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@article{2358922,
author = {Pokorný, Tomáš and Doroshenko, Iaroslav and Macháč, Petr and Šimoníková, Lucie and Bittová, Miroslava and Moravec, Zdeněk and Karaskova, Katerina and Škoda, David and Pinkas, Jiří and Stýskalík, Aleš},
article_location = {WASHINGTON},
article_number = {49},
doi = {http://dx.doi.org/10.1021/acs.inorgchem.3c01678},
keywords = {CONTINUOUS SYMMETRY MEASURES; CRYSTAL-STRUCTURES; MAGNETIC-PROPERTIES},
language = {eng},
issn = {0020-1669},
journal = {Inorganic Chemistry},
title = {Copper Phosphinate Complexes as Molecular Precursors for Ethanol Dehydrogenation Catalysts},
url = {https://pubs.acs.org/doi/full/10.1021/acs.inorgchem.3c01678},
volume = {62},
year = {2023}
}
TY - JOUR
ID - 2358922
AU - Pokorný, Tomáš - Doroshenko, Iaroslav - Macháč, Petr - Šimoníková, Lucie - Bittová, Miroslava - Moravec, Zdeněk - Karaskova, Katerina - Škoda, David - Pinkas, Jiří - Stýskalík, Aleš
PY - 2023
TI - Copper Phosphinate Complexes as Molecular Precursors for Ethanol Dehydrogenation Catalysts
JF - Inorganic Chemistry
VL - 62
IS - 49
SP - 19871-19886
EP - 19871-19886
PB - American Chemical Society
SN - 00201669
KW - CONTINUOUS SYMMETRY MEASURES
KW - CRYSTAL-STRUCTURES
KW - MAGNETIC-PROPERTIES
UR - https://pubs.acs.org/doi/full/10.1021/acs.inorgchem.3c01678
N2 - Nowadays, the production of acetaldehyde heavily relies on the petroleum industry. Developing new catalysts for the ethanol dehydrogenation process that could sustainably substitute current acetaldehyde production methods is highly desired. Among the ethanol dehydrogenation catalysts, copper-based materials have been intensively studied. Unfortunately, the Cu-based catalysts suffer from sintering and coking, which lead to rapid deactivation with time-on-stream. Phosphorus doping has been demonstrated to diminish coking in methanol dehydrogenation, fluid catalytic cracking, and ethanol-to-olefin reactions. This work reports a pioneering application of the well-characterized copper phosphinate complexes as molecular precursors for copper-based ethanol dehydrogenation catalysts enriched with phosphate groups (Cu-phosphate/SiO2). Three new catalysts (CuP-1, CuP-2, and CuP-3), prepared by the deposition of complexes {Cu(SAAP)}(n) (1), [Cu-6(BSAAP)(6)] (2), and [Cu-3(NAAP)(3)] (3) on the surface of commercial SiO2, calcination at 500 degrees C, and reduction in the stream of the forming gas 5% H-2/N-2 at 400 degrees C, exhibited unusual properties. First, the catalysts showed a rapid increase in catalytic activity. After reaching the maximum conversion, the catalyst started to deactivate. The unusual behavior could be explained by the presence of the phosphate phase, which made Cu2+ reduction more difficult. The phosphorus content gradually decreased during time-on-stream, copper was reduced, and the activity increased. The deactivation of the catalyst could be related to the copper diffusion processes. The most active CuP-1 catalyst reaches a maximum of 73% ethanol conversion and over 98% acetaldehyde selectivity at 325 degrees C and WHSV = 2.37 h(-1).
ER -
POKORNÝ, Tomáš, Iaroslav DOROSHENKO, Petr MACHÁČ, Lucie ŠIMONÍKOVÁ, Miroslava BITTOVÁ, Zdeněk MORAVEC, Katerina KARASKOVA, David ŠKODA, Jiří PINKAS and Aleš STÝSKALÍK. Copper Phosphinate Complexes as Molecular Precursors for Ethanol Dehydrogenation Catalysts. \textit{Inorganic Chemistry}. WASHINGTON: American Chemical Society, 2023, vol.~62, No~49, p.~19871-19886. ISSN~0020-1669. Available from: https://dx.doi.org/10.1021/acs.inorgchem.3c01678.
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