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@ARTICLE{Vennewald:1006568,
author = {Vennewald, Maurice and Sackers, Nina Michelle and Iemhoff,
Andree and Kappel, Isabella and Weidenthaler, Claudia and
Meise, Ansgar and Heggen, Marc and Dunin-Borkowski, Rafal
and Keenan, Luke and Palkovits, Regina},
title = {{D}ynamics of palladium single-atoms on graphitic carbon
nitride during ethylene hydrogenation},
journal = {Journal of catalysis},
volume = {421},
issn = {0021-9517},
address = {Amsterdam [u.a.]},
publisher = {Elsevier},
reportid = {FZJ-2023-01716},
pages = {134 - 144},
year = {2023},
abstract = {Single-atoms on carbon–nitrogen supports are considered
catalysts for a multitude of reactions. However, doubts
remain whether really these species or subnanometer clusters
formed under reaction conditions are the active species. In
this work, we investigate the dynamics of palladium
single-atoms on graphitic carbon nitride during ethylene
hydrogenation and H2-D2 exchange. By employing
aberration-corrected scanning transmission electron
microscopy, x-ray photoelectron spectroscopy and x-ray
absorption spectroscopy, we will show that palladium,
originally present as single-atoms, agglomerates to clusters
at 100 °C in a gas atmosphere that contains both ethylene
and hydrogen. This agglomeration goes in hand with the
emergence of catalytic activity in both ethylene
hydrogenation and H2-D2 exchange, suggesting that clusters,
rather than single-atoms, are the active species. The
results presented herein highlight the potential of
analytics over the course of reaction to identify the active
species and provide new insights into the influence of gas
atmosphere on metal speciation.},
cin = {ER-C-1},
ddc = {540},
cid = {I:(DE-Juel1)ER-C-1-20170209},
pnm = {5351 - Platform for Correlative, In Situ and Operando
Characterization (POF4-535)},
pid = {G:(DE-HGF)POF4-5351},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000956023800001},
doi = {10.1016/j.jcat.2023.03.011},
url = {https://juser.fz-juelich.de/record/1006568},
}