Use of different mesostructured materials based on silica as cobalt supports for the Fischer-Tropsch synthesis

被引:70
作者
Gonzalez, O. [1 ]
Perez, H. [2 ]
Navarro, P. [2 ]
Almeida, L. C. [2 ]
Pacheco, J. G. [3 ]
Montes, M. [2 ]
机构
[1] INASMET TECNALIA, Energy Unit, E-20009 San Sebastian, Spain
[2] Univ Basque Country, Dept Appl Chem, E-20018 San Sebastian, Spain
[3] Univ Juarez Autonoma Tabasco, Div Acad Ciencias Basicas, Cunduacan 86690, Tabasco, Mexico
关键词
Fischer-Tropsch synthesis; SBA-15; Al-MCM-41; INT-MM1; Mesoporous support; Supported cobalt catalysts; MESOPOROUS MATERIALS; CATALYTIC-PROPERTIES; HYDROCARBONS; ALUMINA; SBA-15; REDUCIBILITY; ADSORPTION; BEHAVIOR; CO/SIO2; MCM-41;
D O I
10.1016/j.cattod.2009.03.030
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
To obtain a novel, active and selective to diesel catalytic material for syngas processing via Fischer-Tropsch synthesis (FTS), a series of 20 wt.% cobalt catalysts has been prepared by impregnation of a mesoporous molecular sieve based on silica (SBA-15, Al-MCM-41, INT-MM1), and a commercial amorphous silica forcomparison purposes. All materials were characterized by several physico-chemical techniques: AAS, BET surface area, XRD, TPR, and H(2) chemisorption with pulse reoxidation and finally their reactivity on the FTS reaction was evaluated at 523 K, 10 bar, and H(2/)CO = 2. Catalytic and characterization results show a great influence of mesoporous support porosity on the structure, reducibility, and FTS catalytic behavior of cobalt oxide species supported over these ordered materials. It was found that the size of supported cobalt oxide species formed during the calcination step increased with the average pore size (D(p)) of the mesoporous support. Thus, the catalyst with larger Co oxide species located in wide pore silica showed to be easily reducible, more active and very selective toward the diesel fraction. It seems to be the case of the Co/SBA-15 solid, which showed to be the most active solid (XCO similar to 63%) when the same mass of catalyst was used. Under CO iso-conversion conditions (XCO similar to 40%), Co/SBA-15 was more selective toward the formation of C(5+) hydrocarbons (similar to 80%. alpha = 0.76) and less selective to CH(4) (similar to 15%). On the contrary, when Al-MCM-41 and INT-MM1 were used as supports, a lower selectivity to C(5+) and CO conversion and higher CH(4) selectivity (similar to 20%) were observed due to the decrease of D(p), of the cobalt oxide species size and the reducibility degree of such species. (C) 2009 Elsevier B.V. All rights reserved.
引用
收藏
页码:140 / 147
页数:8
相关论文
共 46 条
[1]  
Almeida LC, 2007, STUD SURF SCI CATAL, V167, P79
[2]   Catalytic properties of Co/Al2O3 system for hydrocarbon synthesis [J].
Bechara, R ;
Balloy, D ;
Vanhove, D .
APPLIED CATALYSIS A-GENERAL, 2001, 207 (1-2) :343-353
[4]   SUPPORT EFFECTS IN COBALT-BASED FISCHER-TROPSCH CATALYSIS [J].
BESSELL, S .
APPLIED CATALYSIS A-GENERAL, 1993, 96 (02) :253-268
[5]   Fischer-Tropsch synthesis over γ-calumina-supported cobalt catalysts:: Effect of support variables [J].
Borg, Oyvind ;
Erib, Sigrid ;
Blekkan, Edd A. ;
Storsaeter, Solvi ;
Wigum, Hanne ;
Rytter, Erling ;
Holmen, Anders .
JOURNAL OF CATALYSIS, 2007, 248 (01) :89-100
[6]   Study of nickel catalysts supported on silica of low surface area and prepared by reduction of nickel acetate in aqueous hydrazine [J].
Boudjahem, AG ;
Monteverdi, S ;
Mercy, M ;
Bettahar, MM .
JOURNAL OF CATALYSIS, 2004, 221 (02) :325-334
[7]   On a theory of the van der Waals adsorption of gases [J].
Brunauer, S ;
Deming, LS ;
Deming, WE ;
Teller, E .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1940, 62 :1723-1732
[8]   Characterization of cobalt dispersed on the mixed nanoscale alumina and zirconia supports [J].
Burakorn, Tanuchnun ;
Panpranot, Joonjai ;
Mekasuwandumrong, Okorn ;
Chaisuk, Choowong ;
Praserthdam, Piyasan ;
Jongsomjit, Bunjerd .
JOURNAL OF MATERIALS PROCESSING TECHNOLOGY, 2008, 206 (1-3) :352-358
[9]  
CARRAZA J, 1998, Patent No. 5840271
[10]   Characterization and catalytic properties of cobalt supported on delaminated ITQ-6 and ITQ-2 zeolites for the Fischer-Tropsch synthesis reaction [J].
Concepción, P ;
López, C ;
Martínez, A ;
Puntes, VE .
JOURNAL OF CATALYSIS, 2004, 228 (02) :321-332