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12
acid, the precursor of PETE plastics.8 HZSM-5 has also been used to make
synthetic gasoline, a process that will be discussed further in Chapter 2.
1.4. SAPO-34
SAPO-34, depicted in Figure 1.4, is a synthetic silico-aluminophosphate of
CHA topology patented by Union Carbide chemists in 1984.9 The main use
Figure 1.4. CHA topology shared by chabazite and SAPO-34. In this
illustration, red represents oxygen atoms and blue, tetrahedral T-atoms as
chabazite and SAPO-34 have different framework compositions. The CHA
topology is a small, three-dimensional composed of three 8 T-atom channels,
each perpendicular to two others. If the structure above were rotated 90° in
any direction, the resulting image would be identical. However the more
important feature is the chabazite cage illustrated in subsequent figures.
Object Description
| Title | Modification of methanol-to-olefin hydrocarbon pool species by oxygenates on acidic zeolites |
| Author | Hayman, Miranda Jeanette |
| Author email | mirandah@usc.edu; mirandahayman@gmail.com |
| Degree | Doctor of Philosophy |
| Document type | Dissertation |
| Degree program | Chemistry |
| School | College of Letters, Arts and Sciences |
| Date defended/completed | 2011-02-11 |
| Date submitted | 2011 |
| Restricted until | Unrestricted |
| Date published | 2011-04-26 |
| Advisor (committee chair) | Haw, James F. |
| Advisor (committee member) |
Flood, Thomas C. Jessen, Kristian |
| Abstract | The mechanism of methanol-to-olefin (MTO) catalysis employs organic reaction centers, both aromatic and olefinic, to generate olefins on acid zeolites. Generally, propene is the favored MTO olefin on most zeolite catalysts, but ethylene is a more desirable olefin due to its prevalence in consumer plastics. Much research has been conducted to alter the MTO product selectivities to favor ethylene. This focus of this dissertation is selective modification of the olefinic reaction centers, converting them into aromatic reaction centers known to be responsible for the majority of ethylene production.; Formaldehyde reactivity was studied on HSAPO-34, and found to react with propene through a Prins reaction to form butadiene, which readily cyclized to aromatic species. Evidence of formaldehyde formation was observed from methanol oxidation on the stainless-steel surface of the reactor tubing. This reaction was then studied in HZSM-5 where olefinic reaction centers dominate the hydrocarbon pool. The olefinic reaction centers were converted to aromatic species, and a significant increase in ethylene selectivity was observed. Other oxygenated species, such as acetaldehyde, were also studied in conjunction with methanol on HZSM-5 and an improvement in ethylene selectivity was noted. The consequence of the increased ethylene selectivity however was an increase in the rate of deactivation due to the accelerated formation of aromatic species. |
| Keyword | MTO; methanol-to-olefins; zeolite; heterogeneous catalysis; hydrocarbon pool; HZSM-5 |
| Language | English |
| Part of collection | University of Southern California dissertations and theses |
| Publisher (of the original version) | University of Southern California |
| Place of publication (of the original version) | Los Angeles, California |
| Publisher (of the digital version) | University of Southern California. Libraries |
| Provenance | Electronically uploaded by the author |
| Type | texts |
| Legacy record ID | usctheses-m3780 |
| Contributing entity | University of Southern California |
| Rights | Hayman, Miranda Jeanette |
| Repository name | Libraries, University of Southern California |
| Repository address | Los Angeles, California |
| Repository email | cisadmin@lib.usc.edu |
| Filename | etd-Hayman-4358 |
| Archival file | uscthesesreloadpub_Volume23/etd-Hayman-4358.pdf |
Description
| Title | Page 23 |
| Contributing entity | University of Southern California |
| Repository email | cisadmin@lib.usc.edu |
| Full text | 12 acid, the precursor of PETE plastics.8 HZSM-5 has also been used to make synthetic gasoline, a process that will be discussed further in Chapter 2. 1.4. SAPO-34 SAPO-34, depicted in Figure 1.4, is a synthetic silico-aluminophosphate of CHA topology patented by Union Carbide chemists in 1984.9 The main use Figure 1.4. CHA topology shared by chabazite and SAPO-34. In this illustration, red represents oxygen atoms and blue, tetrahedral T-atoms as chabazite and SAPO-34 have different framework compositions. The CHA topology is a small, three-dimensional composed of three 8 T-atom channels, each perpendicular to two others. If the structure above were rotated 90° in any direction, the resulting image would be identical. However the more important feature is the chabazite cage illustrated in subsequent figures. |
