Synthesis, characterization and selective oxidation properties of Ti-containing mesoporous catalysts

被引:117
作者
Eimer, GA [1 ]
Casuscelli, SG [1 ]
Ghione, GE [1 ]
Crivello, ME [1 ]
Herrero, ER [1 ]
机构
[1] Univ Tecnol Nacl, Fac Reg Cordoba, CITeQ, RA-5016 Cordoba, Argentina
关键词
Ti-MCM-41; mesoporous materials; M41S; titanium; epoxidation; cyclohexene;
D O I
10.1016/j.apcata.2005.10.006
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-containing mesoporous catalysts with MCM-41 structure have been successfully prepared by direct hydrothermal synthesis. These mesoporous materials were compared with pure siliceous MCM-41 synthesized at the same conditions. An extended and detailed study, which includes the effects of several factors such as the state and content of Ti, surfactant/Si ratio and template removal technique on the physicochemical properties and catalytic activity of Ti-MCM-41, is presented in this contribution. Various techniques including XRD, FT-IR, DRUV-vis, ICP and N-2 adsorption were employed for the materials characterization. An optimum surfactant/Si molar ratio in the synthesis gel for the highest regularity of the formed mesostructure was found. Both the structure stability and the local environment of Ti sites in mesostructures with different degrees of Ti loading (0.10-3.22 wt.%) have been carefully investigated. Based on a combined FT-IR and DRUV-vis study and ICP analysis, it was possible to conclude that Infrared spectroscopy can result a powerful tool to verify the Ti(IV) incorporation into the framework of MCM-41. Therefore, a simple and novel method for estimation of framework Ti content could be developed. Also, these materials were catalytically tested in the oxidation of cyclohexene with aqueous hydrogen peroxide. Finally, the catalysts could be regenerated without any loss in activity/selectivity. (c) 2005 Elsevier B.V. All rights reserved.
引用
收藏
页码:232 / 242
页数:11
相关论文
共 81 条
[51]   Ordered mesoporous titanosilicates with better catalytically active titanium sites assembled from preformed titanosilicate precursors with zeolite building units in alkaline media [J].
Lin, KF ;
Sun, ZH ;
Sen, L ;
Jiang, DZ ;
Xiao, FS .
MICROPOROUS AND MESOPOROUS MATERIALS, 2004, 72 (1-3) :193-201
[52]   Structure-functionality relationships of grafted Ti-MCM41 silicas. Spectroscopic and catalytic studies [J].
Marchese, L ;
Gianotti, E ;
Dellarocca, V ;
Maschmeyer, T ;
Rey, F ;
Coluccia, S ;
Thomas, JM .
PHYSICAL CHEMISTRY CHEMICAL PHYSICS, 1999, 1 (04) :585-592
[53]   Selective oxidation of propylene to propylene oxide over Ti-MCM-41 supporting metal nitrate [J].
Miyaji, T ;
Wu, P ;
Tatsumi, T .
CATALYSIS TODAY, 2001, 71 (1-2) :169-176
[54]   Hydrothermally stable restructured mesoporous silica [J].
Mokaya, R .
CHEMICAL COMMUNICATIONS, 2001, (10) :933-934
[55]   Effect of Ti-modified mesoporous materials on the direct epoxidation of propylene by molecular oxygen [J].
Murata, K ;
Liu, YY ;
Inaba, M ;
Mimura, N .
CATALYSIS TODAY, 2004, 91-2 :39-42
[56]  
Notari B, 1996, ADV CATAL, V41, P253, DOI 10.1016/S0360-0564(08)60042-5
[57]  
Notari B., 1988, STUD SURF SCI CATAL, V37, P413, DOI DOI 10.1016/S0167-2991(09)60618-2
[58]  
On DT, 2003, MICROPOR MESOPOR MAT, V57, P169
[59]   A multivariate analysis of the synthesis conditions of mesoporous materials [J].
Oye, G ;
Sjöblom, J ;
Stöcker, M .
MICROPOROUS AND MESOPOROUS MATERIALS, 2000, 34 (03) :291-299
[60]   Mono (V, Nb) or bimetallic (V-Ti, Nb-Ti) ions modified MCM-41 catalysts: synthesis, characterization and catalysis in oxidation of hydrocarbons (aromatics and alcohols) [J].
Parvulescu, V ;
Anastasescu, C ;
Constantin, C ;
Su, BL .
CATALYSIS TODAY, 2003, 78 (1-4) :477-485