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Overall Oxygen Electrocatalysis on Nitrogen-Modified Carbon Catalysts: Identification of Active Sites and In?Situ Observation of Reactive Intermediates.


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 O2 (ads), superoxide anion O2 - *, and OOH* are monitored with in?situ spectroscopy. We propose that the formation of *OOH species from O2 - * (O2 - *+H2 O?OOH*+OH- ) is a possible RDS during the ORR process, whereas the generation of O2 from OOH* species is the most likely RDS during the OER process.

SUBMITTER: Lin Y 

PROVIDER: S-EPMC7898341 | biostudies-literature | 2021 Feb

REPOSITORIES: biostudies-literature

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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 Y   Liu Zigeng Z   Yu Linhui L   Zhang Gui-Rong GR   Tan Hao H   Wu Kuang-Hsu KH   Song Feihong F   Mechler Anna K AK   Schleker P Philipp M PPM   Lu Qing Q   Zhang Bingsen B   Heumann Saskia S  

Angewandte Chemie (International ed. in English) 20201208 6


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  ...[more]

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