The direct oxidation of methane to more desirable, one-carbon oxygenated molecules such as methanol and formaldehyde offers a pathway towards a more sustainable chemical industry as the current commercial reforming process involving two steps features a high carbon footprint and energy consumption. Here, we report the selective photocatalytic oxidation of methane at room temperature using quantum-sized bismuth vanadate nanoparticles as the catalyst and oxygen as a mild oxidant. The reaction offers a high selectivity, of 96.6% for methanol or 86.7% for formaldehyde, under optimum wavelength and intensity of light, reaction time and amount of water solvent. Comprehensive characterizations disclose a multistep reaction mechanism in which the activation of methane by the hydroxyl radical determines the reaction rate. This work broadens the avenue towards the selective conversion of the greenhouse gas methane into desirable chemical products in a sustainable way.

将甲烷直接氧化为更理想的一碳氧化分子（例如甲醇和甲醛）可为实现更可持续的化学工业提供一条途径，因为当前涉及两个步骤的商业重整过程具有很高的碳足迹和能耗。在这里，我们报告在室温下使用量子尺寸的钒酸铋纳米粒子作为催化剂，使用氧气作为弱氧化剂，对甲烷进行选择性光催化氧化。在最佳的波长和光强度，反应时间和水溶剂的量下，该反应具有很高的选择性，对于甲醇为96.6％，对于甲醛为86.7％。综合表征公开了多步反应机理，其中羟基自由基对甲烷的活化决定了反应速率。