101. Accessing Transition Metal-Hydride Complexes Through Proton-Coupled Electron Transfer Processes
- Author
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Kurtz, Daniel Adam
- Abstract
The combustion of fossil fuels such as coal, natural gas, and oil is the primary source of energy to power our everyday lives. These energy sources are non-renewable and their continued consumption will only accelerate the already evident warming of the planet. One of the primary products of burning fossil fuels, carbon dioxide (fossil fuels are carbon-based fuels), has increased by 24% in the past 60 years which can be explained by the increased global energy demand and subsequent acceleration of fossil fuel consumption. It is unreasonable, though, to immediately stop our use of fossil fuels as an energy source without a viable replacement. Although it is 93 million miles away, the largest energy source available to humans is the sun. Nature has evolved to utilize the vast quantity of solar irradiation that illuminates the earth in order to perform complex photochemical reactions such as the biosynthesis of sugars. While there are researchers who are attempting to mimic the structure and function of these biological systems, the research discussed in this dissertation is focused on a more energy-relevant transformation: the conversion of solar energy into the simplest chemical fuel, hydrogen fuel. Transition metal complexes are capable of performing all the required steps needed to convert sunlight into hydrogen fuel: absorption of solar radiation, and catalytic orchestration of the combination of the two electrons and two protons required to form H2. While known technology exists for this conversion, the efficiency of all required steps are currently not at a level that makes the system economically/commercially viable. The work discussed herein is related to key steps in the path from solar energy to H2. The first chapter is focused on factors that influence the formation of a transition metal hydride complex, a key intermediate in catalytic hydrogen production. Chapter 2 then describes a model system in which to study hydride formation using two different methods is described, and Chapter 3 discusses systematic variation in structural parameters on the model system and how they influence hydride formation is then discussed. Finally, presented in Chapter 4 are efforts to improve the spectral absorbance of an existing class of chromophores, followed by efforts to directly form transition metal hydrides via light absorption in Chapter 5.
- Published
- 2019
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