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Enabling and understanding low-temperature kinetic pathways in solid-state metathesis reactions

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dc.contributor.authorTodd, Paul Kendrick, author
dc.contributor.authorNeilson, James, advisor
dc.contributor.authorFinke, Richard, committee member
dc.contributor.authorPrieto, Amy, committee member
dc.contributor.authorHenry, Chuck, committee member
dc.contributor.authorMa, Kaka, committee member
dc.date.accessioned2020-06-22T11:53:59Z
dc.date.available2022-06-15T11:53:59Z
dc.date.issued2020
dc.description.abstractFor the kinetic pathway to influence the outcome of a solid-state reaction, diffusion barriers must be lowered or circumvented through low-temperature chemistry. Traditional ceramic synthesis use high temperatures to overcome diffusion, yet they result in the thermodynamically stable product. If the desired product lies higher in energy, they are unattainable at such temperatures. Extrinsic parameters, like pressure, can be used to change the stability of products (kinetic trapping), yet require extreme conditions. Another strategy involves kinetically controlling the energy barriers of the reaction to select for a given product. Here, we use solid-state metathesis reactions to understand and control kinetic pathways in the formation of complex oxides and binary metal sulfides. Through simple changes to precursor composition, three unique polymorphs of yttrium manganese oxide are synthesized, two of which are metastable phases. Using in situ diagnostics, the reaction pathways are characterized to identity intermediates and the temperature regimes at which they react. Using this information we identify why different polymorphs form using different precursors. Additionally, small functional organosilicon molecules are shown to catalyze the formation of iron(II) sulfide using metathesis reactions. Here we show that the Si-O functional group stabilizes intermediate species along the pathway to avoid forming more stable intermediates. The result is higher yields of FeS2 at lower temperatures and times. The included chapters will hopefully better inform future solid-state chemists when exploring new composition spaces and reaction pathways.
dc.format.mediumborn digital
dc.format.mediumdoctoral dissertations
dc.identifierTodd_colostate_0053A_16042.pdf
dc.identifier.urihttps://hdl.handle.net/10217/208592
dc.languageEnglish
dc.language.isoeng
dc.publisherColorado State University. Libraries
dc.relation.ispartof2020-
dc.rightsCopyright and other restrictions may apply. User is responsible for compliance with all applicable laws. For information about copyright law, please see https://libguides.colostate.edu/copyright.
dc.subjectkinetics
dc.subjectoxides
dc.subjectsulfides
dc.subjectmetathesis
dc.subjectdiffraction
dc.subjectsolid-state
dc.titleEnabling and understanding low-temperature kinetic pathways in solid-state metathesis reactions
dc.typeText
dcterms.embargo.expires2022-06-15
dcterms.embargo.terms2022-06-15
dcterms.rights.dplaThis Item is protected by copyright and/or related rights (https://rightsstatements.org/vocab/InC/1.0/). You are free to use this Item in any way that is permitted by the copyright and related rights legislation that applies to your use. For other uses you need to obtain permission from the rights-holder(s).
thesis.degree.disciplineChemistry
thesis.degree.grantorColorado State University
thesis.degree.levelDoctoral
thesis.degree.nameDoctor of Philosophy (Ph.D.)

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