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dc.contributor.advisorShafer, Jenifer C.
dc.contributor.advisorWu, David T.
dc.contributor.authorServis, Michael J.
dc.date.accessioned2017-10-10T17:01:29Z
dc.date.accessioned2022-02-03T13:01:07Z
dc.date.available2018-10-09T17:01:29Z
dc.date.available2022-02-03T13:01:07Z
dc.date.issued2017
dc.identifierServis_mines_0052E_11352.pdf
dc.identifierT 8361
dc.identifier.urihttps://hdl.handle.net/11124/171783
dc.descriptionIncludes bibliographical references.
dc.description2017 Fall.
dc.description.abstractSolvent extraction is implemented in the nuclear fuel cycle to reprocess used nuclear fuel. One processing challenge in solvent extraction is avoiding third phase formation, which limits metal loading into the organic phase and therefore extraction efficiency. Third phase formation is known to depend strongly on extractant and solvent molecular structure for solvating organophosphorus extractants. Molecular dynamics simulations were employed to study the organic phase association of extractant molecules. Force field optimization and validation were conducted for the extractant molecules for properties relevant to organic phase association, including average molecular dipole, dimerization constant and mixing enthalpy with aliphatic solvents. Network analysis was used to quantify speciation of hydrogen bonded clusters of water and nitric acid extracted by tributyl phosphate into n-dodecane. Large cluster formation under high extracted nitric acid and water concentrations near the third phase formation phase boundary was found to be consistent with percolation theory. Simulations with uranyl nitrate/extractant clusters showed orientational dependence on the inter-cluster interactions. Structural differences between extractants resulted in changes to the uranyl-centered cluster interaction energetics. Future research may link these differences in metal-centered cluster interactions to organic phase solubility and third phase formation under high metal loading.
dc.format.mediumborn digital
dc.format.mediumdoctoral dissertations
dc.languageEnglish
dc.language.isoeng
dc.publisherColorado School of Mines. Arthur Lakes Library
dc.relation.ispartof2017 - Mines Theses & Dissertations
dc.rightsCopyright of the original work is retained by the author.
dc.titleUnderstanding extractant aggregation through molecular simulation
dc.typeText
dc.contributor.committeememberKing, Jeffrey C.
dc.contributor.committeememberSum, Amadeu K.
dc.contributor.committeememberJensen, Mark
dc.contributor.committeememberVyas, Shubham
dcterms.embargo.terms2018-10-09
dcterms.embargo.expires2018-10-09
thesis.degree.nameDoctor of Philosophy (Ph.D.)
thesis.degree.levelDoctoral
thesis.degree.disciplineChemistry
thesis.degree.grantorColorado School of Mines
dc.rights.accessEmbargo Expires: 10/09/2018


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