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

Author:

Liu Longxiang1,Kang Liqun2,Chutia Arunabhiram3,Feng Jianrui1,Michalska Martyna4,Ferrer Pilar5,Grinter David C.5,Held Georg5,Tan Yeshu1,Zhao Fangjia1,Guo Fei1,Hopkinson David G.6,Allen Christopher S.67,Hou Yanbei8,Gu Junwen1,Papakonstantinou Ioannis4,Shearing Paul R.9,Brett Dan J. L.9,Parkin Ivan P.1,He Guanjie19ORCID

Affiliation:

1. Christopher Ingold Laboratory Department of Chemistry University College London 20 Gordon Street London WC1H 0AJ UK

2. Department of Inorganic Spectroscopy Max-Planck-Institute for Chemical Energy Conversion Stiftstr. 34–36 45470 Mülheim an der Ruhr Germany

3. School of Chemistry University of Lincoln Lincolnshire LN6 7DL UK

4. Photonic Innovations Lab Department of Electronic & Electrical Engineering University College London Torrington Place London WC1E 7JE UK

5. Diamond Light Source Rutherford Appleton Laboratory Harwell, Didcot OX11 0DE UK

6. electron Physical Science Imaging Centre Rutherford Appleton Laboratory Harwell, Didcot OX11 0DE UK

7. Department of Materials University of Oxford Parks Road Oxford OX1 3PH UK

8. HP-NTU Digital Manufacturing Corporate Laboratory School of Mechanical and Aerospace Nanyang Technological University 50 Nanyang Avenue Singapore 639798 Singapore

9. Electrochemical Innovation Lab Department of Chemical Engineering University College London London WC1E 7JE UK

Abstract

AbstractThe 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.

Funder

Engineering and Physical Sciences Research Council

Publisher

Wiley

Subject

General Medicine

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