Gold-catalyzed alcohol oxidation reactions : insights from surface science and classical catalysis studies
Mullen, Gregory Michael
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Catalysts play an extremely important role in shaping the world around us. Foods, plastics, fuels, medicines, and countless other materials that are integral to our way of life rely on catalysts for their production. Despite their importance, to this day catalysts are still mysterious materials with active sites and reaction mechanisms that often remain unknown despite decades of investigation. In this dissertation, we investigate the use of gold catalysts for selective oxidation of alcohols, an important class of reaction used in the agrochemical, pharmaceutical, and fine chemicals industries. Using surface science and classical catalysis techniques, we demonstrate that water plays important and previously undiscovered roles in these processes, altering reaction mechanisms and influencing the selectivity exhibited by the catalysts for primary and secondary oxidation pathways. Additionally, we show that the structure and the composition of the support material both influence the activity and selectivity of gold catalysts for alcohol oxidation. Our results highlight the complexity that catalytic reaction mechanisms can exhibit and the structure-function relationships that can dictate their behavior. Knowledge of these factors is extremely valuable optimizing the design and implementation of catalytic processes. By leveraging knowledge like this, we will be able to mitigate the generation of industrial waste make better use of our natural resources.