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ACTIVATION OF METHANE
BY HOMOGENEOUS CATALYSTS
IN WEAKLY ACIDIC SOLVENTS
by
Vadim Rinatovich Ziatdinov
A Dissertation Presented to the
FACULTY OF THE GRADUATE SCHOOL
UNIVERSITY OF SOUTHERN CALIFONIA
In Partial Fulfillment of the
Requirements for the Degree
DOCTOR OF PHILOSOPHY
(CHEMISTRY)
May 2007
Copyright 2007 Vadim Rinatovich Ziatdinov
Object Description
| Title | Activation of methane by homogeneous catalyst in weakly acidic solvents |
| Author | Ziatdinov, Vadim Rinatovich |
| Author email | vadimius@gmail.com |
| Degree | Doctor of Philosophy |
| Document type | Dissertation |
| Degree program | Chemistry |
| School | College of Letters, Arts and Sciences |
| Date defended/completed | 2007 |
| Date submitted | 2007 |
| Restricted until | Unrestricted |
| Date published | 2007-05-17 |
| Advisor (committee chair) | Periana, Roy A. |
| Advisor (committee member) |
Olah, George A. Steier, William H. |
| Abstract | This dissertation describes the latest development in engaging simple hydrocarbons in reaction by CH activation. From initially fuming oleum condition and catalysis like halogens, the trend goes to gold catalyst in 96% sulfuric acid, and later to variety platinum complexes in weak organic acids. The story concentrates on discovery of basic physical phenomenons to enhance reactivity versus specific synthetic applications. -- Chapter One introduces the C-H activation and functionalization of alkanes via the electrophilic mechanism, and discusses the role of non-coordinating solvents and the related problem of inhibition of electophilic catalysts by products such as methanol and water. The simplest iodine and mercury in sulfuric acid catalysts described.; Chapter Two shows another simple catalytic system reported to date for converting methane to a methyl product below 200 °C. Gold dissolved in 2% oleum catalyzes the selective, high yield oxidation of methane to methyl bisulfate using selenic acid as stoichiometric oxidant. -- Chapter Three discusses in details the mechanism of the most efficient and selective low-temperature catalytic system for the conversion of methane to methanol, comprised of a solution of the complex Pt(bpym)Cl2 (bpym=2-{2,2'-bipyrimidyl}) in concentrated sulfuric acid, investigated in direct reactions as well as in microscopic reverse reactions of model intermediates.; Chapter Four describe the discovety of highly effective 6-membered transition state for activation benzene in weak acids such as trifluoroacetic acid and other organic acids by Pt(bpym)TFA2. -- Chapter Five describes the discovery of new fast CH activation of benzene via conceptually proposed resting state destabilization phenomenon and experimentally supported by Pt(pic)TFA2 (pic - picolinate).; Chapter Six discribes the discovery of CH4 CH activation at conditions unprecedented before. Conceptual model for transition state stabilization is discussed and experimentally supported by Pt(nap)TFA2 (nap-2-(2-Pyridinyl)-1,8-naphthyridine). -- Chapter Seven summarizes the above results and makes attemptes to show future directions in CH activation. |
| Keyword | methane; CH activation; Shylov reaction |
| 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 |
| Type | texts |
| Legacy record ID | usctheses-m488 |
| Rights | Ziatdinov, Vadim Rinatovich |
| 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-Ziatdinov-20070517 |
| Archival file | uscthesesreloadpub_Volume32/etd-Ziatdinov-20070517.pdf |
Description
| Title | Page 1 |
| Full text | ACTIVATION OF METHANE BY HOMOGENEOUS CATALYSTS IN WEAKLY ACIDIC SOLVENTS by Vadim Rinatovich Ziatdinov A Dissertation Presented to the FACULTY OF THE GRADUATE SCHOOL UNIVERSITY OF SOUTHERN CALIFONIA In Partial Fulfillment of the Requirements for the Degree DOCTOR OF PHILOSOPHY (CHEMISTRY) May 2007 Copyright 2007 Vadim Rinatovich Ziatdinov |
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