CoMo/Ti-SBA-15 catalysts for dibenzothiophene desulfurization

被引:102
作者
Nava, R.
Ortega, R. A.
Alonso, G.
Ornelas, C.
Pawelec, B.
Fierro, J. L. G.
机构
[1] Univ Nacl Autonoma Mexico, CFATA, Queretaro 76000, Mexico
[2] Univ Nacl Autonoma Mexico, Fac Quim, Mexico City 76010, DF, Mexico
[3] SC Complejo Ind Chihuahua, CIMAV, Chihuahua 3109, Mexico
[4] CSIC, Inst Catalisis & Petroleoquim, E-28049 Madrid, Spain
关键词
CoMo; Ti-SBA-15; MCM-41; SBA-15; dibenzothiophene; hydrodesulfurization;
D O I
10.1016/j.cattod.2007.02.034
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
With a view to reducing the sulfur content in diesel fuels, novel desulfurization CoMo catalysts were supported on a Ti-loaded hexagonal mesoporous SBA-15 material. The Ti-SBA-15 substrates were synthesized using triblock copolymers as structure-directing agents. Catalytic activity was assessed in the model reaction of hydrodesuffurization (HDS) of dibenzothiophene (DBT), carried out in a batch reactor at T = 623 K and with a total hydrogen pressure of 3.1 MPa. The reaction proceeds via the direct desulfurization route (main route) and the hydrogenation (HYD) pathway. The incorporation of Ti into the SBA-15 afforded catalysts that were more active than the Ti-free counterpart, due to the enhancement of the DDS route in this reaction. This difference was explained in terms of a larger number of coordinately unsaturated sites (CUS) of the metal sulfide on Ti-loaded catalysts. Under steady-state conditions, the CoMoST20 catalyst with a Si/Ti ratio of 20 was the most active among the catalysts studied. Since this catalyst exhibited both Ti4+ ions incorporated into the SBA-15 framework and separate anatase TiO2 clusters located on its surface, the activity enhancement on this sample was explained by the larger intrinsic activity of the "Co-Mo-S" phase located on these TiO2 nanoparticles. The Ti-SBA-15 supports and the CoMo/Ti-SBA-15 catalysts were studied by N-2 adsorption-desorption isotherms, XRD, TEM, FTIR of adsorbed pyridine and NO, UV-vis DRS, TPR, micro-Raman and XPS spectroscopy. (C) 2007 Elsevier B.V. All rights reserved.
引用
收藏
页码:70 / 84
页数:15
相关论文
共 75 条
[41]   HDS of dibenzothiophene over polyphosphates supported on mesoporous silica [J].
Pawelec, B ;
Damyanova, S ;
Mariscal, R ;
Fierro, JLG ;
Sobrados, I ;
Sanz, J ;
Petrov, L .
JOURNAL OF CATALYSIS, 2004, 223 (01) :86-97
[42]   Studies of molybdenum sulfide catalyst ex ammonium tetrathiomolybdate: effect of pretreatment on hydrodesulfurization of dibenzothiophene [J].
Pawelec, B ;
Navarro, R ;
Fierro, JLG ;
Vasudevan, PT .
APPLIED CATALYSIS A-GENERAL, 1998, 168 (02) :205-217
[43]   Hydrotreating catalysts containing zeolites and related materials -: mechanistic aspects related to deep desulfurization [J].
Pérot, G .
CATALYSIS TODAY, 2003, 86 (1-4) :111-128
[44]   PHOTOACOUSTIC-SPECTROSCOPY OF PYRIDINE CHEMISORBED ON CALCINED AND SULFIDED MOLYBDENUM CATALYSTS [J].
RISEMAN, SM ;
BANDYOPADHYAY, S ;
MASSOTH, FE ;
EYRING, EM .
APPLIED CATALYSIS, 1985, 16 (01) :29-37
[45]   Hydrodesulfurization of dibenzothiophene on MoS2/MCM-41 and MoS2/SBA-15 catalysts prepared by thermal spreading of MoO3 [J].
Sampieri, A ;
Pronier, S ;
Blanchard, J ;
Breysse, M ;
Brunet, S ;
Fajerwerg, K ;
Louis, C ;
Pérot, G .
CATALYSIS TODAY, 2005, 107-08 :537-544
[46]  
Sawant KR, 2002, STUD SURF SCI CATAL, V141, P53
[47]   Hydrodesulfurization activity of CoMo catalysts supported on stabilized TiO2 [J].
Schacht, P ;
Hernández, G ;
Cedeño, L ;
Mendoza, JH ;
Ramírez, S ;
García, L ;
Ancheyta, J .
ENERGY & FUELS, 2003, 17 (01) :81-86
[48]  
SCHOONHEYDT RA, 1984, CHARACTERIZATION HET, P125
[49]   Oxide loaded ordered mesoporous oxides for catalytic applications [J].
Schüth, F ;
Wingen, A ;
Sauer, J .
MICROPOROUS AND MESOPOROUS MATERIALS, 2001, 44 :465-476
[50]  
Seah M.P., 1990, PRACTICAL SURFACE AN