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Using CoCu$_2$Ga/SiO$_2$ to identify stability-issues in ethanol-selective Co-Cu alloyed catalysts in carbon monoxide hydrogenation

Smitshuysen, Thomas Erik Lyck; Lützen, Mads; Zimina, Anna 1,2; Sheppard, Thomas L. ORCID iD icon 2; Jakobsen, Helene Hagemann; Chorkendorff, Ib; Damsgaard, Christian Danvad
1 Institut für Katalyseforschung und -technologie (IKFT), Karlsruher Institut für Technologie (KIT)
2 Institut für Technische Chemie und Polymerchemie (ITCP), Karlsruher Institut für Technologie (KIT)

Abstract:

Hydrogenation of CO to higher alcohols such as ethanol is an attractive pathway for industrial production while avoiding competition with food crops. However, thermocatalytic ethanol production from syngas is currently hindered by the lack of selective catalysts. The structural integrity of ternary-alloyed CoCu2Ga nanoparticles supported on silica was studied during thermo-catalytic CO hydrogenation. Catalysts of four different CoCu$_2$Ga weight-loadings were tested catalytically under differential conversion, showing their different intrinsic selectivity during CO hydrogenation towards ethanol, methanol, and hydrocarbons. CoCu$_2$Ga catalysts with 3.5 wt% and 17.8 wt% proved most and least selective towards ethanol formation, respectively. These two were studied in depth using STEM-EDX of fresh and spent samples showing different size distributions of the nanoparticles for all samples, and a change in the Co/Cu distribution of the nanoparticles from fresh to spent samples. In situ characterization using XRD, XANES, and EXAFS during CO hydrogenation supported the findings of the STEM-EDX and elucidated that the fresh more homogenous catalyst consisting of ternary CoCu$_2$Ga nanoparticles de-alloyed into Cu-rich and CoGa-rich nanoparticles. ... mehr


Verlagsausgabe §
DOI: 10.5445/IR/1000169077
Veröffentlicht am 07.03.2024
Cover der Publikation
Zugehörige Institution(en) am KIT Institut für Katalyseforschung und -technologie (IKFT)
Institut für Technische Chemie und Polymerchemie (ITCP)
Publikationstyp Zeitschriftenaufsatz
Publikationsdatum 05.04.2024
Sprache Englisch
Identifikator ISSN: 0926-860X, 1873-3875
KITopen-ID: 1000169077
HGF-Programm 38.03.02 (POF IV, LK 01) Power-based Fuels and Chemicals
Erschienen in Applied Catalysis A: General
Verlag Elsevier
Band 675
Seiten 119636
Vorab online veröffentlicht am 21.02.2024
Schlagwörter CO hydrogenation, Catalytic alcohol synthesis, Alloyed nanoparticles, Material stability, STEM, EDX, In situ characterization, XRD, XAS
Nachgewiesen in Web of Science
Dimensions
Scopus
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