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Naphtha is a promising fuel candidate for fuel cell vehicles. However, naphtha contains significant amounts of organosulfur compounds such as thiols, sulfides, disulfides, thiophenes and benzothiophenes, and these sulfur compounds poison the catalysts in fuel processors and fuel cells. Ultra-deep removal of sulfur from naphtha is very important for fuel cell applications and the sulfur content should be reduced to below 0.1 mass ppm1). Organosulfur compounds in petroleumderived fuels are usually removed by hydrodesulfurization (HDS), but the HDS process cannot economically produce fuel with this low sulfur level. Accordingly, alternative methods such as oxidative desulfurization (ODS), adsorptive desulfurization, biodesulfurization, etc. have been developed2),3). ODS has several advantages compared to HDS: operation at near ambient temperatures and pressures, no use of hydrogen, and superior treatment of sterically hindered thiophenic compounds. Various oxidants such as formic acidH2O24),5), H2O2Ti-containing molecular sieves6), H2O2titanium silicate7), t-BuOOHMo/Al2O38), H2O2phosphotungstic acid-phase transfer catalyst-ultrasonication9), and O2Co catalyst-aldehyde10) were recently used in oxidative processes. Thiophenes are the major organosulfur compounds in naphtha, but little is known about the oxidation of thiophenes in the ODS process. The reactivities of thiophenes are lower than those of benzothiophenes and dibenzothiophenes6). Moreover, thiophenes are not oxidized with formic acid and H2O2 at 323 K4). Consequently, a method needs to be developed for the effective oxidation of thiophenes in naphtha. We previously demonstrated that dibenzothiophenes were smoothly oxidized with H2O2 in the presence of 12-tungstophosphoric acid (TPA) in an organic biphasic system, and that the sulfur content of a diesel oil was effi ciently reduced11),12). This oxidative treatment can effectively oxidize thiophenes as well. Here we report the TPA-catalyzed oxidation of organosulfur compounds with H2O2, in both acetic acid (AcOH) and organic biphasic systems. This oxidative process effi ciently reduced the sulfur content of naphtha. The effect of HDS of naphtha on the outcome of ODS was also examined.

Tungstophosphoric Acid-catalyzed Oxidative Desulfurization of Naphtha with Hydrogen Peroxide in Naphtha/Acetic Acid Biphasic System