Understanding catalyst structure-performance relationships through precise synthesis and in situ characterization
Abstract/Contents
- Abstract
- Heterogeneous catalysis will play an important role in facilitating chemical reactions with sustainable energy conversion and environmental applications. The performance of a catalyst can be affected by many different physical, chemical, and electronic properties of the material. The relationships between these properties and catalytic reactivity are not well-understood and as a result, the design of high-performance catalysts has been a significant challenge. In this dissertation, we synthesize catalysts using precise methods, including atomic layer deposition (ALD) and colloidal nanocrystal synthesis. By analyzing the properties of these controlled catalytic materials during reaction using in situ methods, we understand the relationships between structure and performance. This strategy is applied to the study of several catalytic systems for sustainable energy and environmental processes. One promising pathway towards the long-term production of fuels and chemicals is through the catalytic conversion of syngas to higher oxygenates. Several classes of catalysts have emerged as promising candidates for direct higher oxygenate synthesis from syngas: rhodium-based materials, mixed Fischer-Tropsch and methanol synthesis metals, and alternatives to pure metals. In the first part of this dissertation, we study the properties of one example catalyst from each of these classes. The last two studies in this dissertation highlight general design strategies and principles in the study of heterogeneous catalysts. We show the importance of impurity control in achieving the desired catalytic performance, a factor that is often overlooked in catalyst design. Finally, we develop a procedure combining ALD and colloidal nanocrystal synthesis that can be used to study metal-support interaction in a wide variety of catalyst systems. Throughout this dissertation, emphasis is placed on structure-performance relationships, controlled catalyst synthesis using atomically precise methods, and in situ characterization. We show how an understanding of the effects of physical and chemical catalyst properties on reactivity can be used to intelligently design higher performance catalysts. Precise synthesis methods play an important role in elucidating these structure-performance relationships and in enabling the synthesis of catalytic materials with the desired nanoscale properties. Characterization of catalyst structures are further enabled by in situ methods, which allow active sites and surface characteristics to be identified. The results in this dissertation contribute to and provide guidance for the design, synthesis, and characterization of high-performance heterogeneous catalysts.
Description
| Type of resource | text |
|---|---|
| Form | electronic resource; remote; computer; online resource |
| Extent | 1 online resource. |
| Place | California |
| Place | [Stanford, California] |
| Publisher | [Stanford University] |
| Copyright date | 2021; ©2021 |
| Publication date | 2021; 2021 |
| Issuance | monographic |
| Language | English |
Creators/Contributors
| Author | Asundi, Arun Somayaji |
|---|---|
| Degree supervisor | Bent, Stacey |
| Thesis advisor | Bent, Stacey |
| Thesis advisor | Bare, Simon |
| Thesis advisor | Cargnello, Matteo |
| Degree committee member | Bare, Simon |
| Degree committee member | Cargnello, Matteo |
| Associated with | Stanford University, Department of Chemical Engineering |
Subjects
| Genre | Theses |
|---|---|
| Genre | Text |
Bibliographic information
| Statement of responsibility | Arun Somayaji Asundi. |
|---|---|
| Note | Submitted to the Department of Chemical Engineering. |
| Thesis | Thesis Ph.D. Stanford University 2021. |
| Location | https://purl.stanford.edu/gj378zn8906 |
Access conditions
- Copyright
- © 2021 by Arun Somayaji Asundi
- License
- This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).
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