A non-hydrolytic sol-gel route to highly active MoO3-SiO2-Al2O3 metathesis catalysts

被引:45
作者
Debecker, Damien P. [1 ]
Bouchmella, Karim [2 ]
Stoyanova, Mariana [3 ]
Rodemerck, Uwe [3 ]
Gaigneaux, Eric M. [1 ]
Mutin, P. Hubert [2 ]
机构
[1] Catholic Univ Louvain, Inst Condensed Matter & Nanosci MOl Solids & Reac, B-1348 Louvain, Belgium
[2] Univ Montpellier 2, Inst Charles Gerhardt, UMR 5253, CNRS,UM2,ENSCM,UM1, F-34095 Montpellier, France
[3] Univ Rostock, Leibniz Inst Katalyse eV, D-18059 Rostock, Germany
关键词
SUPPORTED MOLYBDENUM OXIDE; SILICA-ALUMINA; OLEFIN METATHESIS; HETEROGENEOUS CATALYSTS; RAMAN-SPECTROSCOPY; ACIDIC PROPERTIES; OXIDATION; TITANIA; PROPENE; SURFACE;
D O I
10.1039/c2cy00475e
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
MoO3-based materials are known to be appropriate catalysts for the heterogeneous metathesis of light olefins. Classical preparation methods involve the deposition of a Mo oxide phase on the surface of preformed support via impregnation, grafting or thermal spreading. An alternative sol-gel approach for the elaboration of Mo-based catalysts is presented in this article. Mesoporous ternary Si-Al-Mo mixed oxides are prepared in one step, via non-hydrolytic condensation of chloride precursors in non-aqueous media. After calcination, effective catalysts with very good textures and highly dispersed surface molybdenum species are obtained. The Si/Al ratio influences both the texture and the acidity of the materials, which significantly affects the propene self-metathesis activity. The activity also increases with the MoO3 content. The best catalysts with optimized composition significantly outperform the catalysts prepared by other
引用
收藏
页码:1157 / 1164
页数:8
相关论文
共 51 条
[1]   Structural change of molybdenum on silica-alumina in contact with propene studied by ESR and Mo LIII-edge XANES [J].
Aritani, H ;
Fukuda, O ;
Miyaji, A ;
Hasegawa, S .
APPLIED SURFACE SCIENCE, 2001, 180 (3-4) :261-269
[2]   Silica-alumina-supported molybdena catalyst for propene metathesis [J].
Aritani, H ;
Fukuda, O ;
Yamamoto, T ;
Tanaka, T ;
Imamura, S .
CHEMISTRY LETTERS, 2000, (01) :66-67
[3]  
Baiker A, 1998, CHIMIA, V52, P517
[4]   OLEFIN DISPROPORTIONATION - NEW CATALYTIC PROCESS [J].
BANKS, RL ;
BAILEY, GC .
INDUSTRIAL & ENGINEERING CHEMISTRY PRODUCT RESEARCH AND DEVELOPMENT, 1964, 3 (03) :170-&
[5]   Physical techniques and catalyst preparation: Determining the interactions of transition-metal complexes with oxide surfaces [J].
Carrier, Xavier ;
Marceau, Eric ;
Che, Michel .
PURE AND APPLIED CHEMISTRY, 2006, 78 (05) :1039-1055
[6]   Non-hydrolytic synthesis of mesoporous silica-titania catalysts for the mild oxidation of sulfur compounds with hydrogen peroxide [J].
Cojocariu, Ana Mihaela ;
Mutin, P. Hubert ;
Dumitriu, Emil ;
Fajula, Francois ;
Vioux, Andre ;
Hulea, Vasile .
CHEMICAL COMMUNICATIONS, 2008, (42) :5357-5359
[7]   Spectroscopic characterization of an MoOx layer on the surface of silica.: An evaluation of the molecular designed dispersion method [J].
Collart, O ;
Van der Voort, P ;
Vansant, EF ;
Gustin, E ;
Bouwen, A ;
Schoemaker, D ;
Rao, RR ;
Weckhuysen, BM ;
Schoonheydt, RA .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 1999, 1 (17) :4099-4104
[8]   One-Pot Aerosol Route to MoO3-SiO2-Al2O3 Catalysts with Ordered Super Microporosity and High Olefin Metathesis Activity [J].
Debecker, Damien P. ;
Stoyanova, Mariana ;
Colbeau-Justin, Frederic ;
Rodemerck, Uwe ;
Boissiere, Cedric ;
Gaigneaux, Eric M. ;
Sanchez, Clement .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 2012, 51 (09) :2129-2131
[9]   Genesis of active and inactive species during the preparation of MoO3/SiO2-Al2O3 metathesis catalysts via wet impregnation [J].
Debecker, Damien P. ;
Stoyanova, Mariana ;
Rodemerck, Uwe ;
Leonard, Alexandre ;
Su, Bao-Lian ;
Gaigneaux, Eric M. .
CATALYSIS TODAY, 2011, 169 (01) :60-68
[10]   Preparation of MoO3/SiO2-Al2O3 metathesis catalysts via wet impregnation with different Mo precursors [J].
Debecker, Damien P. ;
Stoyanova, Mariana ;
Rodemerck, Uwe ;
Gaigneaux, Eric M. .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2011, 340 (1-2) :65-76