TU Darmstadt / ULB / TUprints

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 (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
Article, Secondary publication, Publisher's Version

[img]
Preview
Text
ANIE_ANIE202012615.pdf
Copyright Information: CC BY 4.0 International - Creative Commons, Attribution.

Download (2MB) | Preview
[img] Text (Supplement)
anie202012615-sup-0001-misc_information.pdf
Copyright Information: CC BY 4.0 International - Creative Commons, Attribution.

Download (4MB)
Item Type: Article
Type of entry: Secondary publication
Title: Overall Oxygen Electrocatalysis on Nitrogen‐Modified Carbon Catalysts: Identification of Active Sites and In Situ Observation of Reactive Intermediates
Language: English
Date: 12 February 2024
Place of Publication: Darmstadt
Year of primary publication: 2021
Place of primary publication: Weinheim
Publisher: Wiley-VCH
Journal or Publication Title: Angewandte Chemie International Edition
Volume of the journal: 60
Issue Number: 6
DOI: 10.26083/tuprints-00017811
Corresponding Links:
Origin: Secondary publication DeepGreen
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 AbstractLanguage

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
Status: Publisher's Version
URN: urn:nbn:de:tuda-tuprints-178111
Classification DDC: 500 Science and mathematics > 540 Chemistry
600 Technology, medicine, applied sciences > 660 Chemical engineering
Divisions: 07 Department of Chemistry > Ernst-Berl-Institut > Fachgebiet Technische Chemie > Technische Chemie I
Date Deposited: 12 Feb 2024 13:53
Last Modified: 03 Jul 2024 09:54
SWORD Depositor: Deep Green
URI: https://tuprints.ulb.tu-darmstadt.de/id/eprint/17811
PPN: 519322088
Export:
Actions (login required)
View Item View Item