Hong, Sungil
(2024)
Understanding the Functionality of Zeolite-Stabilized Single-Atom Catalysts.
Doctoral Dissertation, University of Pittsburgh.
(Unpublished)
Abstract
A swift transition from growth-oriented development to sustainable development is an inevitable necessity for the future. Without drastic measures across all the economic sections to limit the Earth’s temperature rise, present and future generations will encounter catastrophic, life-threatening climate changes. Catalysts are key materials for mitigating the carbon footprint of chemical processes. Single-atom catalysts (SACs) have emerged as a new frontier in heterogeneous catalysis due to their superior activity and metal utilization efficiency. Zeolites are promising support materials for SACs due to their shape selectivity and tunable physicochemical properties. The atomic dispersion of active metals in the micropores of zeolites can give rise to exceptionally high catalytic performances.
This dissertation focuses on advancing the understanding of zeolite-stabilized SACs with the use of first-principles calculations and multiscale modeling. Specifically, computational findings rationalize experimental observations in nucleation, phase transition, and modification of zeolites, guiding methodologies for their targeted synthesis for catalytic applications. Furthermore, the computational framework for simulating complex catalytic reactions presented herein paves the way for discovering and designing novel catalysts. The crucial role of oxidation states of the metal sites and their synergistic effects with zeolite supports are addressed in detail, suggesting key features that need to be emphasized in future research endeavors. Overall, this dissertation offers fundamental knowledge for the synthesis, manipulation, and application of zeolite-stabilized SACs, bridging the gap in our current understandings and highlighting their potential to sustainable chemical processes.
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Details
| Item Type: |
University of Pittsburgh ETD
|
| Status: |
Unpublished |
| Creators/Authors: |
|
| ETD Committee: |
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| Date: |
6 September 2024 |
| Date Type: |
Publication |
| Defense Date: |
11 June 2024 |
| Approval Date: |
6 September 2024 |
| Submission Date: |
1 July 2024 |
| Access Restriction: |
No restriction; Release the ETD for access worldwide immediately. |
| Number of Pages: |
130 |
| Institution: |
University of Pittsburgh |
| Schools and Programs: |
Swanson School of Engineering > Petroleum Engineering |
| Degree: |
PhD - Doctor of Philosophy |
| Thesis Type: |
Doctoral Dissertation |
| Refereed: |
Yes |
| Uncontrolled Keywords: |
single atom catalysts, catalysis, heterogeneous catalyst, zeolites, computational chemistry, density functional theory, zeolite crystallization, interzeolite transformation, defect engineering, methane, methane partial oxidation, ammonia, ammonia decomposition, ammonia cracking |
| Date Deposited: |
06 Sep 2024 19:57 |
| Last Modified: |
06 Sep 2024 19:57 |
| URI: |
http://d-scholarship.pitt.edu/id/eprint/46644 |
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