Overall Oxygen Electrocatalysis on Nitrogen-Modified Carbon Catalysts: Identification of Active Sites and In Situ Observation of Reactive Intermediates | |
Lin, Yangming; Liu, Zigeng; Yu, Linhui; Zhang, Gui-Rong; Tan, Hao; Wu, Kuang-Hsu; Song, Feihong; Mechler, Anna K.; Schleker, P. Philipp M.; Lu, Qing; Zhang, Bingsen; Heumann, Saskia | |
2020-12-07 | |
Source Publication | ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
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Abstract | The recent mechanistic understanding of active sites, adsorbed intermediate products, and rate-determining steps (RDS) of nitrogen (N)-modified carbon catalysts in electrocatalytic oxygen reduction (ORR) and oxygen evolution reaction (OER) are still rife with controversy because of the inevitable coexistence of diverse N configurations and the technical limitations for the observation of formed intermediates. Herein, seven kinds of aromatic molecules with designated single N species are used as model structures to investigate the explicit role of each common N group in both ORR and OER. Specifically, dynamic evolution of active sites and key adsorbed intermediate products including O-2 (ads), superoxide anion O-2(-)*, and OOH* are monitored with in situ spectroscopy. We propose that the formation of *OOH species from O-2(-)* (O-2(-)*+H2O -> OOH*+OH-) is a possible RDS during the ORR process, whereas the generation of O-2 from OOH* species is the most likely RDS during the OER process. |
DOI | 10.1002/anie.202012615 |
WOS ID | WOS:000596779800001 |
Citation statistics | |
Document Type | 期刊论文 |
Identifier | http://ir.imr.ac.cn/handle/321006/155644 |
Collection | 中国科学院金属研究所 |
Recommended Citation GB/T 7714 | Lin, Yangming,Liu, Zigeng,Yu, Linhui,et al. Overall Oxygen Electrocatalysis on Nitrogen-Modified Carbon Catalysts: Identification of Active Sites and In Situ Observation of Reactive Intermediates[J]. ANGEWANDTE CHEMIE-INTERNATIONAL EDITION,2020. |
APA | Lin, Yangming.,Liu, Zigeng.,Yu, Linhui.,Zhang, Gui-Rong.,Tan, Hao.,...&Heumann, Saskia.(2020).Overall Oxygen Electrocatalysis on Nitrogen-Modified Carbon Catalysts: Identification of Active Sites and In Situ Observation of Reactive Intermediates.ANGEWANDTE CHEMIE-INTERNATIONAL EDITION. |
MLA | Lin, Yangming,et al."Overall Oxygen Electrocatalysis on Nitrogen-Modified Carbon Catalysts: Identification of Active Sites and In Situ Observation of Reactive Intermediates".ANGEWANDTE CHEMIE-INTERNATIONAL EDITION (2020). |
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