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...
| Main Authors: | , , , , , , , , , , , , , , , , , , , |
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| Format: | Journal article |
| Language: | English |
| Published: |
Wiley
2023
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| _version_ | 1797110530811363328 |
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| author | 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 |
| author_facet | 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 |
| author_sort | Liu, L |
| collection | OXFORD |
| description | 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. |
| first_indexed | 2024-03-07T07:56:10Z |
| format | Journal article |
| id | oxford-uuid:853959b3-a034-4a32-95e3-dfac53e30dc3 |
| institution | University of Oxford |
| language | English |
| last_indexed | 2024-03-07T07:56:10Z |
| publishDate | 2023 |
| publisher | Wiley |
| record_format | dspace |
| spelling | oxford-uuid:853959b3-a034-4a32-95e3-dfac53e30dc32023-08-16T17:01:31ZSpectroscopic identification of active sites of oxygen-doped carbon for selective oxygen reduction to hydrogen peroxideJournal articlehttp://purl.org/coar/resource_type/c_dcae04bcuuid:853959b3-a034-4a32-95e3-dfac53e30dc3EnglishSymplectic Elements Wiley2023Liu, LKang, LChutia, AFeng, JMichalska, MFerrer, PGrinter, DCHeld, GTan, YZhao, FGuo, FHopkinson, DGAllen, CSHou, YGu, JPapakonstantinou, IShearing, PRBrett, DJLParkin, IPHe, GThe 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. |
| spellingShingle | 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 Spectroscopic identification of active sites of oxygen-doped carbon for selective oxygen reduction to hydrogen peroxide |
| title | Spectroscopic identification of active sites of oxygen-doped carbon for selective oxygen reduction to hydrogen peroxide |
| title_full | Spectroscopic identification of active sites of oxygen-doped carbon for selective oxygen reduction to hydrogen peroxide |
| title_fullStr | Spectroscopic identification of active sites of oxygen-doped carbon for selective oxygen reduction to hydrogen peroxide |
| title_full_unstemmed | Spectroscopic identification of active sites of oxygen-doped carbon for selective oxygen reduction to hydrogen peroxide |
| title_short | Spectroscopic identification of active sites of oxygen-doped carbon for selective oxygen reduction to hydrogen peroxide |
| title_sort | spectroscopic identification of active sites of oxygen doped carbon for selective oxygen reduction to hydrogen peroxide |
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