Oxidative dehydrogenation of isobutane on MCM-41 mesoporous molecular sieves

被引:40
|
作者
Sulikowski, B
Olejniczak, Z
Wloch, E
Rakoczy, J
Valenzuela, RX
Corberán, VC
机构
[1] Polish Acad Sci, Inst Catalysis & Surface Chem, PL-30239 Krakow, Poland
[2] CSIC, Inst Catalisis & Petr Quim, Madrid 28049, Spain
[3] Krakow Univ Technol, PL-31155 Krakow, Poland
[4] Inst Nucl Phys, PL-31342 Krakow, Poland
关键词
oxidative dehydrogenation; isobutane; MCM-41; V-51; NMR; vanadium species;
D O I
10.1016/S0926-860X(02)00102-3
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
MCM-41 mesoporous molecular sieves containing silicon and vanadium have been prepared by a direct hydrothermal route. Aluminium-containing [Si,Al]-MCM-41 and purely siliceous [Si]-MCM-41 solids were synthesised for comparison purposes. 51 V static and magic-angle-spinning NMR studies of [Si,V] -MCM-41 showed one type of VO4 in the as-prepared samples (site I) and two types of monodispersed and distorted to various extent VO4 tetrahedra, chemically bound to the walls of MCM-41 (sites IVa and IVb), in the calcined and rehydrated samples. NMR parameters of vanadium units are given. The catalytic performance of MCM-41 materials was probed in the oxidative dehydrogenation (ODH) of isobutane. The highest selectivities to isobutene (48-59%) were observed for the [Si,V]-MCM-41 materials with Si/V = 85 and 30, respectively. On the contrary, a sample containing V2O5 bulk-like species exhibited much lower selectivity to isobutene, especially at the isobutane conversion higher than 5%. The presence of isolated vanadium species, as found by 51 V NMR, was responsible for the high olefin selectivity in the ODH of isobutane. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:189 / 202
页数:14
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