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 (2021)
Overall oxygen electrocatalysis on nitrogen‐modified carbon catalysts: identification of active sites and in situ observation of reactive intermediates.
In: Angewandte Chemie International Edition, 60 (6)
doi: 10.1002/anie.202012615
Article, Bibliographie

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⁻*+H₂O→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.

Item Type:	Article
Erschienen:	2021
Creators:	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
Type of entry:	Bibliographie
Title:	Overall oxygen electrocatalysis on nitrogen‐modified carbon catalysts: identification of active sites and in situ observation of reactive intermediates
Language:	English
Date:	2021
Place of Publication:	Weinheim
Publisher:	Wiley-VCH
Journal or Publication Title:	Angewandte Chemie International Edition
Volume of the journal:	60
Issue Number:	6
DOI:	10.1002/anie.202012615
Corresponding Links:	TUprints secondary publication
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⁻*+H₂O→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.
Alternative Abstract:	Alternative abstract Language Dynamic evolution of active sites and key oxygen intermediate products during the ORR and OER on N-doped carbon catalysts are monitored experimentally with in situ ATR-IR spectra. With the assistance of isotopic labeling, the formation of *OOH species from O₂⁻* (O₂⁻*+H₂O→OOH*+OH⁻) is suggested to be a possible RDS during the ORR process, whereas the generation of O₂ from OOH* species is the most possible RDS during the OER process. English
Uncontrolled Keywords:	active site, in situ infrared spectroscopy, intermediates, metal-free carbon, nitrogen doping
Classification DDC:	500 Science and mathematics > 540 Chemistry 600 Technology, medicine, applied sciences > 660 Chemical engineering
Divisions:	07 Department of Chemistry 07 Department of Chemistry > Ernst-Berl-Institut 07 Department of Chemistry > Ernst-Berl-Institut > Fachgebiet Technische Chemie 07 Department of Chemistry > Ernst-Berl-Institut > Fachgebiet Technische Chemie > Technische Chemie I
Date Deposited:	13 Feb 2024 07:49
Last Modified:	13 Feb 2024 07:49
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• Overall Oxygen Electrocatalysis on Nitrogen‐Modified Carbon Catalysts: Identification of Active Sites and In Situ Observation of Reactive Intermediates. (deposited 12 Feb 2024 13:53)
  • Overall oxygen electrocatalysis on nitrogen‐modified carbon catalysts: identification of active sites and in situ observation of reactive intermediates. (deposited 13 Feb 2024 07:49) [Currently Displayed]

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