Wiley
• Journal: Angewandte Chemie International Edition
• Volume: 62
• Issue: 21
• Article number: e202303525
• Place of publication: Germany
• Publication date: 2023-04-18
• Acceptance date: 2023-03-16
• DOI: 10.1002/anie.202303525
• EISSN: 1521-3773
• ISSN: 1433-7851
• Pmid: 36929681
• Language: English
• Keywords: porous carbon; NEXAFS; quinone; electrocatalysis; hydrogen peroxide; FFR