Copper–cobalt catalysts supported on mechanically mixed HZSM-5 and γ-Al2O3 for higher alcohols synthesis via carbon monoxide hydrogenation |
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Authors: | Xuan Ge Hang Sun Kun Dong Yanqi Tao Qi Wang Yazhong Chen Genlei Zhang Peng Cui Ye Wang Qinghong Zhang |
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Affiliation: | Anhui Province Key Laboratory of Advanced Catalytic Materials and Reaction Engineering, School of Chemistry and Chemical Engineering, Hefei University of Technology, Hefei 230009 China, Fax: +86-551-62901450, +86-551-62901450 ; State Key Laboratory of Physical Chemistry of Solid Surface, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005 China |
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Abstract: | Mechanically mixed γ-Al2O3 and HZSM-5 (Si/Al = 50) with different mass ratio were utilized as support for Cu–Co higher alcohol synthesis catalysts prepared through incipient wetness impregnation. The textural and structural properties were studied using Ar low temperature adsorption and desorption, H2-temperature programmed reduction (H2-TPR), X-ray diffraction (XRD), X-ray photoelectron spectroscopy (XPS), transmission electron microscope (TEM) and catalytic performance measurements. The results indicated that the mechanically mixed HZSM-5 and γ-Al2O3 supported copper–cobalt catalysts were superior to either γ-Al2O3 or HZSM-5 supported ones with the same metal loading. The results revealed that using HZSM-5 and γ-Al2O3 mechanically mixed benefited the dispersion of metallic phases and stronger synergetic functions between smaller nanoparticles containing copper and/or cobalt, which is essential for HAS from CO hydrogenation. Under working conditions of P = 5.0 MPa, T = 300 °C, V(H2) : V(CO) : V(N2) = 4 : 2 : 1 and GHSV = 7200 mL g−1 h−1, mechanically mixed HZSM-5 and γ-Al2O3 supported catalysts showed higher catalytic activity than those over single support. For CuCo catalysts upon support containing 50.0 wt% HZSM-5 and 50.0 wt% γ-Al2O3, the CO conversion was 21.3% and the C2+ alcohol selectivity was 41.8%.CuCo bimetallic catalysts over the mixed supports showed smaller average particle size, better dispersion of cobalt and copper species, and good activity for higher alcohols synthesis. |
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