Electrochemical Methane Activation and Conversion to Oxygenates at Room Temperature

Abstract

Methane was electrochemically activated at room temperature to oxygenates using CO3 2- as an oxygen-donating species over a NiO-ZrO2 bifunctional electrocatalyst. Products identified from this activation using Mass Spectrometry and 1H-Nuclear Magnetic Resonance Spectroscopy include CH3OH, HCHO, CO, HCOO-, C2H5OH, H3CCOO-, C3H8O, and C3H6O. In addition, O2 and OHOH CO2 were also observed as products resulting from carbonate electrolysis and/or the oxygen evolution reaction. Methane was adsorbed and activated by NiO while CO3 2- was adsorbed onto non-conducting ZrO2. Oxygen was then abstracted and donated from CO3 2- to electrocatalytically active sites to form new C-O or O-H bonds. Two- and three-carbon species were formed via a C=O bond resonance mechanism which facilitated new C-C bond formation.