期刊
JOURNAL OF MOLECULAR CATALYSIS A-CHEMICAL
卷 297, 期 2, 页码 110-117出版社
ELSEVIER SCIENCE BV
DOI: 10.1016/j.molcata.2008.09.012
关键词
Mesoporous materials; EXAFS; Molybdenum; Oxidation; Heterogeneous catalysis
资金
- FCT
- POCI
- OE
- FEDER [POCI/QUI/56109/2004]
- The CCLRC Daresbury Laboratory Synchrotron Radiation Source (SRS) [47105]
- Fundação para a Ciência e a Tecnologia [POCI/QUI/56109/2004] Funding Source: FCT
A mesoporous silica-supported molybdenum oxide catalyst with a loading of 0.17 Mo/nm(2) was prepared by liquid phase deposition of MoO2Cl2(dMf)(2) (1) onto MCM-41 (dmf = dimethylformamide). Powder X-ray diffraction and N-2 adsorption studies of Mo-MCM-41 indicate that the texture properties of the support were preserved during the grafting experiment. On the basis of evidence from FTIR spectroscopy, C-13 and Si-29 MAS NMR, and Mo K-edge EXAFS, the Mo atoms in this catalyst are mainly present as isolated {MoO2[(-O)(3)SiO](2)(dmf)(2)} species, with a small contribution from oxo-bridged dimers. Catalysis tests show that complex 1 and Mo-MCM-41 are highly active oxidation catalysts for liquid-phase epoxidation of unfunctionalised olefins using tert-butylhydroperoxide as oxidant, from ambient to 55 degrees C. The high stability and recyclability of the heterogeneous Mo-MCM-41 catalyst is attributed to the strong metal oxide-support interaction. With cyclooctene, 1-octene, trans-2-octene and norbornene substrates, the corresponding epoxides were the only observed reaction products. The reactions of the other substrates gave by-products such as 8,9-p-menthen-1,2-diol from (R)-(+)-limonene, campholenic aldehyde from alpha-pinene, and benzaldehyde from styrene. The addition of dichloromethane as a co-solvent had a beneficial effect on catalytic performance, and in the case of (R)-(+)-limonene allowed the epoxide to be formed as the only reaction product. (C) 2008 Elsevier B.V. All rights reserved.
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