545581 Electrochemical Oxidation of Methane to Olefins in HF/HSO3f

Monday, June 3, 2019: 11:03 AM
Texas Ballroom A (Grand Hyatt San Antonio)
Yuxin Fang1, Christopher G. Arges1, John C. Flake1 and Craig Plaisance2, (1)Cain Department of Chemical Engineering, Louisiana State University, Baton Rouge, LA, (2)Department of Chemical Engineering, Louisiana State University, Baton Rouge, LA

Advances in unconventional natural gas extraction have driven a renewed interest in the direct oxidation of methane to olefins. In 1968 Olah et al.1reported direct oxidation of methane using strong chemical oxidants in the presence superacids. The superacid is thought to facilitate the protonation activation of methane to trimethylcarbonium ion (methanium), however this reaction requires elevated temperatures (at 140 ᵒC). Later research by Jasinski et al.2reported electrochemical oxidation of propane and butane with Sb(V) in superacids; however, the electrochemical oxidation of methane and ethane yielded no measurable products.

In this work, we demonstrate the direct electrochemical oxidation of methane to olefins in super acid (HF/HSO3F) electrolytes. Linear sweep voltammetry experiments with acids of different acidity suggest only strong acids are capable of the activation of methane for oxidative coupling. Products include ethylene and a variety of liquid-phase olefins at relatively high Faradaic efficiencies. We will discuss the efficiency of the direct-electrochemical methane to olefins process and opportunities to selectively form high value olefins.

Reference:

  1. Olah, G. A.; Schlosberg, R. H., J. Am. Chem. Soc. 1968,90, 2726-2727.
  2. Brilmyer, G.; Jasinski, R., J. Electrochem. Soc. 1982,129, 1950-1954.

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