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@ARTICLE{Degerman:629827,
author = {Degerman, David and Lömker, Patrick and Soldemo, Markus
and Garcia Martinez, Fernando and Engel, Robin and Beye,
Martin and Nilsson, Anders},
title = {{S}pectroscopic {S}urvey of {S}electivity {T}rends in
{S}yngas {C}onversion over {S}ingle {C}rystal {C}atalysts},
journal = {The journal of physical chemistry / C},
volume = {129},
number = {22},
issn = {1932-7447},
address = {Washington, DC},
publisher = {Soc.},
reportid = {PUBDB-2025-01826},
pages = {10107 - 10115},
year = {2025},
abstract = {The sustainability transition of the chemical industry
hinges on the educated design of catalysts for reactions
such as the CO hydrogenation, optimizing the materials for
selectivity toward valuable products. So far, theoretical
models have been used to predict reaction selectivity from
the competition of elementary surface processes. Here, we
provide an in situ experimental view of surface adsorbates
during CO hydrogenation. We compare X-ray photoelectron
spectra acquired at reaction conditions (200–325 °C, 150
mbar) over single crystals of Fe, Rh, Ni, Co, and Cu and
infer which elementary steps decide the product
distribution. We find that the chemisorption energies of C
and O, as often used descriptors for catalytic activity,
qualitatively predict the rate-limiting steps. They fail,
although when reaction-induced carburization occurs on Ni
and Fe, steering the selectivity toward methanation on Ni
and hydrocarbon chain growth on Fe. For the noncarburized Co
and Rh we show how the adsorbate distribution and the oxygen
chemisorption energy allow for oxygenate production on Rh,
but hydrocarbon chain growth on stepped Co. Ultimately, we
show how in situ experiments provide a chemical and
mechanistic understanding of CO hydrogenation selectivity,
useful to tailor catalysts for a sustainable production of
high-value chemicals.},
cin = {FS DOOR-User / FS-PET-S},
ddc = {530},
cid = {$I:(DE-H253)FS_DOOR-User-20241023$ /
I:(DE-H253)FS-PET-S-20190712},
pnm = {6G3 - PETRA III (DESY) (POF4-6G3) / FS-Proposal:
II-20211048 EC (II-20211048-EC) / FS-Proposal: II-20190003
EC (II-20190003-EC) / FS-Proposal: I-20191434 EC
(I-20191434-EC) / FS-Proposal: I-20200092 EC (I-20200092-EC)
/ SWEDEN-DESY - SWEDEN-DESY Collaboration
$(2020_Join2-SWEDEN-DESY)$},
pid = {G:(DE-HGF)POF4-6G3 / G:(DE-H253)II-20211048-EC /
G:(DE-H253)II-20190003-EC / G:(DE-H253)I-20191434-EC /
G:(DE-H253)I-20200092-EC /
$G:(DE-HGF)2020_Join2-SWEDEN-DESY$},
experiment = {EXP:(DE-H253)P-P22-20150101},
typ = {PUB:(DE-HGF)16},
UT = {WOS:001492361600001},
doi = {10.1021/acs.jpcc.5c01914},
url = {https://bib-pubdb1.desy.de/record/629827},
}