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Tuning reaction environments for rate and selectivity control in heterogenous catalysis
Vyas, Manasi V.
Vyas, Manasi V.
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Kwon, Stephanie
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2025
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Vyas_mines_0052E_13038.pdf
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- Embargoed until 2026-11-11
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2026-11-11
Abstract
Heterogeneous catalysis is critical in many chemical industries, enabling process efficiency. Advances in understanding the mechanistic details of surface reactions and catalyst properties have facilitated the development of novel catalysts tailored for specific reactions. Catalytic environments, which include active sites and surrounding microenvironments, greatly influence catalytic performance. Active sites, where reactants bind and undergo transformation, are essential for determining reaction rates and selectivities, while microenvironments can also affect reactivity through effects such as confinement.
To fully understand catalytic systems, a range of techniques are required, including kinetic studies, infrared (IR) spectroscopy, and computational methods such as density functional theory (DFT). These approaches provide insights into elementary steps, reaction pathways, and origins of catalytic activity. This thesis explores two projects that advance our understanding of active sites and microenvironments. The first project investigates the impact of Pd to PdO phase transformation on hydrogen peroxide (H2O2) synthesis and decomposition pathways, revealing how geometry and electronic effects of Pd affect catalytic behavior, synthesis rates, and selectivities. The second project focuses on advancing base-catalyzed sol-gel methods to tailor SiO2 microenvironments around Ti-O Lewis-acid base pairs on TiO2, enhancing alcohol dehydration reactions by leveraging confinement effects. An extension of this work investigates 2-propanol dehydration and dehydrogenation mechanisms on TiO2, highlighting the role of water on acid-base sites and their role in reaction rates and product selectivities.
This work advances catalyst design and performance by enhancing our understanding of how active site transformations and microenvironments influence reactivity and selectivity, thereby driving innovation and promoting sustainability in chemical industries.
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