Electrocatalytic oxidation of methane to low-carbon alcohol via stable Ni+/Ni0 interface

Direct oxidation of methane to high-value products under mild conditions is economic interest, but the slow transfer of electrons at the active site during the reaction affects the reaction kinetics significantly. Herein, a stabilized activation of Ni+/Ni0 interface by N2-cold plasma treatment was developed for enhancing Faradaic efficiency (FE) of Methane electrooxidation reaction (CH4OR) into low-carbon alcohol. The resultant Ni3N/Ni-plasma-10 exhibits a low-carbon alcohols (methanol and ethanol) FE of 88.5% at 1.7 V vs. RHE. The presence of Ni3N not only stabilizes Ni+/Ni0 interface but also benefits the stronger adsorption of *CH3 and *CH2OH to facilitate C-C coupling reaction. This presents a novel method for designing and preparing efficient, mild, and durable Ni-based electrocatalysts for CH4OR. Furthermore, the aforementioned findings are expected to contribute to the development of an advanced synthetic methodology for the facile synthesis of other transition metal nitride nanomaterials by N2-cold plasma treatment for various promising applications.