Cerium containing MCM-41-type mesoporous materials and their acidic and redox catalytic properties

被引:242
作者
Laha, SC
Mukherjee, P
Sainkar, SR
Kumar, R [1 ]
机构
[1] Natl Chem Lab, Catalysis Div, Pune 411008, Maharashtra, India
[2] Natl Chem Lab, Div Phys Chem, Pune 411008, Maharashtra, India
关键词
synthesis of MCM-41; cerium; catalytic activity; dehydration of cyclohexanol; hydroxylation of 1-naphthol;
D O I
10.1006/jcat.2002.3516
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
The syntheses of cerium containing MCM-41 mesoporous molecular sieves (Ce-MCM-41) were carried out using different hydrothermal methods. However, the Ce-MCM-41 samples were mainly prepared by refluxing the gel mixture at atmospheric pressure under stirring (similar to600 rpm). For comparison, the syntheses were also carried out in autoclave under autogeneous pressure both in static and in stirring conditions. Powder X-ray diffraction (XRD), N-2 adsorption, diffuse reflectance UV-visible (UV-vis) spectroscopy, IR spectroscopy, solid state magic-angle spinning nuclear magnetic resonance spectroscopy, scanning electron microscopy, energy-dispersive X-ray spectrometry (EDX), transmission electron microscopy and thermogravimetric analyses of the samples reveal that well-ordered MCM-41-type mesoporous materials were prepared and Ce is incorporated presumably into the framework position and/or into the walls of silica matrix of MCM-41 structure. The EDX analyses of the samples confirm the presence of Ce in the Ce-MCM-41 samples. Typical XRD patterns of MCM-41-type hexagonal structures and high BET surface areas (983-1414 m(2) g(-1)) with isotherms of type IV of these materials indicate the presence of hexagonal mesopores in the samples. The presence of a strong absorption band centered at ca. 300 nm and the absence of any absorption band at ca. 400 nm in the diffuse reflectance UV-vis spectra indicate the presence of tetra-coordinated cerium in the silica network of Ce-MCM-41 samples. The Ce-MCM-41 samples are active as catalysts for vapor-phase dehydration of cyclohexanol to cyclohexene and hydroxylation of 1-naphthol with aqueous H2O2 and tert-butyl hydroperoxide. :, (C) 2002 Elsevier Science (USA).
引用
收藏
页码:213 / 223
页数:11
相关论文
共 27 条
[1]   Titanosilicate mesoporous molecular sieve MCM-41: Synthesis and characterization [J].
Alba, MD ;
Luan, ZH ;
Klinowski, J .
JOURNAL OF PHYSICAL CHEMISTRY, 1996, 100 (06) :2178-2182
[2]   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
[3]   SYNTHESIS, CHARACTERIZATION, AND CATALYTIC ACTIVITY OF TI-MCM-41 STRUCTURES [J].
BLASCO, T ;
CORMA, A ;
NAVARRO, MT ;
PARIENTE, JP .
JOURNAL OF CATALYSIS, 1995, 156 (01) :65-74
[4]  
Boccuti M.R., 1989, STUD SURF SCI CATAL, P133
[5]   Mesoporous redox molecular sieves analogous to MCM-41 [J].
Carvalho, WA ;
Varaldo, PB ;
Wallau, M ;
Schuchardt, U .
ZEOLITES, 1997, 18 (5-6) :408-416
[6]   Synthesis, characterization, and catalytic properties of mesoporous tin-containing analogs of MCM-41 [J].
Chaudhari, K ;
Das, TK ;
Rajmohanan, PR ;
Lazar, K ;
Sivasanker, S ;
Chandwadkar, AJ .
JOURNAL OF CATALYSIS, 1999, 183 (02) :281-291
[7]   STUDIES ON MESOPOROUS MATERIALS .2. SYNTHESIS MECHANISM OF MCM-41 [J].
CHEN, CY ;
BURKETT, SL ;
LI, HX ;
DAVIS, ME .
MICROPOROUS MATERIALS, 1993, 2 (01) :27-34
[8]   Hydrothermal transformation and characterization of porous silica templated by surfactants [J].
Chen, XY ;
Huang, LM ;
Li, QZ .
JOURNAL OF PHYSICAL CHEMISTRY B, 1997, 101 (42) :8460-8467
[9]   From microporous to mesoporous molecular sieve materials and their use in catalysis [J].
Corma, A .
CHEMICAL REVIEWS, 1997, 97 (06) :2373-2419
[10]   SYNTHESIS OF GLASSES BY HOT-PRESSING OF GELS [J].
DECOTTIGNIES, M ;
PHALIPPOU, J ;
ZARZYCKI, J .
JOURNAL OF MATERIALS SCIENCE, 1978, 13 (12) :2605-2618