Core-shell Cu[at](CuCo-alloy)/Al sub(2)O sub(3) catalysts for the synthesis of higher alcohols from syngas

The production of higher alcohols by the catalytic conversion of synthesis gas (CO + H sub(2)) is one of the most promising approaches for the utilization of nonoil resources, in which bimetallic catalysts based on Cu and Fischer-Tropsch (FT) reaction active elements (e.g. Co, Fe, Ni) are efficient...

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Published in:Green chemistry : an international journal and green chemistry resource : GC 2015-03, Vol.17 (3), p.1525-1534
Main Authors: Gao, Wa, Zhao, Yufei, Chen, Haoran, Chen, Hao, Li, Yinwen, He, Shan, Zhang, Yingkui, Wei, Min, Evans, David G, Duan, Xue
Format: Article
Language:English
Subjects:
ALCOHOLS
ALUMINUM OXIDE
BIMETALS
Carbon monoxide
Catalysis
CATALYSTS
Copper
Hydrogenation
PARTICLE SIZE AND SHAPE
PARTICLES
X RAY SPECTROSCOPY
X-ray photoelectron spectroscopy
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Summary:The production of higher alcohols by the catalytic conversion of synthesis gas (CO + H sub(2)) is one of the most promising approaches for the utilization of nonoil resources, in which bimetallic catalysts based on Cu and Fischer-Tropsch (FT) reaction active elements (e.g. Co, Fe, Ni) are efficient and cost-effective candidates. Herein, we demonstrate the fabrication of core-shell Cu[at](CuCo-alloy) nanoparticles (NPs) embedded on a Al sub(2)O sub(3) matrix via an in situ growth of CuCoAl-LDH nanoplatelets on aluminum substrates followed by a calcination-reduction process, and they serve as efficient catalysts toward CO hydrogenation to produce higher alcohols. The composition, particle size and shell thickness can be tuned by changing the Cu/Co molar ratio in the LDH precursors, and the best catalytic behavior was obtained over the Cu/Co (1/2) catalyst with a CO conversion of 21.5% and a selectivity (C sub(6+) slate 1-alcohols) of 48.9%, which is superior to the traditional modified FT catalysts. XPS, in situ FTIR spectroscopy and HAADF-STEM revealed that the unique electronic and geometric interaction between Cu and Co in the Cu[at](CuCo-alloy) NPs contributes to the significantly enhanced catalytic performances. In addition, the 3D hierarchical structure of the Cu[at](CuCo-alloy)/Al sub(2)O sub(3) catalyst facilitates mass diffusion/transportation as well as prevents hotspot formation, accounting for its stability and recyclability. The Cu[at](CuCo-alloy)/Al sub(2)O sub(3) catalyst with significantly improved catalytic behavior can be potentially used in CO hydrogenation to produce higher alcohols.
ISSN:1463-9262
1463-9270
DOI:10.1039/c4gc01633e