Modification of MCM-48-, SBA-15-, MCF-, and MSU-type mesoporous silicas with transition metal oxides using the molecular designed dispersion method

被引:82
作者
Kustrowski, P
Chmielarz, L
Dziembaj, R
Cool, P
Vansant, EF
机构
[1] Jagiellonian Univ, Fac Chem, PL-30060 Krakow, Poland
[2] Univ Instelling Antwerp, Dept Chem, Lab Adsorpt & Catalysis, B-2610 Antwerp, Belgium
关键词
D O I
10.1021/jp050696o
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
Four various mesoporous silicas (MCM-48, SBA-15, MCF, and MSU) were modified by the molecular designed dispersion method using Fe(acac)(3), Cr(acac)(3), and Cu(acac)2 complexes. The deposition was performed at the same concentration of the metal acetylacetonate (acac) complex in a toluene solution. All as-synthesized samples were investigated by diffuse reflectance infrared Fourier transform spectroscopy, Fourier transform infrared photoacoustic spectroscopy, and thermogravimetric analysis. The calcined materials were studied with respect to their textural properties (Brunauer-Emmett-Teller adsorption isotherm) and chemical composition (electron microprobe analysis). It allowed elucidation of the mechanism of interaction between the acac complex and the silanol groups. For the MCM-48, SBA-15, and MCF materials, the formation of hydrogen bonding was found for the chromium- and copper-modified samples, whereas the Fe-containing materials showed the ligand exchange mechanism. The strong interaction of the MSU support and the different acetylacetonate complexes, resulting in a loss of at least one acac ligand, was observed. The mesoporous silicas modified with transition metal oxides were studied by UV-vis-DR spectroscopy. The different metal dispersions were found for the samples containing various transition metal oxides.
引用
收藏
页码:11552 / 11558
页数:7
相关论文
共 40 条
[1]   Synthesis of supported transition metal oxide catalysts by the designed deposition of acetylacetonate complexes [J].
Baltes, M ;
Collart, O ;
Van der Voort, P ;
Vansant, EF .
LANGMUIR, 1999, 15 (18) :5841-5845
[2]   The adsorption of VO(acac)2 on a mesoporous silica support by liquid phase and gas phase modification to prepare supported vanadium oxide catalysts [J].
Baltes, M ;
Van Der Voort, P ;
Collart, O ;
Vansant, EF .
JOURNAL OF POROUS MATERIALS, 1998, 5 (3-4) :317-324
[3]   A NEW FAMILY OF MESOPOROUS MOLECULAR-SIEVES PREPARED WITH LIQUID-CRYSTAL TEMPLATES [J].
BECK, JS ;
VARTULI, JC ;
ROTH, WJ ;
LEONOWICZ, ME ;
KRESGE, CT ;
SCHMITT, KD ;
CHU, CTW ;
OLSON, DH ;
SHEPPARD, EW ;
MCCULLEN, SB ;
HIGGINS, JB ;
SCHLENKER, JL .
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY, 1992, 114 (27) :10834-10843
[4]   Structure and reactivity of framework and extraframework iron in Fe-silicalite as investigated by spectroscopic and physicochemical methods [J].
Bordiga, S ;
Buzzoni, R ;
Geobaldo, F ;
Lamberti, C ;
Giamello, E ;
Zecchina, A ;
Leofanti, G ;
Petrini, G ;
Tozzola, G ;
Vlaic, G .
JOURNAL OF CATALYSIS, 1996, 158 (02) :486-501
[5]   ADSORPTION AND REACTIVITY OF NO ON COPPER-ON-ALUMINA CATALYSTS .1. FORMATION OF NITRATE SPECIES AND THEIR INFLUENCE ON REACTIVITY IN NO AND NH3 CONVERSION [J].
CENTI, G ;
PERATHONER, S ;
BIGLINO, D ;
GIAMELLO, E .
JOURNAL OF CATALYSIS, 1995, 152 (01) :75-92
[6]   Effect of two-step sol-gel reaction on the mesoporous silica structure [J].
Choi, DG ;
Yang, SM .
JOURNAL OF COLLOID AND INTERFACE SCIENCE, 2003, 261 (01) :127-132
[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]   A high-yield reproducible synthesis of MCM-48 starting from fumed silica [J].
Collart, O ;
Van Der Voort, P ;
Vansant, EF ;
Desplantier, D ;
Galarneau, A ;
Di Renzo, F ;
Fajula, F .
JOURNAL OF PHYSICAL CHEMISTRY B, 2001, 105 (51) :12771-12777
[9]   Chromia/zirconia catalysts with Cr content exceeding the monolayer. A comparison with chromia/alumina and chromia/silica for isobutane dehydrogenation [J].
De Rossi, S ;
Casaletto, MP ;
Ferraris, G ;
Cimino, A ;
Minelli, G .
APPLIED CATALYSIS A-GENERAL, 1998, 167 (02) :257-270
[10]   Characterization of chromium species in catalysts for dehydrogenation and polymerization [J].
Gaspar, AB ;
Brito, JLF ;
Dieguez, LC .
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2003, 203 (1-2) :251-266