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iii
ACKNOWLEDGEMENTS
I would like to thank my advisor Dr. James Haw. In 2003, he took a
chance on small town girl from Ohio and invited me to join his group for a
summer REU program. That experience was what encouraged me to attend
graduate school. His support and guidance regarding the chemistry, as well
as discussions far removed from chemistry, are what kept me here.
I would like to thank all of my committee members: Dr. Flood,
Dr. Jessen, Dr. Reisler, Dr. Barrios, and Dr. Stott for taking the time to
participate in my progress towards a Ph.D. I am grateful for USC and the
Chemistry Department in particular for allowing me this opportunity.
Special thanks are extended to all the members of the Haw lab, past
and present, which helped me learn the ropes and provided companionship
throughout the course of research: Dr. Joe Abubakar, Dr. Phil Kletnieks, Dr.
David McCann, Dr. Darryl Guenther, Cara Malolepsy, Meghan Klaric, Yoni
Blau, Abbey Joyce, and Mallory Pirogovsky. Dr. David Marcus was
particularly helpful in teaching me the chemistry of the Haw lab.
I wish to thank my family for supporting me through this whole
process, and especially my mother Cathy McCoy. Words alone cannot
describe how grateful I am for all the sacrifices she made to provide me with
this education.
Finally, thank-you to my wonderful fiancé Darryl for helping me
maintain my sanity.
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 3 |
| Contributing entity | University of Southern California |
| Repository email | cisadmin@lib.usc.edu |
| Full text | iii ACKNOWLEDGEMENTS I would like to thank my advisor Dr. James Haw. In 2003, he took a chance on small town girl from Ohio and invited me to join his group for a summer REU program. That experience was what encouraged me to attend graduate school. His support and guidance regarding the chemistry, as well as discussions far removed from chemistry, are what kept me here. I would like to thank all of my committee members: Dr. Flood, Dr. Jessen, Dr. Reisler, Dr. Barrios, and Dr. Stott for taking the time to participate in my progress towards a Ph.D. I am grateful for USC and the Chemistry Department in particular for allowing me this opportunity. Special thanks are extended to all the members of the Haw lab, past and present, which helped me learn the ropes and provided companionship throughout the course of research: Dr. Joe Abubakar, Dr. Phil Kletnieks, Dr. David McCann, Dr. Darryl Guenther, Cara Malolepsy, Meghan Klaric, Yoni Blau, Abbey Joyce, and Mallory Pirogovsky. Dr. David Marcus was particularly helpful in teaching me the chemistry of the Haw lab. I wish to thank my family for supporting me through this whole process, and especially my mother Cathy McCoy. Words alone cannot describe how grateful I am for all the sacrifices she made to provide me with this education. Finally, thank-you to my wonderful fiancé Darryl for helping me maintain my sanity. |
