Direct synthesis gas conversion to alcohols and hydrocarbons using a catalytic membrane reactor.

In this work, inorganic membranes with highly dispersed metallic catalysts on macroporous titania-washcoated alumina supports were produced, characterized and tested in a catalytic membrane reactor. The reactor, operated as a contactor in the forced pore-flow-through mode, was used for the conversion of synthesis gas (H2 + CO) into mixed alcohols and hydrocarbons via the Fischer-Tropsch synthesis. Carbon monoxide conversions of 78% and 90% at near atmospheric pressure (300kPa) and 493K were recorded over cobalt and bimetallic Co-Mn membranes respectively. The membranes also allowed for the conversion of carbon dioxide, thus eliminating the need for a CO2 separation interphase between synthesis gas production and Fischer-Tropsch synthesis. Catalytic tests conducted with the membrane reactor with different operating conditions (of temperature, pressure and feed flow rate) on cobalt-based membranes gave very high selectivity to specific products, mostly higher alcohols (C2 “ C8) and paraffins within the gasoline range, thereby making superfluous any further upgrading of products to fuel grade other than simple dehydration. Manganese-promoted cobalt membranes were found not only to give better Fischer-Tropsch activity, but also to promote isomerization of paraffins, which is good for boosting the octane number of the products, with the presence of higher alcohols improving the energy density. The membrane reactor concept also enhanced the ability of cobalt to catalyze synthesis gas conversions, giving an activation energy Ea of 59.5 kJ/mol.K compared with 86.9 “ 170 kJ/mol.K recorded in other reactors. Efficient heat transfer was observed because of the open channel morphology of the porous membranes. A simplified mechanism for both alcohol and hydrocarbon production based on hydroxycarbene formation was proposed to explain both the stoichiometric reactions formulated and the observed product distribution pattern.

Name dc:type.qualificationname

PhD

Level dc:type.qualificationlevel

Doctoral

Grantor dc:publisher.institution

Robert Gordon University

Year dc:date.issued

2009

Author dc:creator

• Umoh, Reuben Mfon

Advisor dc:contributor.advisor

• Edward Gobina

• Inorganic membranes
• Hydrocarbons
• Fischer Tropsch synthesis
• Catalytic membrane reactor

Language dc:language

en

Identifier

oai:rgu-repository.worktribe.com:248867

OAI identifier oai:identifier

oai:rgu-repository.worktribe.com:248867