Synthesis, characterization and reactivity of transition metal containing zeolites

dc.contributor.authorRossin, Joseph A.en
dc.contributor.committeechairDavis, M.E.en
dc.contributor.committeememberGibbs, Gerald V.en
dc.contributor.committeememberHanson, Brian E.en
dc.contributor.committeememberSquires, A.en
dc.contributor.committeememberWills, George B.en
dc.contributor.departmentChemical Engineeringen
dc.date.accessioned2017-03-10T20:22:14Zen
dc.date.available2017-03-10T20:22:14Zen
dc.date.issued1986en
dc.description.abstractTransition metal containing zeolites (zeolite A and ZSM-5) were prepared by addition of various transition metal containing substrates to zeolite synthesis gels. Crystal growth data were recorded in order to determine the influence of the transition metal species on the rate of crystal growth. X-ray diffraction, oxygen adsorption, FTIR and SEM were utilized to evaluate crystal purity. X-ray photoelectron spectroscopy (XPS), chemical analysis and electron microprobe analysis were performed in order to ascertain the position (intrazeolitic versus surface) and homogeneity of the transition metal. It was concluded that intrazeolitic transition metals were produced by the novel procedure presented in this work. 1-Hexene hydroformylation by rhodium zeolite A showed intrazeolitic rhodium to migrate to the external surface of the zeolite. However, in the presence of a solution and surface rhodium poison, intrazeolitic rhodium was found to hydroformylate 1-hexene exclusively to heptanal. Ruthenium containing zeolite A was evaluated under CO-hydrogenation conditions. No migration of intrazeolitic ruthenium to the external surface of the zeolite was observed over the course of the reaction. The product distribution obtained for this catalyst did not follow a log normal behavior. Also, loss of zeolite crystallinity was observed following the reaction. Cobalt ZSM-5 was evaluated under CO-hydrogenation conditions. No migration of cobalt to the external surface of the zeolite occurred. XPS analysis of the catalyst following various stages of the reaction indicated that intrazeolitic cobalt was not reduced to the zero valent state. Consequently, the non-zero valent cobalt was not capable of hydrogenating carbon monoxide.en
dc.description.degreePh. D.en
dc.format.extentxviii, 398 leavesen
dc.format.mimetypeapplication/pdfen
dc.identifier.urihttp://hdl.handle.net/10919/76271en
dc.language.isoen_USen
dc.publisherVirginia Polytechnic Institute and State Universityen
dc.relation.isformatofOCLC# 14642402en
dc.rightsIn Copyrighten
dc.rights.urihttp://rightsstatements.org/vocab/InC/1.0/en
dc.subject.lccLD5655.V856 1986.R677en
dc.subject.lcshTransition metals -- Analysisen
dc.subject.lcshZeolitesen
dc.subject.lcshTransition metals -- Reactivityen
dc.titleSynthesis, characterization and reactivity of transition metal containing zeolitesen
dc.typeDissertationen
dc.type.dcmitypeTexten
thesis.degree.disciplineChemical Engineeringen
thesis.degree.grantorVirginia Polytechnic Institute and State Universityen
thesis.degree.leveldoctoralen
thesis.degree.namePh. D.en
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