Preparation of MoO3/SiO2-Al2O3 metathesis catalysts via wet impregnation with different Mo precursors

被引:73
作者
Debecker, Damien P. [1 ]
Stoyanova, Mariana [2 ]
Rodemerck, Uwe [2 ]
Gaigneaux, Eric M. [1 ]
机构
[1] Catholic Univ Louvain, Inst Condensed Matter & Nanosci MOl Solids & Reac, IMCN MOST, B-1348 Louvain, Belgium
[2] Univ Rostock, Leibniz Inst Katalyse eV, D-18059 Rostock, Germany
关键词
Propylene; Alkene metathesis; Anderson-type alumino heteropolymolybdate; Peroxopolymolybdate; Alumino-silicate; OLEFIN METATHESIS; THIN-FILMS; SPECTROSCOPIC CHARACTERIZATION; RAMAN-SPECTROSCOPY; ALUMINA CATALYSTS; MOLYBDENA-ALUMINA; MESOPOROUS SILICA; PROPENE; MORPHOLOGY; COMPLEXES;
D O I
10.1016/j.molcata.2011.03.011
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
Molybdenum oxide supported on mesoporous silica-alumina is an efficient catalyst for the light olefins metathesis. Preparation via the classical wet impregnation with ammonium heptamolybdate (AHM) suffers from several downsides related to the control of the species formed on the surface and the build up of inactive species (MoO3 crystals and Al-2(MoO4)(3)). This study explores the synthesis, properties and propene metathesis activity of MoO3/SiO2-Al2O3 catalysts prepared with two Mo precursors chosen as alternatives to AHM. Characterization is done on the precursor solutions, on the dried catalyst precursors and on the calcined catalysts (ICP-AES, N-2-physisorption, XRD, Raman spectroscopy, XPS and Al-27 MAS NMR). Firstly, oxalic acid is used as an additive with the objective to perturb the Mo speciation in the AHM impregnation solution. It affects the catalysts texture and impedes the formation of Al-2(MoO4)(3). Samples are totally amorphous and outcompete the reference samples prepared with AHM. Secondly, a molybdenum oxide hydrates solution is used as impregnation solution. The MoO3 phase formed is also totally amorphous, the texture is preserved, the spreading of the Mo phase is enhanced and the activity is high. However, at high Mo loading the build-up of Al-2(MoO4)(3) provokes a decrease in activity. (C) 2011 Elsevier B.V. All rights reserved.
引用
收藏
页码:65 / 76
页数:12
相关论文
共 67 条
[1]   HDS of 4,6-dimethyldibenzothiophene over MoS2 catalysts supported on macroporous carbon coated with aluminosilicate nanoparticles [J].
Aridi, Toufic N. ;
Al-Daous, Mohammed A. .
APPLIED CATALYSIS A-GENERAL, 2009, 359 (1-2) :180-187
[2]   Comparison of the conventional impregnation method using ammonium heptamolybdate with a simple route to silica-supported molybdenum(VI) materials [J].
Bakala, Paul Celestin ;
Briot, Emmanuel ;
Piquemal, Jean-Yves ;
Bregeault, Jean-Marie ;
Beaunier, Patricia .
CATALYSIS COMMUNICATIONS, 2007, 8 (10) :1447-1451
[3]   Comparison of liquid-phase olefin epoxidation over MoOx inserted within mesoporous silica (MCM-41, SBA-15) and grafted onto silica [J].
Bakala, PC ;
Briot, E ;
Salles, L ;
Brégeault, JM .
APPLIED CATALYSIS A-GENERAL, 2006, 300 (02) :91-99
[4]  
Balcar H, 2007, NATO SCI SER II-MATH, V243, P151
[5]   Molybdenum oxide catalysts for metathesis of higher 1-alkenes via supporting MoO2(acetylacetonate)2 and MoO2(glycolate)2 on SBA-15 mesoporous molecular sieves [J].
Balcar, Hynek ;
Mishra, Diwa ;
Marceau, Eric ;
Carrier, Xavier ;
Zilkova, Nadezda ;
Bastl, Zdenek .
APPLIED CATALYSIS A-GENERAL, 2009, 359 (1-2) :129-135
[6]   INVESTIGATION AND MODELING OF THE GAMMA-AL2O3/WATER SYSTEM [J].
BAUMGARTEN, E ;
GELDSETZER, FO ;
KIRCHHAUSENDUSING, U .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 1995, 173 (01) :104-111
[7]   Vibrational spectra of eight-coordinate niobium and tantalum complexes with peroxo ligands: A theoretical simulation [J].
Bayot, D ;
Devillers, M ;
Peeters, D .
EUROPEAN JOURNAL OF INORGANIC CHEMISTRY, 2005, (20) :4118-4123
[8]   Spectroscopic and structural characterizations of ammonium peroxo-carboxylato molybdate(VI) complexes [J].
Bayot, D ;
Tinant, B ;
Devillers, M .
INORGANICA CHIMICA ACTA, 2004, 357 (03) :809-816
[9]   Investigations of reasons for the deactivation of rhenium oxide alumina catalyst in the metathesis of pentene-1 [J].
Behr, A. ;
Schueller, U. ;
Bauer, K. ;
Maschmeyer, D. ;
Wiese, K. -D. ;
Nierlich, F. .
APPLIED CATALYSIS A-GENERAL, 2009, 357 (01) :34-41
[10]   MO(VI) OXALATE COMPLEXES [J].
BELTRAN, A ;
CATURLA, F ;
CERVILLA, A ;
BELTRAN, J .
JOURNAL OF INORGANIC & NUCLEAR CHEMISTRY, 1981, 43 (12) :3277-3282