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 (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
Artikel, Bibliographie

Dies ist die neueste Version dieses Eintrags.

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:

2021

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:

Bibliographie

Titel:

Overall oxygen electrocatalysis on nitrogen‐modified carbon catalysts: identification of active sites and in situ observation of reactive intermediates

Sprache:

Englisch

Publikationsjahr:

2021

Ort:

Weinheim

Verlag:

Wiley-VCH

Titel der Zeitschrift, Zeitung oder Schriftenreihe:

Angewandte Chemie International Edition

Jahrgang/Volume einer Zeitschrift:

(Heft-)Nummer:

DOI:

10.1002/anie.202012615

Zugehörige Links:

TUprints Zweitveröffentlichung

Kurzbeschreibung (Abstract):

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

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:

13 Feb 2024 07:49

Letzte Änderung:

13 Feb 2024 07:49

PPN: