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INVESTIGATION OF THE HYDROCARBON POOL SPECIES RESPONSIBLE FOR METHANOL TO OLEFIN CATALYSIS ON ACIDIC ZEOLITE AND ZEOTYPE CATALYSTS
by
Darryl Roy Guenther
____________________________________________________________________
A Dissertation Presented to the
FACULTY OF THE USC GRADUATE SCHOOL
UNIVERSITY OF SOUTHERN CALIFORNIA
In Partial Fulfillment of the
Requirements for the Degree
DOCTOR OF PHILOSOPHY
(CHEMISTRY)
December 2010
Copyright 2010 Darryl Roy Guenther
Object Description
| Title | Investigation of the hydrocarbon pool species responsible for methanol to olefin catalysis on acidic zeolite and zeotype catalysts |
| Author | Guenther, Darryl Roy |
| Author email | dguenthe@usc.edu; hazywater@gmail.com |
| Degree | Doctor of Philosophy |
| Document type | Dissertation |
| Degree program | Chemistry |
| School | College of Letters, Arts and Sciences |
| Date submitted | 2010 |
| Restricted until | Unrestricted |
| Date published | 2010-09-14 |
| Advisor (committee chair) | Haw, James |
| Advisor (committee member) |
Jessen, Kristian Wittig, Kurt |
| Abstract | The main theme of this dissertation is the study of aromatic hydrocarbon pool in the catalysis of methanol conversion to light olefins on zeolite and zeotype materials through the usage of gas chromatography, mass spectrometry, and isotopic labeling. The goal was to identify and characterize the species responsible for the majority of ethylene produced in methanol-to-olefin catalysis. The mechanism for methanol to olefin catalysis was originally thought to only proceed through an aromatic hydrocarbon pool, but this was difficult to reconcile with product spectrums of different catalysts. From this developed a dual cycle mechanism consisting of two hydrocarbon pools.; Ethylene is the most valuable of the products produced from methanol to olefin catalysis. Modifying catalysts or reaction conditions to maximize ethylene selectivity requires an understanding of which hydrocarbon pool produces ethylene in the highest selectivity and just how selective that hydrocarbon pool is.; The first two chapters of this dissertation pertain to a general overview of zeolites, zeotypes, and the methanol to olefins reaction. An understanding of the methanol to olefins reaction and the catalysts that make it possible are necessary for the remaining two chapters. The latter two chapters focus on the aromatic hydrocarbon pool and its role in methanol to olefins catalysis. Chapter three focuses on determining the selectivity of the two most valuable products of methanol to olefin catalysis – ethylene and propylene. This selectivity is determined for both the aromatic hydrocarbon pool and the olefinic hydrocarbon pool while minimizing the effects of the alternate hydrocarbon pool. In chapter four, the product spectrum of the reaction of several polymethylbenzenes are determined over a zeotype and zeolite that share the faujasite topology. Results confirm that methylated aromatic species are the best route to ethylene in methanol to olefins catalysis, and that a higher acid strength is more selective for ethylene. |
| Keyword | MTO; catalysis; zeolite; methanol to olefin; solid acid |
| 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-m3429 |
| Rights | Guenther, Darryl Roy |
| Repository name | Libraries, University of Southern California |
| Repository address | Los Angeles, California |
| Repository email | http://www.usc.edu/isd/libraries/services/ask_a_librarian/email/ |
| Filename | etd-Guenther-4095 |
| Archival file | uscthesesreloadpub_Volume29/etd-Guenther-4095.pdf |
Description
| Title | Page 1 |
| Full text | INVESTIGATION OF THE HYDROCARBON POOL SPECIES RESPONSIBLE FOR METHANOL TO OLEFIN CATALYSIS ON ACIDIC ZEOLITE AND ZEOTYPE CATALYSTS by Darryl Roy Guenther ____________________________________________________________________ A Dissertation Presented to the FACULTY OF THE USC GRADUATE SCHOOL UNIVERSITY OF SOUTHERN CALIFORNIA In Partial Fulfillment of the Requirements for the Degree DOCTOR OF PHILOSOPHY (CHEMISTRY) December 2010 Copyright 2010 Darryl Roy Guenther |
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