Product distribution change in the early stages of carbon monoxide hydrogenation over cobalt magnesium Fischer-Tropsch catalyst

被引:9
|
作者
Melaet, Gerome [1 ,3 ]
Ralston, Walter T. [1 ,2 ]
Liu, Wen-Chi [1 ,3 ]
Somorjai, Gabor A. [1 ,2 ,3 ]
机构
[1] Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA
[2] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA
[3] Univ Calif Berkeley, Lawrence Berkeley Natl Lab, Div Mat Sci, Berkeley, CA 94720 USA
关键词
Fischer-Tropsch synthesis; CO hydrogenation; Cobalt; Transient experiments; Time-resolved; Temporal analysis of products; PARTICLE-SIZE; TRANSIENT KINETICS; CO HYDROGENATION; SYNTHESIS GAS;
D O I
10.1016/j.cattod.2016.03.027
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The catalytic hydrogenation of carbon monoxide, known as the Fischer-Tropsch process, is a technologically important, complex multipath reaction which produces long chain hydrocarbons. In order to access the initial kinetics and the mechanism, we developed a reactor that provides information under non-steady state conditions. We tested a CoMgO catalyst and monitored the initial product formation within 2 s of exposure to CO as well as the time dependence of high molecular weight products (in a 60 s window) and found drastic changes in the product selectivity. The probability for forming branched isomers (C-4 and C-5) peaks in the first 25 s, and within that time frame no unsaturated products were detected. The subsequent decline (at 35 to 40 s) of branched isomers coincides with the detection of olefins (from C-2 to C-5) and the change in carbon coverage at the surface of the catalyst. This indicates a change in the reaction pathway. (C) 2016 Elsevier B.V. All rights reserved.
引用
收藏
页码:69 / 73
页数:5
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