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Synergistic computational and experimental chemical investigations for the advancement of sustainable energy technologies
Etz, Brian D.
Etz, Brian D.
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2020
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2021-10-15
Abstract
Sustainable energy technologies are becoming ever more crucial to support the increasing energy demands facing society and to stem the growing effects of pollution on the diminished health of our planet. Advancing current sustainable energy technologies will be critical in suppressing and eliminating the current reliance on harmful fossil fuel-based energy sources. The research presented in this thesis involves the investigation of underlying chemistry of three viable sustainable energy technologies. The technologies pursued in this work are solar, nuclear, and biomass energy sources, and the investigation of the three research projects was performed using a combined computational and experimental approach. Density functional theory (DFT) calculations in conjunction with synthetic and spectroscopic methods were employed to effectively probe the photochemistry of flavins for the improvement of organic photocatalysts, to elucidate the structure of important metal-extractant complexes during recycling of spent nuclear fuel, and to determine the effect chemical structure and position of oxygen functional groups has on the sooting tendencies of biomass-derived oxygen aromatic compounds. Modulation of the photochemistry of flavinium cations and flavins, biomimetic photocatalysts, was determined to occur with varying the electronic nature of functional groups and the position of functionalization. Synthesis of a series of chlorinated flavins was performed, and computational and experimental results indicate that functionalizing the C7 and C8 position will either improve or hurt the activity of the triplet excited state, catalytically active state, and lead to tuning of the flavin photocatalysis. Furthermore, insight into the synthetic mechanism of flavin materials was gained by studying the structure and reactivity of alloxan monohydrate, an important reagent in the formation of the flavin tricyclic structure. The Actinide Lanthanide SEParation process was investigated to gain insight into the separation mechanism and promote the improved reprocessing of spent nuclear fuel from nuclear reactors. The identity of important metal-extractant complexes was elucidated using time-resolved laser-induced fluorescence spectroscopy and DFT calculations. Lastly, the soot formation chemical pathways of promising biomass-derived fuels was investigated computationally. The formation of soot was determined to be heavily affected by the position of oxygen substituents and strategies for designing low-emission fuels has been presented. In conclusion, the present dissertation presents the investigations of three tangential research projects aiming to collectively further the chemical understanding of solar, nuclear, and biomass energy technologies.
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