Identifier

etd-06032010-071804

Degree

Master of Science in Chemical Engineering (MSChE)

Department

Chemical Engineering

Document Type

Major Paper

Abstract

An analysis of heterogeneous oxidation catalysts was performed to determine the activities and optimal operating conditions for the multiphase oxidative desulfurization (ODS) reactions, using a model diesel. Catalysts studied included well-characterized Pd on Al2O3 and activated carbon supports, and carbon-supported Mo2C and W2C, which were prepared by temperature programmed reaction. Several other typical oxidation catalysts were also examined. The model diesel consisted of ~1 wt% sulfur compounds (thiophene and dibenzothiophene) with appropriate amounts of aliphatic, alkylaromatic and N-heterocyclic compounds to simulate a raw number 2 diesel. With oxygen as the oxidant in ODS reactions of this model diesel (70-90ºC, 0.8-1.8 MPa, feed vol/wt cat. = 100 mL/g), Pd/C and Mo2C/C showed the best selectivity for oxidizing the N- and S-heterocycles vs. the alkylaromatics. Increasing the pressure increased the reaction rates of the N- and S-heterocycles. Except for thiophene, there was only a small dependence of observed rates on temperature, which suggests the reactions were partially diffusion (of O2) controlled. The optimal ODS catalysts (carbides and 5%Pd/MPT-5) also showed high activity for the conversion of N-heterocycles. Current work includes further investigations of the better catalysts, full characterization of the products by GC-MS, and kinetics measurements using catalyst monoliths in a pistonoscillating reactor, which can eliminate the diffusion limitations and provide a uniform hydrodynamic environment.

Date

2010

Document Availability at the Time of Submission

Release the entire work immediately for access worldwide.

Committee Chair

Dooley, Kerry M.

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