Direct synthesis and characterization of titanium-substituted mesoporous molecular sieve SBA-15

被引:299
作者
Zhang, WH
Lu, JQ
Han, B
Li, MJ
Xiu, JH
Ying, PL
Li, C
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian 116023, Peoples R China
[2] Dalian Univ Technol, State Key Lab Fine Chem Engn, Dalian 116012, Peoples R China
关键词
D O I
10.1021/cm011686c
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
Ti-substituted mesoporous SBA-15 (Ti-SBA-15) materials have been synthesized by using a new approach in which the hydrolysis of the silicon precursor (tetramethoxysilane, TMOS) is accelerated by fluoride. These materials were characterized by powder X-ray diffraction patterns (XRD), X-ray fluorescence spectroscopy (Y-RF), N-2 sorption isotherms, diffuse-reflectance UV-visible (UV-vis) and UV-Raman spectroscopy, Si-29 MAS NMR, and the catalytic epoxidation reaction of styrene. Experiments show that Ti-SBA-15 samples of high quality can be obtained under the following conditions: F/Si greater than or equal to 0.03 (molar ratio), pH less than or equal to 1.0, aging temperature less than or equal to 80 degreesC, and Ti/Si less than or equal to 0.01. It was found that the hydrolysis rate of TMOS was remarkably accelerated by fluoride, which was suggested to play the main role in the formation of Ti-SBA-15 materials of high quality. There is no stoichiometric incorporation of Ti, and the Ti contents that are obtained are quite low in the case of the approach that is proposed. The calcined Ti-SBA-15 materials show highly catalytic activity in the epoxidation of styrene.
引用
收藏
页码:3413 / 3421
页数:9
相关论文
共 93 条
[1]   Kinetics of cosurfactant-surfactant-silicate phase behavior.: 1.: Short-chain alcohols [J].
Ågren, P ;
Lindén, M ;
Rosenholm, JB ;
Schwarzenbacher, R ;
Kriechbaum, M ;
Amenitsch, H ;
Laggner, P ;
Blanchard, J ;
Schüth, F .
JOURNAL OF PHYSICAL CHEMISTRY B, 1999, 103 (29) :5943-5948
[2]   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
[3]   Oxidative transformations of organic compounds mediated by redox molecular sieves [J].
Arends, IWCE ;
Sheldon, RA ;
Wallau, M ;
Schuchardt, U .
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION, 1997, 36 (11) :1144-1163
[4]  
Bae SJ, 2000, CHEM COMMUN, P31
[5]   Mesoporous [M]-MSU-x metallo-silicate catalysts by non-ionic polyethylene oxide surfactant templating acid [N0(N+)X-I+] and base (N0M+I-) catalysed pathways [J].
Bagshaw, SA ;
Kemmitt, T ;
Milestone, NB .
MICROPOROUS AND MESOPOROUS MATERIALS, 1998, 22 (1-3) :419-433
[6]   TEMPLATING OF MESOPOROUS MOLECULAR-SIEVES BY NONIONIC POLYETHYLENE OXIDE SURFACTANTS [J].
BAGSHAW, SA ;
PROUZET, E ;
PINNAVAIA, TJ .
SCIENCE, 1995, 269 (5228) :1242-1244
[7]   Preparation of metal-incorporated MSU mesoporous silica molecular sieves. Ti incorporation via a totally non-ionic route [J].
Bagshaw, SA ;
DiRenzo, F ;
Fajula, F .
CHEMICAL COMMUNICATIONS, 1996, (18) :2209-2210
[8]   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
[9]   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
[10]   A new synthesis of mesoporous MSU-X silica controlled by a two-step pathway [J].
Boissière, C ;
Larbot, A ;
van der Lee, A ;
Kooyman, PJ ;
Prouzet, E .
CHEMISTRY OF MATERIALS, 2000, 12 (10) :2902-2913