Effects of pore diameter on particle size, phase, and turnover frequency in mesoporous silica supported cobalt Fischer-Tropsch catalysts

被引:75
作者
Ghampson, I. T. [2 ,3 ,5 ]
Newman, C. [1 ,5 ]
Kong, L. [1 ,5 ]
Pier, E. [1 ,5 ]
Hurley, K. D. [2 ,5 ]
Pollock, R. A. [3 ,5 ,6 ]
Walsh, B. R. [3 ,4 ,5 ]
Goundie, B. [3 ,5 ]
Wright, J. [3 ,5 ]
Wheeler, M. C. [2 ,5 ]
Meulenberg, R. W. [3 ,5 ,6 ]
DeSisto, W. J. [2 ,3 ,5 ,6 ]
Frederick, B. G. [3 ,4 ,5 ]
Austin, R. N. [1 ,5 ]
机构
[1] Bates Coll, Dept Chem, Lewiston, ME 04240 USA
[2] Univ Maine, Dept Chem & Biol Engn, Orono, ME 04469 USA
[3] Univ Maine, Surface Sci & Technol Lab, Orono, ME 04469 USA
[4] Univ Maine, Dept Chem, Orono, ME 04469 USA
[5] Univ Maine, Forest Bioprod Res Inst, Orono, ME 04469 USA
[6] Univ Maine, Dept Phys & Astron, Orono, ME 04469 USA
关键词
Fischer-Tropsch synthesis; Co heterogeneous catalyst; MCM-41; MCM-48; HMS; SBA15; X-ray diffraction; Turnover frequency; Pore size; X-RAY-ABSORPTION; MOLECULAR-SIEVES; MCM-41; DEACTIVATION; ADSORPTION; OXIDATION; CRYSTALLITES; HYDROCARBONS; STABILITY; ALUMINA;
D O I
10.1016/j.apcata.2010.08.028
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
A series of mesoporous silica supported cobalt catalysts for the Fischer-Tropsch reaction with pore diameters from 3 to 22 urn was synthesized and characterized. Detailed X-ray diffraction measurements were used to determine the composition and particle diameters of the metal fraction, analyzed as a three-phase system containing Co-fcc, Co-hcp, and CoO. Catalyst properties were determined at three stages of catalyst history: (1) after the initial calcination step to thermally decompose the catalyst precursor into Co3O4, (2) after the hydrogen reduction step to activate the catalyst to Co and (3) after the FT reaction. Small Co-hcp particles were detected in all reduced catalysts contributing significantly to the Co surface area. The reaction rate increased with the pore diameter of the silica support. The results indicate the importance of careful catalyst characterization in determining die factors that contribute to reactivity. In addition, the identification of significant quantities of two cobalt metal phases suggests that further study of the intrinsic activity of each phase, as well as the structural features of the supports that determine the distribution of cobalt phases and particle sizes is warranted. (C) 2010 Elsevier B.V. All rights reserved.
引用
收藏
页码:57 / 67
页数:11
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