An investigation of active and selective oxygen in vanadium phosphorus oxide catalysts for n-butane conversion to maleic anhydride
dc.contributor.advisor | Glenn L. Schrader | |
dc.contributor.author | Lashier, Mark | |
dc.contributor.department | Chemical and Biological Engineering | |
dc.date | 2018-08-17T01:39:26.000 | |
dc.date.accessioned | 2020-07-02T06:11:34Z | |
dc.date.available | 2020-07-02T06:11:34Z | |
dc.date.copyright | Sun Jan 01 00:00:00 UTC 1989 | |
dc.date.issued | 1989 | |
dc.description.abstract | <p>The role of lattice oxygens in two model catalysts, [beta]-VOPO[subscript]4 and (VO)[subscript]2P[subscript]2O[subscript]7, was investigated for the selective and nonselective oxidation of C[subscript]4 hydrocarbons to maleic anhydride and combustion products. Specific catalytic oxygen sites in each model catalyst were labeled with specific amounts of [superscript]18O. Labeled sites were identified by laser Raman spectroscopy and Fourier transform infrared spectroscopy. The level of [superscript]18O enrichment in each site was estimated from the laser Raman spectra and the stoichiometry of reactions involved in the synthesis of the labeled catalysts. Products of the anaerobic C[subscript]4 hydrocarbon oxidation and, in the case of (VO)[subscript]2P[subscript]2O[subscript]7, alternating pulses of oxygen with pulses of hydrocarbon, over labeled catalysts were monitored by quadrupole mass spectrometry. These studies reveal that, on both catalysts, more than one path to CO[subscript]2 exists involving lattice oxygens. The consecutive combustion of maleic anhydride involves mainly V=O oxygen, while all other oxygen sites are utilized to form small amounts of CO[subscript]2. In both catalyst systems, P-O-V sites are the source for selective oxygens. Additionally, specific selective oxygen sites could be related to mechanistic steps in the conversion of n-butane to maleic anhydride for both model catalysts. The results of this work indicate that the initial selective interaction of n-butane with the surface of the catalyst results in an intermediate which is very different than that of the other C[subscript]4's studied, and that this strongly adsorbed intermediate is constrained to react with specific P-O sites. Additional evidence suggests that [beta]-VOPO[subscript]4 is not the V(V) species formed in the oxidation-reduction couple on the surface of (VO)[subscript]2P[subscript]2O[subscript]7.</p> | |
dc.format.mimetype | application/pdf | |
dc.identifier | archive/lib.dr.iastate.edu/rtd/9145/ | |
dc.identifier.articleid | 10144 | |
dc.identifier.contextkey | 6348277 | |
dc.identifier.doi | https://doi.org/10.31274/rtd-180813-11846 | |
dc.identifier.s3bucket | isulib-bepress-aws-west | |
dc.identifier.submissionpath | rtd/9145 | |
dc.identifier.uri | https://dr.lib.iastate.edu/handle/20.500.12876/82212 | |
dc.language.iso | en | |
dc.source.bitstream | archive/lib.dr.iastate.edu/rtd/9145/r_9014920.pdf|||Sat Jan 15 02:29:01 UTC 2022 | |
dc.subject.disciplines | Chemical Engineering | |
dc.subject.keywords | Chemical engineering | |
dc.title | An investigation of active and selective oxygen in vanadium phosphorus oxide catalysts for n-butane conversion to maleic anhydride | |
dc.type | article | |
dc.type.genre | dissertation | |
dspace.entity.type | Publication | |
relation.isOrgUnitOfPublication | 86545861-382c-4c15-8c52-eb8e9afe6b75 | |
thesis.degree.level | dissertation | |
thesis.degree.name | Doctor of Philosophy |
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