The performance of Ti-MCM-41 in aqueous media and after mechanical treatment studied by in situ XANES, UV/Vis and test reactions

被引:47
作者
Hagen, A
Schueler, K
Roessner, F
机构
[1] Tech Univ Denmark, Interdisciplinary Res Ctr Catalysis, DK-2800 Lyngby, Denmark
[2] Carl von Ossietzky Univ Oldenburg, Dept Chem, D-26111 Oldenburg, Germany
关键词
Ti-MCM-41; XANES; oxidation; water; mechanical stability;
D O I
10.1016/S1387-1811(01)00465-6
中图分类号
O69 [应用化学];
学科分类号
081704 ;
摘要
The influence of water on the epoxidation of cyclohexene with H2O2 and tert-butyl hydroperoxide (tbhp) on Ti-MCM-41 molecular sieves prepared by post-synthetic modification of the support with titanium alkoxides was investigated. The catalytic performance depends on the hydrophilicity/hydrophobicity of the MCM-41 surface, but also on the interactions between titanium centers and oxidants. Using XANES, a higher coordination number and an irreversible transformation of isolated into oxide-like titanium species was observed when the reaction was performed with H2O2 compared to tbhp. The mechanical treatment of Ti-MCM-41 in a ball mill or press did not influence the local environment around the titanium centers, whereas the MCM-41 structure was damaged causing a decrease of the conversion of cyclohexene. (C) 2002 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:23 / 33
页数:11
相关论文
共 31 条
  • [1] Organically modified titanium-rich Ti-MCM-41, efficient catalysts for epoxidation reactions
    Bhaumik, A
    Tatsumi, T
    [J]. JOURNAL OF CATALYSIS, 2000, 189 (01) : 31 - 39
  • [2] X-RAY-ABSORPTION NEAR-EDGE STRUCTURE OF 3D TRANSITION-ELEMENTS IN TETRAHEDRAL COORDINATION - THE EFFECT OF BOND-LENGTH VARIATION
    BIANCONI, A
    FRITSCH, E
    CALAS, G
    PETIAU, J
    [J]. PHYSICAL REVIEW B, 1985, 32 (06): : 4292 - 4295
  • [3] SYNTHESIS, CHARACTERIZATION, AND CATALYTIC ACTIVITY OF TI-MCM-41 STRUCTURES
    BLASCO, T
    CORMA, A
    NAVARRO, MT
    PARIENTE, JP
    [J]. JOURNAL OF CATALYSIS, 1995, 156 (01) : 65 - 74
  • [4] Monoglyceride synthesis by heterogeneous catalysis using MCM-41 type silicas functionalized with amino groups
    Cauvel, A
    Renard, G
    Brunel, D
    [J]. JOURNAL OF ORGANIC CHEMISTRY, 1997, 62 (03) : 749 - 751
  • [5] Optimal parameters for the synthesis of the mesoporous molecular sieve [Si]-MCM-41
    Cheng, CF
    Park, DH
    Klinowski, J
    [J]. JOURNAL OF THE CHEMICAL SOCIETY-FARADAY TRANSACTIONS, 1997, 93 (01): : 193 - 197
  • [6] Ordered mesoporous materials
    Ciesla, U
    Schüth, F
    [J]. MICROPOROUS AND MESOPOROUS MATERIALS, 1999, 27 (2-3) : 131 - 149
  • [7] CORMA A, 1994, STUD SURF SCI CATAL, V84, P69
  • [8] SYNTHESIS OF AN ULTRALARGE PORE TITANIUM SILICATE ISOMORPHOUS TO MCM-41 AND ITS APPLICATION AS A CATALYST FOR SELECTIVE OXIDATION OF HYDROCARBONS
    CORMA, A
    NAVARRO, MT
    PARIENTE, JP
    [J]. JOURNAL OF THE CHEMICAL SOCIETY-CHEMICAL COMMUNICATIONS, 1994, (02) : 147 - 148
  • [9] Solvent effects during the oxidation of olefins and alcohols with hydrogen peroxide on Ti-beta catalyst: The influence of the hydrophilicity-hydrophobicity of the zeolite
    Corma, A
    Esteve, P
    Martinez, A
    [J]. JOURNAL OF CATALYSIS, 1996, 161 (01) : 11 - 19
  • [10] Oxidation of crotyl alcohol using Ti-β and Ti-MCM-41 catalysts
    Davies, LJ
    McMorn, P
    Bethell, D
    Page, PCB
    King, F
    Hancock, FE
    Hutchings, GJ
    [J]. JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL, 2001, 165 (1-2) : 243 - 247