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 (2024)
Overall Oxygen Electrocatalysis on Nitrogen‐Modified Carbon Catalysts: Identification of Active Sites and In Situ Observation of Reactive Intermediates.
In: Angewandte Chemie International Edition, 2021, 60 (6)
doi: 10.26083/tuprints-00017811
Artikel, Zweitveröffentlichung, Verlagsversion

Kurzbeschreibung (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.

Typ des Eintrags:	Artikel
Erschienen:	2024
Autor(en):	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
Art des Eintrags:	Zweitveröffentlichung
Titel:	Overall Oxygen Electrocatalysis on Nitrogen‐Modified Carbon Catalysts: Identification of Active Sites and In Situ Observation of Reactive Intermediates
Sprache:	Englisch
Publikationsjahr:	12 Februar 2024
Ort:	Darmstadt
Publikationsdatum der Erstveröffentlichung:	2021
Ort der Erstveröffentlichung:	Weinheim
Verlag:	Wiley-VCH
Titel der Zeitschrift, Zeitung oder Schriftenreihe:	Angewandte Chemie International Edition
Jahrgang/Volume einer Zeitschrift:	60
(Heft-)Nummer:	6
DOI:	10.26083/tuprints-00017811
URL / URN:	https://tuprints.ulb.tu-darmstadt.de/17811
Zugehörige Links:	Verlags-DOI
Herkunft:	Zweitveröffentlichung DeepGreen
Kurzbeschreibung (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.
Alternatives oder übersetztes Abstract:	Alternatives Abstract Sprache 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. Englisch
Freie Schlagworte:	active site, in situ infrared spectroscopy, intermediates, metal-free carbon, nitrogen doping
Status:	Verlagsversion
URN:	urn:nbn:de:tuda-tuprints-178111
Sachgruppe der Dewey Dezimalklassifikatin (DDC):	500 Naturwissenschaften und Mathematik > 540 Chemie 600 Technik, Medizin, angewandte Wissenschaften > 660 Technische Chemie
Fachbereich(e)/-gebiet(e):	07 Fachbereich Chemie 07 Fachbereich Chemie > Ernst-Berl-Institut 07 Fachbereich Chemie > Ernst-Berl-Institut > Fachgebiet Technische Chemie 07 Fachbereich Chemie > Ernst-Berl-Institut > Fachgebiet Technische Chemie > Technische Chemie I
Hinterlegungsdatum:	12 Feb 2024 13:53
Letzte Änderung:	13 Feb 2024 07:48
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Verfügbare Versionen dieses Eintrags

• 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) [Gegenwärtig angezeigt]
  • 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)

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