Surface Reactions of Biomass Derived Oxygenates on Lewis Acidic Metal Oxides
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Najmi, Sean
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Abstract
Lignocellulosic biomass is currently the only source of organic carbon making it a sustainable source for production of liquid hydrocarbon fuels. One main challenge for valorization of biomass is reducing the oxygen content of the starting feedstock and producing high value chemicals. Using heterogeneous catalysts for conversion of biomass feedstock to commodity chemicals is one strategy for the valorization process. Specifically, using Lewis acidic metal oxides for this upgrading process has shown promise due to its ability to catalyze relevant reactions such as isomerization and (retro-) aldol condensation. This work seeks to elucidate the surface interactions of biomass derived oxygenates with solid Lewis acid sites. This is done using in-situ spectroscopic techniques such as Fourier transformed infrared, nuclear magnetic resonance and ultra-violet spectroscopies. These techniques were applied for studying the following reactions: (i) aldol condensation of ethanol and acetaldehyde over reduced molybdenum oxide; (ii) aldol condensation of acetaldehyde over supported molybdenum oxides; (iii) dehydration and retro-aldol condensation of C4 polyoxygenates using various Lewis acidic metal oxides and (iv) ring opening and esterification of erythrose using various Lewis acidic metal oxides. Surface properties such as Lewis and Brønsted acid site and reducibility of metal center are essential to rationalizing the reaction pathway of the above reactions. The aforementioned studies provide fundamental knowledge regarding how different oxygenates can interact with solid Lewis acid sites.
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2021-12-13
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Dissertation