Journal
JOURNAL OF CATALYSIS
Volume 378, Issue -, Pages 1-16Publisher
ACADEMIC PRESS INC ELSEVIER SCIENCE
DOI: 10.1016/j.jcat.2019.08.013
Keywords
CO hydrogenation; Ethanol; Higher alcohols; CuCoMn; Spherical-platelike structure
Categories
Funding
- National Natural Science Foundation of China [21573269, U1510110, 91645113]
- Key Research Program of Frontier Sciences, CAS [QYZDB-SSW-JSC043]
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Novel CuCoMn ternary catalyst with a spherical-platelike (CuMn-Co) nanosized particles structure was designed and successfully performed in ethanol and higher alcohols (HA) production via heterogeneous CO hydrogenation. The spherical-platelike CuCoMn catalyst, achieved through a simple co-precipitation (CP) route followed by a calcination-reduction process, contained a CuMn-rich sphere structure and a Co-dominated nanosheet. The catalyst demonstrated a total alcohols selectivity of 46.2%, and the fraction of ethanol reached up to 45.4% among the total alcohols products, which is superior to the classical modified CuCo-based catalysts. The outstanding catalytic performance was attributed to the unique spherical-platelike structure, which altered the surface Cu+/Cu-0 distribution and the dispersion of Co species. As revealed by in situ XRD, H-2-TPR, in situ XPS, HAADF-STEM and in situ DRIFT spectra techniques, a strong electronic and geometric interaction between Cu and Mn species in optimized CuCoMn catalyst modified the chemical states of Cu species to present a higher proportion of surface Cu+/(Cu-0 + Cu+) and, especially, enhanced the linear CO adsorption on Cu+ active sites, which provided a higher probability of CO insertion, and eventually contributed to promotion of catalytic performance. In addition, a higher probability of bridge CO adsorption on metallic Co was also observed over the CuCoMn catalyst, which was beneficial for the formation of CHx intermediates. It is concluded that a synergistic effect between Cu+ and Co species, promoted by the presence of manganese species, was responsible for CO hydrogenation to produce ethanol. (C) 2019 Elsevier Inc. All rights reserved.
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