Design and characterization of zeolite supported cobalt carbonyl catalysts

dc.contributor.authorConnaway, Melissa Clareen
dc.contributor.committeechairHanson, Brian E.en
dc.contributor.committeememberDillard, John G.en
dc.contributor.committeememberWightman, James P.en
dc.contributor.committeememberTanko, James M.en
dc.contributor.committeememberDavis, Mark E.en
dc.contributor.departmentChemistryen
dc.date.accessioned2018-04-24T19:23:14Zen
dc.date.available2018-04-24T19:23:14Zen
dc.date.issued1987en
dc.description.abstractTransition metal compounds such as Co₂(CO)₈ have often been used to catalyze various organic reactions. Severe difficulties may be encountered when attempts are made to recover and separate the soluble catalysts. A heterogeneous system consisting of Co₂(CO)₈ impregnated on zeolites with faujasitic structure has been designed and investigated using a variety of techniques. In situ FTIR spectroscopy and carbon monoxide evolution were used to identify the major products generated, namely Co₄(CO)₁₂ and Co(CO)<sub>4<sup>-</sup></sub>. Disproportionation may be induced thus forming Co(CO)<sub>4<sup>-</sup></sub> and an associated cation from the supported subcarbonyls by addition of various ligands such as methanol. The location of the supported cobalt carbonyls is determined by their reactivity toward various phosphines with various kinetic diameters. The materials prepared in this manner were found to be active in catalyzing the methanol carbonylation reaction and following thermolysis were also found to be active Fischer-Tropsch catalysts. Major products observed in the carbonylation of methanol were methyl acetate and an acetaldehyde dimethyl acetal. The supported cobalt catalyst displays greater activity than Co₂(CO)₈ in solution for the carbonylation reaction when conducted under similar conditions. In the Fischer-Tropsch process, selectivity is seen for the production of linear, short-chain hydrocarbons.en
dc.description.degreePh. D.en
dc.format.extentx, 112 leavesen
dc.format.mimetypeapplication/pdfen
dc.identifier.urihttp://hdl.handle.net/10919/82894en
dc.language.isoen_USen
dc.publisherVirginia Polytechnic Institute and State Universityen
dc.relation.isformatofOCLC# 16963293en
dc.rightsIn Copyrighten
dc.rights.urihttp://rightsstatements.org/vocab/InC/1.0/en
dc.subject.lccLD5655.V856 1987.C666en
dc.subject.lcshZeolitesen
dc.subject.lcshCarbonyl compoundsen
dc.titleDesign and characterization of zeolite supported cobalt carbonyl catalystsen
dc.typeDissertationen
dc.type.dcmitypeTexten
thesis.degree.disciplineChemistryen
thesis.degree.grantorVirginia Polytechnic Institute and State Universityen
thesis.degree.leveldoctoralen
thesis.degree.namePh. D.en

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