Title:
Silica supported palladium nanoparticles for the decarboxylation of high-acid feedstocks: design, deactivation and regeneration

dc.contributor.advisor Jones, Christopher W.
dc.contributor.advisor Fuller, Thomas F.
dc.contributor.author Ping, Eric Wayne en_US
dc.contributor.committeeMember Agrawal, Pradeep K.
dc.contributor.committeeMember Fedorov, Anei
dc.contributor.committeeMember Pierson, John
dc.contributor.committeeMember Wallace, Robert
dc.contributor.department Chemical and Biomolecular Engineering en_US
dc.date.accessioned 2011-07-06T16:46:37Z
dc.date.available 2011-07-06T16:46:37Z
dc.date.issued 2011-03-29 en_US
dc.description.abstract The major goals of this thesis were to (1) design and synthesize a supported catalyst with well-defined monodisperse palladium nanoparticles evenly distributed throughout an inorganic oxide substrate with tunable porosity characteristics, (2) demonstrate the catalytic activity of this material in the decarboxylation of long chain fatty acids and their derivatives to make diesel-length hydrocarbons, (3) elucidate the deactivation mechanism of supported palladium catalysts under decarboxylation conditions via post mortem catalyst characterization and develop a regeneration methodology thereupon, and (4) apply this catalytic system to a real low-value biofeedstock. In an effort to maximize loading and minimize mass transfer limitations, mesoporous silica MCF was synthesized as catalyst support. Functionalization with various silane ligands facilitated even distribution of palladium precursor salts throughout the catalyst particle, and, after reduction, monodisperse palladium nanoparticles approximately 2 nm in diameter. The Pd-MCF catalyst showed high one-time activity in the decarboxylation of fatty acids to hydrocarbons in dodecane at 300 °C. Subsequent reactions were performed on acid derivatives to elucidate a decarboxylation reaction pathway. The catalyst experienced severe deactivation after only one use and substantial effort was put into elucidating the nature of this deactivation via post mortem catalyst characterization. The deactivation was found not to be caused by nanoparticle sintering, agglomeration or ripening, but instead by organic deposition, mainly of reactant acid. A regeneration methodology was developed and subsequent catalyst reuse exhibited high activity. Finally, the Pd-MCF catalyst was applied to a wastewater-derived brown grease from a poultry rendering facility, in an unpolished and polished form. The latter was successfully decarboxylated to diesel-length hydrocarbons with high conversion and selectivity. en_US
dc.description.degree Ph.D. en_US
dc.identifier.uri http://hdl.handle.net/1853/39537
dc.publisher Georgia Institute of Technology en_US
dc.subject Decarboxylation en_US
dc.subject Mesoporous silica en_US
dc.subject Palladium en_US
dc.subject Biofuel en_US
dc.subject Catalyst en_US
dc.subject Nanoparticle en_US
dc.subject.lcsh Decarboxylation
dc.subject.lcsh Feedstock
dc.subject.lcsh Nanoparticles
dc.subject.lcsh Palladium catalysts
dc.title Silica supported palladium nanoparticles for the decarboxylation of high-acid feedstocks: design, deactivation and regeneration en_US
dc.type Text
dc.type.genre Dissertation
dspace.entity.type Publication
local.contributor.advisor Fuller, Thomas F.
local.contributor.advisor Jones, Christopher W.
local.contributor.corporatename School of Chemical and Biomolecular Engineering
local.contributor.corporatename College of Engineering
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