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Spectroscopic Identification of Active Sites of Oxygen-Doped Carbon for Selective Oxygen Reduction to Hydrogen Peroxide.
Liu, Longxiang; Kang, Liqun; Chutia, Arunabhiram; Feng, Jianrui; Michalska, Martyna; Ferrer, Pilar; Grinter, David C; Held, Georg; Tan, Yeshu; Zhao, Fangjia; Guo, Fei; Hopkinson, David G; Allen, Christopher S; Hou, Yanbei; Gu, Junwen; Papakonstantinou, Ioannis; Shearing, Paul R; Brett, Dan J L; Parkin, Ivan P; He, Guanjie.
Afiliação
  • Liu L; Christopher Ingold Laboratory, Department of Chemistry, University College London, 20 Gordon Street, London, WC1H 0AJ, UK.
  • Kang L; Department of Inorganic Spectroscopy, Max-Planck-Institute for Chemical Energy Conversion, Stiftstr. 34-36, 45470, Mülheim an der Ruhr, Germany.
  • Chutia A; School of Chemistry, University of Lincoln, Lincolnshire, LN6 7DL, UK.
  • Feng J; Christopher Ingold Laboratory, Department of Chemistry, University College London, 20 Gordon Street, London, WC1H 0AJ, UK.
  • Michalska M; Photonic Innovations Lab, Department of Electronic & Electrical Engineering, University College London, Torrington Place, London, WC1E 7JE, UK.
  • Ferrer P; Diamond Light Source, Rutherford Appleton Laboratory, Harwell, Didcot, OX11 0DE, UK.
  • Grinter DC; Diamond Light Source, Rutherford Appleton Laboratory, Harwell, Didcot, OX11 0DE, UK.
  • Held G; Diamond Light Source, Rutherford Appleton Laboratory, Harwell, Didcot, OX11 0DE, UK.
  • Tan Y; Christopher Ingold Laboratory, Department of Chemistry, University College London, 20 Gordon Street, London, WC1H 0AJ, UK.
  • Zhao F; Christopher Ingold Laboratory, Department of Chemistry, University College London, 20 Gordon Street, London, WC1H 0AJ, UK.
  • Guo F; Christopher Ingold Laboratory, Department of Chemistry, University College London, 20 Gordon Street, London, WC1H 0AJ, UK.
  • Hopkinson DG; electron Physical Science Imaging Centre, Rutherford Appleton Laboratory, Harwell, Didcot, OX11 0DE, UK.
  • Allen CS; electron Physical Science Imaging Centre, Rutherford Appleton Laboratory, Harwell, Didcot, OX11 0DE, UK.
  • Hou Y; Department of Materials, University of Oxford, Parks Road, Oxford, OX1 3PH, UK.
  • Gu J; HP-NTU Digital Manufacturing Corporate Laboratory, School of Mechanical and Aerospace, Nanyang Technological University, 50 Nanyang Avenue, Singapore, 639798, Singapore.
  • Papakonstantinou I; Christopher Ingold Laboratory, Department of Chemistry, University College London, 20 Gordon Street, London, WC1H 0AJ, UK.
  • Shearing PR; Photonic Innovations Lab, Department of Electronic & Electrical Engineering, University College London, Torrington Place, London, WC1E 7JE, UK.
  • Brett DJL; Electrochemical Innovation Lab, Department of Chemical Engineering, University College London, London, WC1E 7JE, UK.
  • Parkin IP; Electrochemical Innovation Lab, Department of Chemical Engineering, University College London, London, WC1E 7JE, UK.
  • He G; Christopher Ingold Laboratory, Department of Chemistry, University College London, 20 Gordon Street, London, WC1H 0AJ, UK.
Angew Chem Int Ed Engl ; 62(21): e202303525, 2023 May 15.
Article em En | MEDLINE | ID: mdl-36929681
ABSTRACT
The electrochemical synthesis of hydrogen peroxide (H2 O2 ) 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 H2 O2 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 H2 O2 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.
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Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Tipo de estudo: Diagnostic_studies Idioma: En Revista: Angew Chem Int Ed Engl Ano de publicação: 2023 Tipo de documento: Article País de afiliação: Reino Unido

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Tipo de estudo: Diagnostic_studies Idioma: En Revista: Angew Chem Int Ed Engl Ano de publicação: 2023 Tipo de documento: Article País de afiliação: Reino Unido