ADVANCED OXIDATION PROCESS

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The design of new, high efficiency and cleaner burning engines is strongly coupled with the removal of recalcitrant sulfur species, dibenzothiophene and its derivatives, from fuels. Oxidative desulfurization (ODS) wherein these dibenzothiophene derivatives are oxidized to their corresponding sulfoxides and sulfones is an approach that has gained significant attention. Fe-TAML{reg_sign} activators of hydrogen peroxide (TAML is Tetra-Amido-Macrocyclic-Ligand) convert in a catalytic process dibenzothiophene and its derivatives to the corresponding sulfoxides and sulfones rapidly at moderate temperatures (60 C) and ambient pressure. The reaction can be performed in both an aqueous system containing an alcohol (methanol, ethanol, or t-butanol) to solubilize ... continued below

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10 pages

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Horwitz, Colin P. & Collins, Terrence J. October 22, 2003.

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Description

The design of new, high efficiency and cleaner burning engines is strongly coupled with the removal of recalcitrant sulfur species, dibenzothiophene and its derivatives, from fuels. Oxidative desulfurization (ODS) wherein these dibenzothiophene derivatives are oxidized to their corresponding sulfoxides and sulfones is an approach that has gained significant attention. Fe-TAML{reg_sign} activators of hydrogen peroxide (TAML is Tetra-Amido-Macrocyclic-Ligand) convert in a catalytic process dibenzothiophene and its derivatives to the corresponding sulfoxides and sulfones rapidly at moderate temperatures (60 C) and ambient pressure. The reaction can be performed in both an aqueous system containing an alcohol (methanol, ethanol, or t-butanol) to solubilize the DBT and in a two-phase hydrocarbon/aqueous system where the alcohol is present in both phases and facilitates the oxidation. Under a consistent set of conditions using the FeBF{sub 2} TAML activator, the degree of conversion was found to be t-butanol > methanol > ethanol. In the cases of methanol and ethanol, both the sulfoxide and sulfone were observed while for t-butanol only the sulfone was detected. In the two-phase system, the alcohol may function as an inverse phase transfer agent. The oxidation was carried out using two different TAML activators. In homogeneous solution, approximately 90% oxidation of the DBT could be achieved using the prototype TAML activator, FeB*, by sonicating the solution at near room temperature. In bi-phasic systems conversions as high as 50% were achieved using the FeB* TAML activator and hydrogen peroxide at 100 C. The sonication method yielded only {approx}6% conversion but this may have been due to mixing.

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10 pages

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OSTI as DE00824769

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  • Other Information: PBD: 22 Oct 2003

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  • Report No.: NONE
  • Grant Number: FC26-02NT41625
  • DOI: 10.2172/824769 | External Link
  • Office of Scientific & Technical Information Report Number: 824769
  • Archival Resource Key: ark:/67531/metadc781795

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Creation Date

  • October 22, 2003

Added to The UNT Digital Library

  • Dec. 3, 2015, 9:30 a.m.

Description Last Updated

  • Jan. 17, 2018, 4:37 p.m.

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Horwitz, Colin P. & Collins, Terrence J. ADVANCED OXIDATION PROCESS, report, October 22, 2003; [Pittsburgh, Pennsylvania]. (digital.library.unt.edu/ark:/67531/metadc781795/: accessed October 21, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.