Direct partial oxidation of methane to liquid oxygenates has been regarded as a potential route to valorize methane. However, CH₄ activation usually requires a high temperature and pressure, which lowers the feasibility of the reaction. Here, we propose an electro-assisted approach for the partial oxidation of methane, using in-situ cathodically generated reactive oxygen species, at ambient temperature and pressure. Upon using acid-treated carbon as the electrocatalyst, the electro-assisted system enables the partial oxidation of methane in an acidic electrolyte to produce oxygenated liquid products. We also demonstrate a high production rate of oxygenates (18.9 μmol h⁻¹) with selective HCOOH production. Mechanistic analysis reveals that reactive oxygen species such as ∙OH and ∙OOH radicals are produced and activate CH₄ and CH₃OH. In addition, unstable CH₃OOH generated from methane partial oxidation can be additionally reduced to CH₃OH on the cathode, and so-produced CH₃OH is further oxidized to HCOOH, allowing selective methane partial oxidation.

甲烷直接部分氧化为液态含氧化合物被认为是甲烷增值的潜在途径。然而，CH ₄活化通常需要高温和高压，这降低了反应的可行性。在这里，我们提出了一种在环境温度和压力下使用原位阴极产生的活性氧来部分氧化甲烷的电辅助方法。使用酸处理的碳作为电催化剂后，电辅助系统能够在酸性电解质中部分氧化甲烷，产生含氧液体产物。我们还证明了含氧化合物的高生产率（18.9 μmol h ^-1）和选择性 HCOOH 的产生。机理分析表明，会产生诸如∙OH和∙OOH自由基等活性氧，并激活CH ₄和CH ₃ OH。此外，由甲烷部分氧化产生的不稳定的CH ₃ OOH可以在阴极上另外被还原为CH ₃ OH，并且如此产生的CH ₃ OH被进一步氧化为HCOOH，从而允许选择性甲烷部分氧化。