Reactions of Unsaturated Hydrocarbons Over Supported Metal Carbonyl Catalysts

Morgan, Geoffrey E (1977) Reactions of Unsaturated Hydrocarbons Over Supported Metal Carbonyl Catalysts. PhD thesis, University of Glasgow.

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An investigation has been carried out on the effect of supporting metal carbonyl complexes in a highly dispersed state on an "inert" carrier. A study of the catalytic activity of these complexes in the heterogeneous phase has also been carried out. The metal carbonyls which have been examined are Os3(CO)12 and Re2(CO)10, both of which retain their molecular structure when supported on silica, and the tetranuclear mixed-metal carbonyl Rh2Co2(CO)12 which has been found to be less stable when supported, undergoing the loss of bridging carbonyl groups. Whereas the former carbonyls are very stable on exposure to air, the latter complex shows a tendency to decompose to the metals after only a short time. By the use of various techniques including T. V. A. , T. G. A. , infrared analysis and electron microscopy it has been found possible to monitor the change in structure and loss of carbon monoxide which occurs when the supported complex is thermally activated in vacuo. Hence the supported complex may be characterised at various stages in the activation process. From the studies which have been carried out using the three supported complexes it has been found that a prerequisite for catalytic activity as measured by the hydrogenation and isomerisation of the n-butenes, is the loss of at least some of the carbonyl ligands on the complex. In the case of Os3(CO)12 supported on silica, the active forms of the catalyst examined are (a) Os3(CO)g and (b) a very high . dispersion of osmium atoms, obtained after the loss of all carbonyls from the complex, in which there may or may not be cluster retention. Comparisons between this latter catalyst and a more conventional supported osmium catalyst prepared by impregnation of osmium chloride followed by reduction at 320

Item Type: Thesis (PhD)
Qualification Level: Doctoral
Keywords: Organic chemistry
Date of Award: 1977
Depositing User: Enlighten Team
Unique ID: glathesis:1977-78763
Copyright: Copyright of this thesis is held by the author.
Date Deposited: 30 Jan 2020 14:56
Last Modified: 30 Jan 2020 14:56

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