Ni and Mo interaction with Al-containing MCM-41 support and its effect on the catalytic behavior in DBT hydrodesulfurization

被引:137
|
作者
Klimova, T [1 ]
Calderón, M [1 ]
Ramírez, J [1 ]
机构
[1] Univ Nacl Autonoma Mexico, Fac Quim, Dept Ingn Quim, UNICAT, Mexico City 04510, DF, Mexico
关键词
hydrodesulfurization; Mo and NiMo catalysts; Al-MCM-41; characterization; interaction; bifunctional catalysts;
D O I
10.1016/S0926-860X(02)00417-9
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 Mo and NiMo catalysts supported on Al-containing MCM-41 was prepared and characterized by N-2 physisorption, XRD, ammonia TPD, temperature programmed reduction (TPR), UV-Vis diffuse reflectance spectroscopy (DRS) and (27)AlMAS-NMR. It was shown that the incorporation of Al atoms into the siliceous MCM-41 framework causes a deterioration of the textural characteristics and some loss in the periodicity of the MCM-41 pore structure. However, the acidity of the Al-containing MCM-41 is substantially higher. The dispersion of Mo and Ni oxidic species increases with the incorporation of aluminum in the MCM-41 support due to the strong interaction of Mo and Ni oxidic species with aluminum atoms of the support. However, the strong interaction of metal species with the Al-containing MCM-41 supports, up to the. formation of Al-2(MoO4)(3) in the case of unpromoted Mo catalysts, produces an increase in the proportion of Ni and Mo species difficult to reduce. When Ni and Mo are impregnated simultaneously the formation of Al-2(MoO4)(3) is prevented because of the competitive interaction of both, Ni and Mo species, with Al atoms of the support. For both, Mo and NiMo catalysts, maximum catalytic activity in dibenzothiophene (DBT) hydrodesulfurization is observed for the catalysts supported on Al-MCM-41 with SiO2/Al2O3 molar ratio of 30. When Al-containing MCM-41 is used as a support for NiMo catalyst, some cracking of the main reaction products (biphenyl (BiP), cyclohexylbenzene (CHB) and dicyclohexyl (DCH)) is observed. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:29 / 40
页数:12
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