Photoelectrochemical Homocoupling of Methane under Blue Light Irradiation

Abstract

Direct conversion of methane (CH4) into valuable chemicals with low-energy input is an important goal in the sustainable chemical industry. Herein, we report a photoelectrochemical activation of CH4 in the gas phase under visible light irradiation at room temperature. The proof-of-concept study revealed that homocoupling of CH4 to form ethane (C2H6) with high selectivity of 54% was induced by photogenerated holes over a tungsten trioxide (WO3) gas-diffusion photoanode coated with a proton-conducting ionomer in the presence of water vapor. The gas–electrolyte–solid triple-phase boundary enables the oxidation of the inert carbon–hydrogen bond of CH4, and the formation of carbon oxides and ethane with a carbon–carbon bond. The gas-phase photoelectrochemical system shows incident photon-to-current conversion efficiency of 11% under blue light at an applied voltage of 1.2 V. This work is also the first demonstration of a visible-light-driven hydrogen evolution from CH4. The hydrogen is separated from CH4 and oxidized products by a solid polymer electrolyte membrane.