Studies Towards the Development of New Catalysts for Methane Conversion

Author: Main, Rebekah Mary

Year: 2002

Degree: Master's thesis

Advisors: Davis, Mark E.; Bercaw, John E.

Committee Member: Unknown, Unknown

Option: Chemistry

DOI: 10.7907/xxcm-zd60

Abstract

In efforts to develop new catalysts for the partial oxidation of methane to methanol, studies were focused on developing supported aqueous phase (SAP) catalysts for this chemistry. The work can be separated into two main projects. First, steps were taken to prepare an organometallic SAP catalyst. A water-soluble sulfonated Pt diimine species has been prepared and supported on controlled-pore glass. The compound was characterized by solid state 13C CP-MAS NMR, and observations were made on the compounds behavior. This work is carried out in collaboration with research into homogeneous organometallic catalysts, and progress in this area is dependent on the development of successful homogeneous catalysts. The second project involves using platinum/copper salt catalyst for the hydroxylation of alkanes, where dioxygen is the ultimate oxidant. Several homogeneous reactions were carried out to investigate the reactivity of this catalyst system in solution. The catalysts were found to successfully hydroxylate sulfonated alkanes as well as ethane and methane, all with multiple platinum turnovers. Product characterizations were carried out using 1H NMR and GC/MS. Efforts were also begun to develop a SAP catalyst with the Pt/Cu system, modeled after the SAP Pd/Cu Wacker oxidation catalyst.

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