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@ARTICLE{Schulte:622772,
author = {Schulte, Mariam L. and Truttmann, Vera and Doronkin, Dmitry
E. and Baumgarten, Lorena and Nicolai, Alexander and
Beltran, Diego Alejandro Montalvo and Summ, Florian J. and
Kiener, Christoph and Warmuth, Lucas and Pitter, Stephan and
Saraçi, Erisa and Grunwaldt, Jan-Dierk},
title = {{M}onitoring the {F}ate of {Z}n in the
{C}u/{Z}n{O}/{Z}r{O}$_2$ {C}atalyst during
{CO}$_2$‐to‐{M}ethanol {S}ynthesis at {H}igh
{C}onversions by {O}perando {S}pectroscopy},
journal = {Angewandte Chemie / International edition},
volume = {64},
number = {15},
issn = {1433-7851},
address = {Weinheim},
publisher = {Wiley-VCH},
reportid = {PUBDB-2025-00466},
pages = {e202423281},
year = {2025},
note = {Supposed to be Open Access covered by Project Deal (after
corresponding author signs the publishing agreement).},
abstract = {In the frame of developing a sustainable chemical industry,
heterogeneously catalyzed CO$_2$ hydrogenation to methanol
has attracted considerable interest. However, the Cu-Zn
based catalyst system employed in this process is very
dynamic, especially in the presence of the products methanol
and water. Deactivation needs to be prevented, but its
origin and mechanism are hardly investigated at high
conversion where product condensation is possible. Here, we
report on the structural dynamics of a Cu/ZnO/ZrO$_2$
catalyst at 90 bar and 40\% CO$_2$ conversion (at
equilibrium conditions), investigated in a dedicated
metal-based spectroscopic cell specially fabricated using
additive manufacturing. This particular reactor
configuration aims to mimic the high CO$_2$ conversion part
of the catalyst bed and can induce product condensation,
which is monitored by operando X-ray absorption
spectroscopy. While Cu remained mostly stable throughout the
experiment, Zn underwent strong restructuring. The chosen
reaction conditions, including the use of CO$_2$ as carbon
source and in situ product condensation, were selected to
provide insights under industrial conditions. This work
highlights the importance of spectroscopic investigations at
high conversion levels, offering insights into chemical
transformations during deactivation, extending the concept
of spatially resolved studies, and thus providing guidance
for the design of more stable catalysts.},
cin = {FS DOOR-User},
ddc = {540},
cid = {$I:(DE-H253)FS_DOOR-User-20241023$},
pnm = {6G3 - PETRA III (DESY) (POF4-6G3) / FS-Proposal: I-20230260
(I-20230260) / DFG project G:(GEPRIS)460248799 - DAPHNE4NFDI
- DAten aus PHoton- und Neutronen Experimenten für NFDI
(460248799)},
pid = {G:(DE-HGF)POF4-6G3 / G:(DE-H253)I-20230260 /
G:(GEPRIS)460248799},
experiment = {EXP:(DE-H253)P-P65-20150101},
typ = {PUB:(DE-HGF)16},
pubmed = {pmid:39866096},
UT = {WOS:001421758200001},
doi = {10.1002/anie.202423281},
url = {https://bib-pubdb1.desy.de/record/622772},
}