A review of the various means of catalyst immobilisation available to chemists is presented with particular emphasis on the areas of supported- and fluorous biphase-catalysis. Chapters 2 and 3 describe the design, development and realisation of a novel method of catalyst immobilisation, supported fluorous phase catalysis (SFPC). The efficacy of this approach is demonstrated via a series of rhodium-catalysed hydrogenation reactions using a perfluoroalkylated catalyst immobilised in a perfluorocarbon solvent physisorbed onto a variety of fluorine-containing support materials. The solid supports have been investigated by scanning electron microscopy, DRIFTS IR spectroscopy, CP MAS NMR spectroscopy and simultaneous thermal analysis (STA), whilst the catalyst activities and leaching levels have been determined by gas chromatography and AA/ICP spectroscopy. In Chapters 4 and 5 the synthesis of a number of novel perfluoroalkylated phosphorus(III) compounds, formulated for use in the SFPC system, is described. The compounds have been fully analysed by multinuclear NMR spectroscopy, mass spectroscopy and elemental analysis. The co-ordination chemistry of these ligands has been investigated using a range of late transition metals in order to evaluate the electronic properties of the various phosphorus centres. These novel co-ordination complexes have also been analysed by multinuclear NMR spectroscopy, mass spectroscopy, and elemental analysis. The solubilities of the various compounds in perfluorocarbon solvents have been determined in order to assess their suitability for use in perfluorocarbon-based catalytic technologies. Preliminary work is also described on the development of a novel range of perfluoroalkylated palladium complexes for use in carbon-carbon bond formation reactions. Chapter 6 describes the synthesis of two diphosphine compounds and a series of novel co-ordination complexes based on these ligands.
Identifer | oai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:432924 |
Date | January 2003 |
Creators | Sherringham, James |
Publisher | University of Leicester |
Source Sets | Ethos UK |
Detected Language | English |
Type | Electronic Thesis or Dissertation |
Source | http://hdl.handle.net/2381/30083 |
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