TY  - JOUR
AU  - Lin, Yangming
AU  - Liu, Zigeng
AU  - Yu, Linhui
AU  - Zhang, Gui‐Rong
AU  - Tan, Hao
AU  - Wu, Kuang‐Hsu
AU  - Song, Feihong
AU  - Mechler, Anna
AU  - Schleker, Peter Philipp Maria
AU  - Lu, Qing
AU  - Zhang, Bingsen
AU  - Heumann, Saskia
TI  - Overall Oxygen Electrocatalysis on Nitrogen‐Modified Carbon Catalysts: Identification of Active Sites and In Situ Observation of Reactive Intermediates
JO  - Angewandte Chemie / International edition
VL  - 60
IS  - 6
SN  - 1521-3773
CY  - Weinheim
PB  - Wiley-VCH
M1  - FZJ-2021-00513
SP  - 3299-3306
PY  - 2021
AB  - 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.
LB  - PUB:(DE-HGF)16
C6  - 33151593
UR  - <Go to ISI:>//WOS:000596779800001
DO  - DOI:10.1002/anie.202012615
UR  - https://juser.fz-juelich.de/record/889905
ER  -