Title page for ETD etd-06032010-071804


Type of Document Major Paper
Author Liu, Dongxing
Author's Email Address dliu11@lsu.edu, liudongxing@gmail.com
URN etd-06032010-071804
Title Catalytic Oxidative Desulfurization of a Model Diesel
Degree Master of Science in Chemical Engineering (M.S.Ch.E.)
Department Chemical Engineering
Advisory Committee
Advisor Name Title
Dooley, Kerry M. Committee Chair
Knopf, F. Carl Committee Co-Chair
Pike, Ralph W. Committee Member
Keywords
  • N-heterocycles oxdiation with oxygen
  • S-heterocycles oxidation with oxygen
Date of Defense 2010-05-07
Availability unrestricted
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.

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