Ligand Design for Energy Conversion and Storage Applications

dc.contributor.advisorRoesler, Roland
dc.contributor.authorHeidebrecht, Joshua
dc.contributor.committeememberPiers, Warren E.
dc.contributor.committeememberVan Humbeck, Jeffrey Francis
dc.date2020-06
dc.date.accessioned2019-12-19T15:52:12Z
dc.date.available2019-12-19T15:52:12Z
dc.date.issued2019-12-17
dc.description.abstractThe contents of this thesis are divided into two topics that fall under the umbrella of energy conversion and storage. The first section focuses on tuning the standard reduction potential of the Fe3+/2+ redox couple with the aid of nitrogen-based ligands, in pursuit of an all-iron, water-based redox-flow battery. Also included is the synthesis and characterization of iron coordination complexes with redox-active ligands featuring quinone/hydroquinone functional groups. This study aims to exploit the potential of this system incorporating Fe3+/2+ and a redox non-innocent ligand for application in single-component redox-flow batteries. The second portion of the thesis targets homogeneous single-site catalysts for the electrochemical reduction of CO2. The ability of nickel and iron complexes incorporating a redox non-innocent bis(triazapentadienyl) ligand to promote this transformation was investigated. The nickel complex was identified as more promising and infrared spectroelectrochemistry was used to determine the fate of the metal during controlled potential electrolysis, as well as to identify the extent to which a large excess of ligand-based redox behavior impacts electrocatalytic CO2 reduction. The synthesis and characterization of other ligand scaffolds based on tetradentate bis(carbene) macrocycles and porphyrinoids is discussed, with alterations to the parent framework aimed at increasing solubility and stability during metal complexation. Also reported are efforts tailored towards the synthesis of ligands based on a bipyridine central donor with flanking phosphine chalcogenides. The phosphine oxide generated iron, nickel and rhenium complexes while the phosphine sulfide analog proved to be a surprisingly incompetent ligand.en_US
dc.identifier.citationHeidebrecht, J. (2019). Ligand Design for Energy Conversion and Storage Applications (Master's thesis, University of Calgary, Calgary, Canada). Retrieved from https://prism.ucalgary.ca.en_US
dc.identifier.doihttp://dx.doi.org/10.11575/PRISM/37346
dc.identifier.urihttp://hdl.handle.net/1880/111355
dc.language.isoengen_US
dc.publisher.facultyScienceen_US
dc.publisher.institutionUniversity of Calgaryen
dc.rightsUniversity of Calgary graduate students retain copyright ownership and moral rights for their thesis. You may use this material in any way that is permitted by the Copyright Act or through licensing that has been assigned to the document. For uses that are not allowable under copyright legislation or licensing, you are required to seek permission.en_US
dc.subjectEnergyen_US
dc.subjectRedox Flow Batteriesen_US
dc.subjectBatteriesen_US
dc.subjectCarbon Dioxideen_US
dc.subjectElectrochemistryen_US
dc.subjectOrganometallicsen_US
dc.subject.classificationEnergyen_US
dc.subject.classificationEngineering--Chemicalen_US
dc.titleLigand Design for Energy Conversion and Storage Applicationsen_US
dc.typemaster thesisen_US
thesis.degree.disciplineChemistryen_US
thesis.degree.grantorUniversity of Calgaryen_US
thesis.degree.nameMaster of Science (MSc)en_US
ucalgary.item.requestcopytrueen_US
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