Design and characterization of zeolite supported cobalt carbonyl catalysts

Transition 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)_4^-. Disproportionation may be induced thus forming Co(CO)_4^- 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.

Name thesis:degree_name

Ph. D.

Level thesis:degree_level

doctoral

Discipline thesis:degree_discipline

Chemistry

Department dc:contributor.department

Chemistry

Grantor dc:publisher

Virginia Polytechnic Institute and State University

Year dc:date.issued

1987

Author dc:creator

• Connaway, Melissa Clare

Chair dc:contributor.committeechair

• Hanson, Brian E.

Committee members dc:contributor.committeemember

• Dillard, John G.
• Wightman, James P.
• Tanko, James M.
• Davis, Mark E.

Statement dc:rights

• In Copyright

Licence dc:rights.uri

• http://rightsstatements.org/vocab/InC/1.0/

Language dc:language.iso

en_US

Handle dc:identifier.uri

http://hdl.handle.net/10919/82894

OAI identifier oai:identifier

oai:vtechworks.lib.vt.edu:10919/82894