Abstract
A series of carbon nanotube (CNTs)-supported copper-cobalt catalysts were prepared and investigated in a slurry reactor for their ability to selectively convert syngas into higher carbon number alcohols. The 7.5Cu7.5Co/CNTs catalyst achieved superior selectivity towards the formation of ethanol (30.1%) and C2+ alcohols (57.7%), while the 10Co5Cu/CNTs catalyst exhibited the largest alcohol space-time yield (372.9 mg gcat -1 h-1). However, the pure Cu (15Cu/CNTs) catalyst displayed negligible activity. Cobalt reduction was enhanced in the presence of copper. In addition to the Cu0-Co0 center, Co0-Co2+ also presented dual active sites for higher alcohols synthesis, the Co2+ site could terminate carbon chain growth to produce alcohols. The ratio of Cu/Co considerably influences the metal particle properties-synergistically effecting the active species.
Highlights
The conversion of synthesis gas derived from coal, natural gas or biomass into higher carbon number alcohols is both attractive and challenging to the field of C1 chemistry.[1,2,3] The alcohols obtained from this process can be used as fuel blends or as value-added chemicals in fine chemical synthesis.[4,5] higher alcohols synthesis (HAS) is a prototypical example of reactions that rely on synergistic effects between dual catalytic sites with different functionalities, one active site catalysis CO dissociation, while the second site enables CO non-dissociation centers to form.[6]
The characteristic CNTs peak was observed at a 2θ value of 25.8° and the intensity of peaks decreased gradually as a function of increased cobalt loading
When the Co loading exceeded that of Cu, peaks corresponding to CoO (JCPDS No 65-5474) were observed at very low intensities in these samples
Summary
The conversion of synthesis gas derived from coal, natural gas or biomass into higher carbon number alcohols is both attractive and challenging to the field of C1 chemistry.[1,2,3] The alcohols obtained from this process can be used as fuel blends or as value-added chemicals in fine chemical synthesis.[4,5] higher alcohols synthesis (HAS) is a prototypical example of reactions that rely on synergistic effects between dual catalytic sites with different functionalities, one active site catalysis CO dissociation, while the second site enables CO non-dissociation centers to form.[6]. The 15Co/CNTs catalyst had a considerably higher activity with a CO conversion of 48.8% and a corresponding total alcohol selectivity of 13.4%.
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