Abstract

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.

Graduation Date

2016

Semester

Fall

Advisor

Roldan Cuenya, Beatriz

Degree

Doctor of Philosophy (Ph.D.)

College

College of Sciences

Department

Physics

Degree Program

Physics

Format

application/pdf

Identifier

CFE0006482

URL

http://purl.fcla.edu/fcla/etd/CFE0006482

Language

English

Release Date

December 2017

Length of Campus-only Access

1 year

Access Status

Doctoral Dissertation (Campus-only Access)

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