Electrocatalytic Conversion of CH4 to Oxygenates over Ni and Ce Doped LaCoO3 Perovskite in Aqueous Carbonate Electrolyte

In this study, an electrochemical system for methane conversion was developed, employing Ni- and Ce-doped LaCoO3 perovskite as the anode catalyst in an Na2CO3 electrolyte. Structural characterization revealed that the La1−yCeyCo1−xNixO3 (x = 0–0.5, y = 0–0.12) synthesized by the sol–gel method maintains the perovskite structure, but is rich in oxygen vacancies. Electrochemical studies revealed that the performance of methane activation is related to the presence of Ni(III) in the catalyst, and reactive oxygen species (•OH and HOO−) are provided through water oxidation reactions (WOR) in the Na2CO3 electrolyte. The electrocatalytic performance of the synthesized La0.92Ce0.08Co0.5Ni0.5O3 during methane conversion was verified in an electrolysis cell, and ethanol and acetic acid were identified as the methane conversion oxygenates. Under ambient conditions, the formation rate of ethanol reached 577.0 μmol gcat−1 h−1 at 0.90 V (vs. Ag/AgCl) in 0.5 mol L−1 Na2CO3. The catalyst was found to retain structural integrity and sustain catalytic activity over multiple reaction cycles.