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

The electrochemical synthesis of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) via a two-electron (2 e<sup>−</sup>) oxygen reduction reaction (ORR) process provides a promising alternative to replace the energy-intensive anthraquinone process. Herein, we develop...

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Үндсэн зохиолчид: Liu, L, Kang, L, Chutia, A, Feng, J, Michalska, M, Ferrer, P, Grinter, DC, Held, G, Tan, Y, Zhao, F, Guo, F, Hopkinson, DG, Allen, CS, Hou, Y, Gu, J, Papakonstantinou, I, Shearing, PR, Brett, DJL, Parkin, IP, He, G
Формат: Journal article
Хэл сонгох:English
Хэвлэсэн: Wiley 2023
Тодорхойлолт
Тойм:The electrochemical synthesis of hydrogen peroxide (H<sub>2</sub>O<sub>2</sub>) via a two-electron (2 e<sup>−</sup>) 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<sub>2</sub>O<sub>2</sub> electrochemical production. The optimized PCC<sub>900</sub> 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<sub>2</sub>O<sub>2</sub> 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<sup>−</sup> 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.