Identifier

etd-10012012-125615

Degree

Master of Science in Chemical Engineering (MSChE)

Department

Chemical Engineering

Document Type

Thesis

Abstract

A novel technology, a pulsed oscillating monolith reactor (POMR), was compared to a standard autoclave reactor for oxidative desulfurization (ODS) of a model diesel fuel. Two classes of catalysts, mesoporous Ti-MCM-41 and Pd on carbon, were used for ODS. The oxidants used were O2 and peroxide. The model diesel compound was 75 wt% alkanes, 24 wt% alkylaromatic, 0.95 wt% sulfur heterocycles and 0.05% nitrogen heterocycles. ODS reactions were conducted from 343-423 K and pressures from 1.0-1.3 MPa O2. The only component that was not oxidized was the alkane. The POMR showed promise; there was up to a factor of 20 enhancement in turnover frequency for alkylaromatics, up to a factor of 9 for sulfur heterocycles and up to 20 for nitrogen heterocycles. However, the POMR was no more selective and in some cases less selective when compared to runs performed in an autoclave. It was determined that the Ti-MCM-41 has a higher initial catalytic activity then supported Pd, but it deactivates more quickly due to the condensation of products on the surface and in the pores. It additionally had a higher selectivity than the carbon-supported Pd. The Ti-MCM-41 catalyst specifically did a better job of oxidizing dibenzothiophene, which is one of the most refractory sulfur compounds. There was no significant improvement from the substitution of benzoyl peroxide for O2 as oxidant. Neither the sulfur compound turnover frequencies nor the overall dibenzothiophene conversion were improved, when roughly equal amounts of oxidant were provided.

Date

2012

Document Availability at the Time of Submission

Secure the entire work for patent and/or proprietary purposes for a period of one year. Student has submitted appropriate documentation which states: During this period the copyright owner also agrees not to exercise her/his ownership rights, including public use in works, without prior authorization from LSU. At the end of the one year period, either we or LSU may request an automatic extension for one additional year. At the end of the one year secure period (or its extension, if such is requested), the work will be released for access worldwide.

Committee Chair

Kerry M Dooley

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