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
[51]   Morphology and orientation of MoS2 clusters on Al2O3 and TiO2 supports and their effect on catalytic performance [J].
Shimada, H .
CATALYSIS TODAY, 2003, 86 (1-4) :17-29
[52]  
SONG C, 1996, PREPR AM CHEM SOC DI, V41, P567
[53]   Fuel processing for low-temperature and high-temperature fuel cells - Challenges, and opportunities for sustainable development in the 21st century [J].
Song, CS .
CATALYSIS TODAY, 2002, 77 (1-2) :17-49
[54]   INSITU MOSSBAUER EMISSION-SPECTROSCOPY STUDIES OF UNSUPPORTED AND SUPPORTED SULFIDED CO-MO HYDRODESULFURIZATION CATALYSTS - EVIDENCE FOR AND NATURE OF A CO-MO-S PHASE [J].
TOPSOE, H ;
CLAUSEN, BS ;
CANDIA, R ;
WIVEL, C ;
MORUP, S .
JOURNAL OF CATALYSIS, 1981, 68 (02) :433-452
[55]   EVIDENCE OF BRONSTED ACIDITY ON SULFIDED PROMOTED AND UNPROMOTED MO/AL2O3 CATALYSTS [J].
TOPSOE, NY ;
TOPSOE, H ;
MASSOTH, FE .
JOURNAL OF CATALYSIS, 1989, 119 (01) :252-255
[56]   CHARACTERIZATION OF THE STRUCTURES AND ACTIVE-SITES IN SULFIDED CO-MO/AL2O3 AND NI-MO/AL2O3 CATALYSTS BY NO CHEMISORPTION [J].
TOPSOE, NY ;
TOPSOE, H .
JOURNAL OF CATALYSIS, 1983, 84 (02) :386-401
[57]   FTIR STUDIES OF MO/AL2O3-BASED CATALYSTS .2. EVIDENCE FOR THE PRESENCE OF SH-GROUPS AND THEIR ROLE IN ACIDITY AND ACTIVITY [J].
TOPSOE, NY ;
TOPSOE, H .
JOURNAL OF CATALYSIS, 1993, 139 (02) :641-651
[58]   Nanometric monodispersed titanium oxide particles on mesoporous silica: synthesis, characterization, and catalytic activity in oxidation reactions in the liquid phase [J].
Tuel, A ;
Hubert-Pfalzgraf, LG .
JOURNAL OF CATALYSIS, 2003, 217 (02) :343-353
[59]   MCM-41-supported Co-Mo catalysts for deep hydrodesulfurization of light cycle oil [J].
Turaga, UT ;
Song, CS .
CATALYSIS TODAY, 2003, 86 (1-4) :129-140
[60]   Influence of the preparation method on the thiophene HDS activity of silica supported CoMo catalysts [J].
Venezia, AM ;
La Parola, V ;
Deganello, G ;
Cauzzi, D ;
Leonardi, G ;
Predieri, G .
APPLIED CATALYSIS A-GENERAL, 2002, 229 (1-2) :261-271