Copper and iron zeolites : their active sites and contributions to reactivity

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Abstract/Contents

Abstract
Copper and iron exchanged zeolites have been shown to selectively convert methane to methanol at low temperatures. This one-step, selective conversion of methane to methanol is extremely difficult and further understanding is required to create materials that could perform this controlled reaction at a larger scale. This thesis presents advancements in the spectroscopic and computational characterization of these unique active sites as well as the requirements for their formation. This work builds off concepts from bioinorganic to define the contributions from the first and second coordination sphere of zeolites that contribute to this reactivity. The first part of this thesis focuses on copper active sites and describes the structural assignments of a new binuclear active site and a mononuclear active site. This enables an evaluation of the effects of nuclearity on reactivity. The second part of this thesis focuses on iron zeolites and presents the structural assignments of the alpha-Fe(II) precursor and the alpha-O active site that takes methane to methanol at room temperatures. Included are the formation of the alpha-Fe site in the zeolite lattice, the reactivity of alpha-O with benzene in the Fe-*BEA lattice, and a comparison of the reaction of alpha-O with methane in the large channel Fe-*BEA and small pore Fe-CHA zeolite lattices. The last study demonstrates that lattice topology can control the reactivity.

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 2022; ©2022
Publication date 2022; 2022
Issuance monographic
Language English

Creators/Contributors

Author Rhoda, Hannah Marie
Degree supervisor Solomon, Edward I
Thesis advisor Solomon, Edward I
Thesis advisor Hodgson, K. O. (Keith O.), 1947-
Thesis advisor Karunadasa, Hemamala
Degree committee member Hodgson, K. O. (Keith O.), 1947-
Degree committee member Karunadasa, Hemamala
Associated with Stanford University, Department of Chemistry

Subjects

Genre Theses
Genre Text

Bibliographic information

Statement of responsibility Hannah Marie Rhoda.
Note Submitted to the Department of Chemistry.
Thesis Thesis Ph.D. Stanford University 2022.
Location https://purl.stanford.edu/dh725jn8714

Access conditions

Copyright
© 2022 by Hannah Marie Rhoda
License
This work is licensed under a Creative Commons Attribution Non Commercial 3.0 Unported license (CC BY-NC).

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