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@ARTICLE{Degerman:605387,
author = {Degerman, David and Shipilin, Mikhail and Lömker, Patrick
and Soldemo, Markus and Goodwin, Christopher and Wagstaffe,
Michael and Börner, Mia and Schlueter, Christoph and Amann,
Peter and Nilsson, Anders},
title = {{E}ffect of ${CO}_2$-{R}ich {S}yngas on the {C}hemical
{S}tate of {F}e(110) during {F}ischer–{T}ropsch
{S}ynthesis},
journal = {The journal of physical chemistry / C},
volume = {128},
number = {13},
issn = {1932-7447},
address = {Washington, DC},
publisher = {Soc.},
reportid = {PUBDB-2024-01454},
pages = {5542-5552},
year = {2024},
abstract = {We have used in situ X-ray photoelectron spectroscopy to
obtain information about the chemical state of a Fe single
crystal catalyst upon addition of CO$_2$ in the syngas feed
duringFischer−Tropsch synthesis (FTS) between 85 and 550
mbar. We found that at certain temperatures, the ternary
mixture of CO, CO$_2$, and H$_2$ yields a chemical state
which is resemblant of neither the CO hydrogenation nor the
CO$_2$ hydrogenation reaction mixtures in isolation. The
addition of CO$_2$ to a CO + H$_2$ reaction mixture mostly
affects the chemical state at low-temperature FTS conditions
(i.e., below 254 °C). In this temperature span, the ternary
reaction mixture resulted in a carburized surface, whereas
the CO + H$_2$ reaction led to surface oxidation. We propose
a hypothesis, where a carbonate intermediate produced by
CO$_2$ interaction with Fe oxide aids the reduction of the
Fe oxide, paving the way for the carburization of the Fe by
dissociated CO. Very small differences in the spectra of the
CO + H$_2$ and the CO + CO$_2$ + H$_2$ reaction mixtures
were observed above 254 °C, suggesting that the CO$_2$ is a
spectator in these conditions. Changing the total pressure
of both the CO hydrogenation and ternary reaction mixture
causes quantitative changes in the spectra at both low- and
high-temperature FTS conditions, the degree of oxidation/
carburization was affected in the low-temperature-FTS
regime, and the degree of hydrocarbon build-up was affected
in the high-temperature-FTS.},
cin = {DOOR ; HAS-User / FS-PETRA-S},
ddc = {530},
cid = {I:(DE-H253)HAS-User-20120731 /
I:(DE-H253)FS-PETRA-S-20210408},
pnm = {631 - Matter – Dynamics, Mechanisms and Control
(POF4-631) / 6G3 - PETRA III (DESY) (POF4-6G3) /
FS-Proposal: I-20181131 EC (I-20181131-EC) / FS-Proposal:
I-20200292 EC (I-20200292-EC) / CALIPSOplus - Convenient
Access to Light Sources Open to Innovation, Science and to
the World (730872) / SWEDEN-DESY - SWEDEN-DESY Collaboration
$(2020_Join2-SWEDEN-DESY)$},
pid = {G:(DE-HGF)POF4-631 / G:(DE-HGF)POF4-6G3 /
G:(DE-H253)I-20181131-EC / G:(DE-H253)I-20200292-EC /
G:(EU-Grant)730872 / $G:(DE-HGF)2020_Join2-SWEDEN-DESY$},
experiment = {EXP:(DE-H253)P-P22-20150101},
typ = {PUB:(DE-HGF)16},
UT = {WOS:001189795000001},
doi = {10.1021/acs.jpcc.3c08180},
url = {https://bib-pubdb1.desy.de/record/605387},
}