Electrochemical Oxidation of Methane to Methylamine

作者：Qiang Song, Wanping Xu, Xin Zeng, Tianqi Zhang, Jungmi Hong, Patrick J. Cullen · 发表于：Journal of the American Chemical Society · 年份：2025 · DOI：10.1021/jacs.5c04802 · 被引用次数：16 · 研究领域：Catalysis and Oxidation Reactions、CO2 Reduction Techniques and Catalysts、Catalytic Processes in Materials Science

The electrochemical methane (CH 4 ) oxidation reaction under ambient conditions is a promising approach for natural gas utilization. However, the highly stable nature of CH 4 restrains efficient cleavage of the C–H bond without overoxidation. To this end, we proposed a coupled oxidative strategy for converting CH 4 to value-added products via NH 2 intermediates. The ammonia-oxidation-driven anodic reaction facilitates the formation of NH 2 species and activates CH 4 through nucleophilic attack to achieve C–N bond formation. Further the generated methylamine could be protected from overoxidation in the ammonia-based anolyte. Under such conditions, a methylamine productivity of 3.8 mmol g –1 cat h –1 at 1.55 V vs a reversible hydrogen electrode is reported. This work provides new insights into electrocatalytic C–N coupling based on the ammonia oxidation reaction, which could extend to other alkane or alkene conversions.