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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 PublicationANGEWANDTE CHEMIE-INTERNATIONAL EDITION
AbstractThe 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.
DOI10.1002/anie.202012615
WOS IDWOS:000596779800001
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Document Type期刊论文
Identifierhttp://ir.imr.ac.cn/handle/321006/82308
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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