Selective monooxidation of light alkanes using chloride and iodate

George C. Fortman, Nicholas C. Boaz, Dominik Munz, Michael M. Konnick, Roy A. Periana, John Taylor Groves, T. Brent Gunnoe

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31 Scopus citations

Abstract

We describe an efficient system for the direct partial oxidation of methane, ethane, and propane using iodate salts with catalytic amounts of chloride in protic solvents. In HTFA (TFA = trifluoroacetate), >20% methane conversion with >85% selectivity for MeTFA have been achieved. The addition of substoichiometric amounts of chloride is essential, and for methane the conversion increases from <1% in the absence of chloride to >20%. The reaction also proceeds in aqueous HTFA as well as acetic acid to afford methyl acetate. 13C labeling experiments showed that less than 2% of methane is overoxidized to 13CO2 at 15% conversion of 13CH4. The system is selective for higher alkanes: 30% ethane conversion with 98% selectivity for EtTFA and 19% propane conversion that is selective for mixtures of the mono- and difunctionalized TFA esters. Studies of methane conversion using a series of iodine-based reagents [I2, ICl, ICl3, I(TFA)3, I2O4, I 2O5, (IO2)2S2O 7, (IO)2SO4] indicated that the chloride enhancement is not limited to iodate.

Original languageEnglish (US)
Pages (from-to)8393-8401
Number of pages9
JournalJournal of the American Chemical Society
Volume136
Issue number23
DOIs
StatePublished - Jun 11 2014

All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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    Fortman, G. C., Boaz, N. C., Munz, D., Konnick, M. M., Periana, R. A., Groves, J. T., & Brent Gunnoe, T. (2014). Selective monooxidation of light alkanes using chloride and iodate. Journal of the American Chemical Society, 136(23), 8393-8401. https://doi.org/10.1021/ja502657g