Nanomaterial design via ALD : new methods and applications in catalysis
Abstract/Contents
- Abstract
- Producing chemicals and liquid fuels from renewable carbon monoxide and hydrogen (syngas) is a key route towards an environmentally sustainable economy. Alcohols beyond methanol are key targets for fuel and chemical production; however despite almost a century of research, there are no industrially appropriate catalysts for the direct formation of these compounds. New methods are needed to synthesize catalysts for higher alcohol production from syngas. Atomic layer deposition (ALD) is one such synthetic strategy. In this thesis, a new method for ALD nanoparticle synthesis was developed that can be used to prepare catalysts. Using oxygen gas as the co-reactant, area-selective ALD of metal oxides by metalorganic precursors that typically reactive strong oxidants to proceed was achieved selectively on noble metal surfaces by exploiting the catalytic dissociation of oxygen molecules at the metal surface. To explore metal alloy catalysts for syngas conversion, CoZn and PtCo catalysts were synthesized through a combination of traditional wet synthesis and ALD. During synthesis, the number ALD cycles was tuned to optimize catalytic performance with precise control. These catalysts had greatly improved selectivity for the alcohols during syngas conversion. By performing in-situ measurements of CoZn at high pressure, it was discovered that the presence of Zn leads to Co2C formation during catalyst operation. The resulting Co2C was found to be critical in alcohol formation on these catalysts. Beyond CO, CO2 is an emerging feedstock for renewable chemical production. New CoGa catalysts were synthesized for CO2 hydrogenation. The Co:Ga ratio was found to play a critical role in the selectivity, with increasing Co content favoring methane production and increasing Ga content favoring dimethyl ether production.
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 | 2018; ©2018 |
| Publication date | 2018; 2018 |
| Issuance | monographic |
| Language | English |
Creators/Contributors
| Author | Singh, Joseph |
|---|---|
| Degree supervisor | Bent, Stacey |
| Thesis advisor | Bent, Stacey |
| Thesis advisor | Chidsey, Christopher E. D. (Christopher Elisha Dunn) |
| Thesis advisor | Kanan, Matthew William, 1978- |
| Degree committee member | Chidsey, Christopher E. D. (Christopher Elisha Dunn) |
| Degree committee member | Kanan, Matthew William, 1978- |
| Associated with | Stanford University, Department of Chemistry. |
Subjects
| Genre | Theses |
|---|---|
| Genre | Text |
Bibliographic information
| Statement of responsibility | Joseph Singh. |
|---|---|
| Note | Submitted to the Department of Chemistry. |
| Thesis | Thesis Ph.D. Stanford University 2018. |
| Location | electronic resource |
Access conditions
- Copyright
- © 2018 by Joseph Singh
- License
- This work is licensed under a Creative Commons Attribution Non Commercial No Derivatives 3.0 Unported license (CC BY-NC-ND).
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