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@ARTICLE{Lin:889905,
author = {Lin, Yangming and Liu, Zigeng and Yu, Linhui and Zhang,
Gui‐Rong and Tan, Hao and Wu, Kuang‐Hsu and Song,
Feihong and Mechler, Anna and Schleker, Peter Philipp Maria
and Lu, Qing and Zhang, Bingsen and Heumann, Saskia},
title = {{O}verall {O}xygen {E}lectrocatalysis on
{N}itrogen‐{M}odified {C}arbon {C}atalysts:
{I}dentification of {A}ctive {S}ites and {I}n {S}itu
{O}bservation of {R}eactive {I}ntermediates},
journal = {Angewandte Chemie / International edition},
volume = {60},
number = {6},
issn = {1521-3773},
address = {Weinheim},
publisher = {Wiley-VCH},
reportid = {FZJ-2021-00513},
pages = {3299-3306},
year = {2021},
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.},
cin = {IEK-9},
ddc = {540},
cid = {I:(DE-Juel1)IEK-9-20110218},
pnm = {899 - ohne Topic (POF4-899)},
pid = {G:(DE-HGF)POF4-899},
typ = {PUB:(DE-HGF)16},
pubmed = {33151593},
UT = {WOS:000596779800001},
doi = {10.1002/anie.202012615},
url = {https://juser.fz-juelich.de/record/889905},
}