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125
B. Lok, C. Messina, R. Patton, R. Gajek, T. Cannan, and E. Flanigen,
“Crystalline Silicoaluminophosphates,” U.S. Patent 4,440,871, 1984.
T. Maesen, “The Zeolite Scene- An Overview,” Introduction of Zeolite
Science and Practice, Oxford: Elsevier, 2007, pp. 1-12.
C.J. Maiden, “The New Zealand Gas-to-Gasoline Project,” Studies in
Surface Science and Cataylsis, Elsevier, 1988, pp. 1-16.
D. McCann, D. Lesthaeghe, P. Kletnieks, D. Guenther, M. Hayman, V. Van
Speybroeck, M. Waroquier, and J. Haw, “A Complete Catalytic Cycle for
Supramolecular Methanol‐to‐Olefins Conversion by Linking Theory with
Experiment,” Angewandte Chemie International Edition, vol. 47, 2008, pp.
5179-5182.
“Methanol Institute,” Methanol Institute. www.methanol.org
T. Mole, J.A. Whiteside, and D. Seddon, “Aromatic co-catalysis of methanol
conversion over zeolite catalysts,” Journal of Catalysis, vol. 82, Aug. 1983,
pp. 261-266.
T. Mole, G. Bett, and D. Seddon, “Conversion of methanol to hydrocarbons
over ZSM-5 zeolite: An examination of the role of aromatic hydrocarbons
using 13carbon- and deuterium-labeled feeds,” Journal of Catalysis, vol. 84,
Dec. 1983, pp. 435-445.
D.K. Murray, J.W. Chang, and J.F. Haw, “Conversion of methyl halides to
hydrocarbons on basic zeolites: a discovery by in situ NMR,” Journal of the
American Chemical Society, vol. 115, Jun. 1993, pp. 4732-4741.
G.A. Olah and R.H. Schlosberg, “Chemistry in super acids. I. Hydrogen
exchange and polycondensation of methane and alkanes in FSO3H-SbF5
("magic acid") solution. Protonation of alkanes and the intermediacy of CH5+
and related hydrocarbon ions. The high chemical reactivity of "paraffins" in
ionic solution reactions,” Journal of the American Chemical Society, vol. 90,
May. 1968, pp. 2726-2727.
U. Olsbye, M. Bjørgen, S. Svelle, K. Lillerud, and S. Kolboe, “Mechanistic
insight into the methanol-to-hydrocarbons reaction,” Catalysis Today, vol.
106, Oct. 2005, pp. 108-111.
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 136 |
| Contributing entity | University of Southern California |
| Repository email | cisadmin@lib.usc.edu |
| Full text | 125 B. Lok, C. Messina, R. Patton, R. Gajek, T. Cannan, and E. Flanigen, “Crystalline Silicoaluminophosphates,” U.S. Patent 4,440,871, 1984. T. Maesen, “The Zeolite Scene- An Overview,” Introduction of Zeolite Science and Practice, Oxford: Elsevier, 2007, pp. 1-12. C.J. Maiden, “The New Zealand Gas-to-Gasoline Project,” Studies in Surface Science and Cataylsis, Elsevier, 1988, pp. 1-16. D. McCann, D. Lesthaeghe, P. Kletnieks, D. Guenther, M. Hayman, V. Van Speybroeck, M. Waroquier, and J. Haw, “A Complete Catalytic Cycle for Supramolecular Methanol‐to‐Olefins Conversion by Linking Theory with Experiment,” Angewandte Chemie International Edition, vol. 47, 2008, pp. 5179-5182. “Methanol Institute,” Methanol Institute. www.methanol.org T. Mole, J.A. Whiteside, and D. Seddon, “Aromatic co-catalysis of methanol conversion over zeolite catalysts,” Journal of Catalysis, vol. 82, Aug. 1983, pp. 261-266. T. Mole, G. Bett, and D. Seddon, “Conversion of methanol to hydrocarbons over ZSM-5 zeolite: An examination of the role of aromatic hydrocarbons using 13carbon- and deuterium-labeled feeds,” Journal of Catalysis, vol. 84, Dec. 1983, pp. 435-445. D.K. Murray, J.W. Chang, and J.F. Haw, “Conversion of methyl halides to hydrocarbons on basic zeolites: a discovery by in situ NMR,” Journal of the American Chemical Society, vol. 115, Jun. 1993, pp. 4732-4741. G.A. Olah and R.H. Schlosberg, “Chemistry in super acids. I. Hydrogen exchange and polycondensation of methane and alkanes in FSO3H-SbF5 ("magic acid") solution. Protonation of alkanes and the intermediacy of CH5+ and related hydrocarbon ions. The high chemical reactivity of "paraffins" in ionic solution reactions,” Journal of the American Chemical Society, vol. 90, May. 1968, pp. 2726-2727. U. Olsbye, M. Bjørgen, S. Svelle, K. Lillerud, and S. Kolboe, “Mechanistic insight into the methanol-to-hydrocarbons reaction,” Catalysis Today, vol. 106, Oct. 2005, pp. 108-111. |
