期刊
JOURNAL OF ORGANOMETALLIC CHEMISTRY
卷 696, 期 22, 页码 3543-3550出版社
ELSEVIER SCIENCE SA
DOI: 10.1016/j.jorganchem.2011.07.040
关键词
Molybdenum; Schiff base ligands; Carbonyl ligands; Supported catalysts; Oxidative decarbonylation; Olefin epoxidation
资金
- Fundacao para a Ciencia e a Tecnologia (FCT)
- Programa Operacional Ciencia e Inovacao (POCI)
- Orcamento do Estado (OE)
- Fundo Europeu de Desenvolvimento Regional (FEDER) [PTDC/QUI/71198/2006]
- European Social Fund
- CICECO
- [SFRH/BPD/25269/2005]
- [SFRH/BPD/46473/2008]
- Fundação para a Ciência e a Tecnologia [PTDC/QUI/71198/2006, SFRH/BPD/46473/2008] Funding Source: FCT
The ligand N-(n-propyl)-2-pyridylmethanimine (pyim) and an immobilised analogue of this ligand (MCM-41-pyim) were prepared by the condensation reaction of 2-pyridinecarboxaldehyde with either propylamine or aminopropyl groups covalently attached to the ordered mesoporous silica MCM-41. Free and immobilised tetracarbonyl complexes of the type cis-[Mo(CO)(4)(L)] (L = pyim (1), MCM-41-pyim) were then prepared by microwave-assisted heating of a mixture of Mo(CO)(6) and the organic ligand or ligand-silica in toluene at 110 degrees C for 30-45 min. The products were characterised by NMR spectroscopy ((1)H, (13)C and (29)Si, in solution and in the solid state), elemental analysis, N(2) adsorption, and FT-IR spectroscopy. When used as catalyst precursors for the epoxidation of cis-cyclooctene by tert-butylhydroperoxide at 55 degrees C (1 mol% catalyst (Mo), no additional co-solvent), 1,2-epoxy-cyclooctane was obtained as the only reaction product in quantitative yield after 5 h for 1 and 36% yield after 24 h for the supported complex. The use of the ionic liquid (IL) 1-butyl-3-methylimidazolium tetrafluoroborate as co-solvent led to lower catalytic activities (epoxide selectivity was always 100%) but allowed the catalyst/IL mixtures (homogeneous mixture for IL+1 and a biphasic solid + IL system for IL+MCM-41-pyim/Mo) to be easily recovered and reused in subsequent runs without loss of catalytic performance. (C) 2011 Elsevier B. V. All rights reserved.
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