One of the most pressing challenges of our time is meeting growing global energy demands while limiting human impact on the environment. To meet this challenge, new catalysts are needed to enable carbon neutral energy production processes and low cost synthesis of alternative fuels. In order to design new catalysts for such processes, fundamental understanding is needed on how the structural and chemical properties of nanostructured materials influences their surface chemistry. In this dissertation, I explore how the properties of nanoparticles, such as particle size, shape, composition, and chemical state, can be used to tune their reactivity. For this work, model nanoparticles were synthesized with well-defined structural and chemical properties, and a variety of surface science approaches were used for catalyst characterization. In particular, emphasis was placed on understanding the changes which may occur in the catalyst structure and chemical state during a reaction using advanced in situ techniques and correlating these changes to reactivity. After exploring how nanostructuring the catalyst surface can be used to tune reactivity and how dynamic changes can occur to nanocatalysts in reactive environments, these general principles are applied to a model reaction, the electroreduction of carbon dioxide, which is a promising process for synthesizing valuable products using renewable energy while consuming waste carbon dioxide. I explore the mechanisms behind how catalyst particle size, composition, and oxidation state can be used to improve activity and tune selectivity towards different carbon dioxide reduction products. Such fundamental mechanistic insights are critically needed to design efficient catalysts for this reaction.
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Roldan Cuenya, Beatriz
Doctor of Philosophy (Ph.D.)
College of Sciences
Length of Campus-only Access
Doctoral Dissertation (Open Access)
Mistry, Hemma, "Model Nanocatalysts with Tunable Reactivity: Tailoring the Structure and Surface Chemistry of Nanomaterials for Energy and Alternative Fuels Catalysis" (2016). Electronic Theses and Dissertations, 2004-2019. 5324.