Uniformly Dispersed Cu Nanoparticles over Mesoporous Silica as a Highly Selective and Recyclable Ethanol Dehydrogenation Catalyst

Selective dehydrogenation of ethanol to acetaldehyde has been considered as an important pathway to produce acetaldehyde due to the atom economy and easy separation of acetaldehyde and hydrogen. Copper catalysts have attracted much attention due to the high activity of Cu species in O-H and C-H bond...

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Bibliographic Details
Published inCatalysts Vol. 12; no. 9; p. 1049
Main Authors Hao, Yan, Zhao, Dajie, Liu, Wen, Zhang, Min, Lou, Yixiao, Wang, Zhenzhen, Tang, Qinghu, Yang, Jinghe
Format Journal Article
LanguageEnglish
Published Basel MDPI AG 01.09.2022
Subjects
Acetaldehyde
Acetates
Acetic acid
Adsorption
Alcohol
Alcohol, Denatured
Ammonia
Catalysts
Chemical reactions
Copper
Dehydrogenation
Dispersion
Ethanol
ethanol dehydrogenation
Ethylene
High temperature
mesoporous silica
Metal oxides
Morphology
Nanoparticles
Oxidation
Particle size
Pore size
Selectivity
Silica
Valence
China
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Summary:Selective dehydrogenation of ethanol to acetaldehyde has been considered as an important pathway to produce acetaldehyde due to the atom economy and easy separation of acetaldehyde and hydrogen. Copper catalysts have attracted much attention due to the high activity of Cu species in O-H and C-H bonds oxidative cleavage, and low process cost; however, the size of the Cu nanoparticle is difficult to control since it is easily suffers from metal sintering at high temperatures. In this work, the Cu/KIT-6 catalyst exhibited an ultra-high metal dispersion of 62.3% prepared by an electrostatic adsorption method, due to the advantages of the confinement effect of mesoporous nanostructures and the protective effect of ammonia water on Cu nanoparticles. The existence of an oxidation atmosphere had a significant effect on the valence state of copper species and enhancing moderate acid sites. The catalyst treated by reduction and then oxidation possessed a moderate/weak acid site ratio of ~0.42 and a suitable proportion of Cu+/Cu0 ratio of ~0.53, which conceivably rendered its superior ethanol conversion of 96.8% and full acetaldehyde selectivity at 250 °C. The catalyst also maintained a high selectivity of >99% to acetaldehyde upon time-on-stream of 288 h.
ISSN:2073-4344
2073-4344
DOI:10.3390/catal12091049