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Determination of reliable minimum, disproof-based particle formation mechanisms: investigation of a second-generation Ir(0)n nanoparticle system

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dc.contributor.authorWhitehead, Christopher Breck, author
dc.contributor.authorFinke, Richard, advisor
dc.contributor.authorNeilson, Jamie, committee member
dc.contributor.authorVan Orden, Alan, committee member
dc.contributor.authorShipman, Patrick, committee member
dc.date.accessioned2021-06-07T10:21:02Z
dc.date.available2022-06-02T10:21:02Z
dc.date.issued2021
dc.description.abstractA long-sought goal in particle formation is an understanding of the chemical reaction mechanism. The complete understanding of the associated processes (nucleation, growth, and agglomeration) will yield particle size and distribution control. Mechanistic control and knowledge will yield improvements in the development of renewable energy and catalytic materials. The current state of chemical reaction mechanisms and the direct methods to study them are presented in an in-depth literature review in Chapter II. The best, state-of-the-art case studies are examined and the minimum criteria for a reliable, disproof-based chemical mechanism are presented. The experimental work presented in this dissertation centers on a second-generation {[(1,5-COD)IrI•HPO4]2}2– precursor to Ir(0)~150(HPO42–)x nanoparticle system. The exhaustive investigation of the reaction speciation and the dependence of IrI and HPO42– concentrations on the reaction kinetics are presented in Chapter III. Based on the reaction kinetics and there experimentally determined nucleation step, the molecular mechanism of Ir(0)~150(HPO42–)x nanoparticle formation is elucidated. Next, in Chapter IV, the second-generation {[(1,5-COD)IrI•HPO4]2}2– precursor to Ir(0)~150(HPO42–)x nanoparticle system is monitored directly by X-ray absorption spectroscopy and small-angle X-ray scattering and indirectly by in-house cyclohexene reporter reaction, gas-liquid chromatography, proton nuclear magnetic resonance, and transmission electron microscopy. A total of 6 physical methods are used to follow the particle formation kinetics. Finally, mechanism-enabled population balance modeling is applied as a final test of the proposed mechanism.
dc.format.mediumborn digital
dc.format.mediumdoctoral dissertations
dc.identifierWhitehead_colostate_0053A_16469.pdf
dc.identifier.urihttps://hdl.handle.net/10217/232586
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.subjectiridium
dc.subjectnanoparticle
dc.subjectdisproof-based
dc.subjectnucleation
dc.subjectmechanism
dc.titleDetermination of reliable minimum, disproof-based particle formation mechanisms: investigation of a second-generation Ir(0)n nanoparticle system
dc.typeText
dcterms.embargo.expires2022-06-02
dcterms.embargo.terms2022-06-02
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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