Abstract

Electrocatalytic oxidation of methane (CH4) to value-added chemicals under mild conditions derived by renewable electricity is an attractive approach to directly use natural gas as a hydrocarbon feedstock. Herein, we report a novel composite electrode constructed by uniformly dispersing hydrophobic polytetrafluoroethylene (PTFE) polymer on the surface of Ni(OH)2 nanosheets catalyst for selective electrooxidation of CH4 to methanol (CH3OH) and ethanol (CH3CH2OH). This hydrophobic composite electrode can establish a directional transport channel for CH4 and effectively enhance the enrichment of CH4 on the electrode surface, forming a rich solid-liquid-gas three-phase reaction interface. The optimized 6 %PTFE-Ni(OH)2 electrode can achieve the highest alcohols’ Faradaic efficiency (FE) of 75.8 %, which is 21 times higher than that of the hydrophilic Ni(OH)2/NF electrode, and the highest concentration of alcohols can reach 9.00 mM. In addition, mechanistic analysis reveals that Ni(OH)2 is oxidized to NiOOH, which can oxidizes water to *OH, and then *OH activates and oxidizes CH4 to *CH3 and CH3OH. In addition, the formation mechanism of CH3CH2OH is only formed by coupling *OCH3 with CH4 activated on the catalyst surface. This work provides a feasible approach to tailor the hydrophilicity of catalyst to improve the efficiency of CH4 oxidation.

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