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@ARTICLE{Sarma:611720,
author = {Sarma, Bidyut Bikash and Neukum, Dominik and Doronkin,
Dmitry and Lakshmi Nilayam, Ajai Raj and Baumgarten, Lorena
and Krause, Baerbel and Grunwaldt, Jan-Dierk},
title = {{U}nderstanding the role of supported {R}h atoms and
clusters during hydroformylation and {CO} hydrogenation
reactions with in situ / operando {XAS} and {DRIFT}
spectroscopy},
journal = {Chemical science},
volume = {15},
number = {31},
issn = {2041-6520},
address = {Cambridge},
publisher = {RSC},
reportid = {PUBDB-2024-05033},
pages = {12369-12379},
year = {2024},
abstract = {Supported Rh single-atoms and clusters on CeO2, MgO, and
ZrO2 were investigated as catalysts for hydroformylation of
ethylene to propionaldehyde and CO hydrogenation to
methanol/ethanol with in situ/operando diffuse reflectance
infrared Fourier transform spectroscopy (DRIFTS) and X-ray
absorption spectroscopy (XAS). Under hydroformylation
reaction conditions, operando spectroscopic investigations
unravel the presence of both single atoms and clusters and
detected at first propanal and then methanol. We find that
the formation of methanol is associated with CO
hydrogenation over Rh clusters which was further confirmed
under CO hydrogenation conditions at elevated pressure. The
activity of catalysts synthesized via a precipitation (PP)
method over various supports towards the hydroformylation
reaction follows the order: Rh/ZrO2 > Rh/CeO2 > Rh/MgO.
Comparing Rh/CeO2 catalysts synthesized via different
methods, catalysts prepared by flame spray pyrolysis (FSP)
showed catalytic activity for the hydroformylation reaction
at lower temperatures (413 K), whereas catalysts prepared by
wet impregnation (WI) showed the highest stability. These
results not only provide fundamental insights into the
atomistic level of industrially relevant reactions but also
pave the way for a rational design of new catalysts in the
future.},
cin = {DOOR ; HAS-User},
ddc = {540},
cid = {I:(DE-H253)HAS-User-20120731},
pnm = {6G3 - PETRA III (DESY) (POF4-6G3) / FS-Proposal: I-20200891
(I-20200891) / FS-Proposal: I-20211473 (I-20211473) / SFB
1441 B03 - In situ/operando-Charakterisierung von
Edelmetallclustern und Partikeln auf Metalloxiden unter
Reaktionsbedingungen (B03) (446701131)},
pid = {G:(DE-HGF)POF4-6G3 / G:(DE-H253)I-20200891 /
G:(DE-H253)I-20211473 / G:(GEPRIS)446701131},
experiment = {EXP:(DE-H253)P-P65-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:39118611},
UT = {WOS:001275391000001},
doi = {10.1039/D4SC02907K},
url = {https://bib-pubdb1.desy.de/record/611720},
}