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Spectroscopic Identification of Active Sites of Oxygen-Doped Carbon for Selective Oxygen Reduction to Hydrogen Peroxide |
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| Authors: | Longxiang Liu Dr Liqun Kang Dr Arunabhiram Chutia Jianrui Feng Dr Martyna Michalska Dr Pilar Ferrer Dr David C Grinter Prof Georg Held Yeshu Tan Fangjia Zhao Fei Guo Dr David G Hopkinson Dr Christopher S Allen Dr Yanbei Hou Junwen Gu Prof Ioannis Papakonstantinou Prof Paul R Shearing Prof Dan J L Brett Prof Ivan P Parkin Prof?Dr Guanjie He |
| Institution: | 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. electron Physical Science Imaging Centre, Rutherford Appleton Laboratory, Harwell, Didcot, OX11 0DE UK
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: | 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. |
| Keywords: | Electrocatalysis Hydrogen Peroxide NEXAFS Porous Carbon Quinone |