甲烷
催化作用
化学
氧气
部分氧化
电子转移
化学工程
甲烷厌氧氧化
光化学
有机化学
工程类
作者
Taikang Jia,Wenjing Wang,Chuanqi Zhang,Ling Zhang,Wenzhong Wang
标识
DOI:10.1002/anie.202413343
摘要
The direct conversion and efficient utilization of methane pose a critical scientific challenge. Indirect activation via reactive oxygen species (ROS) offers a high probability of contact with methane and conversion efficiency under mild conditions. However, reported product yields are suboptimal due to challenges in activating oxygen and facilitating mass transfer in suspension systems. We propose the use of contact‐electro‐catalysis (CEC), employing polydopamine (PDA) as a catalyst that undergoes electron transfer with oxygen under ultrasound, generating ROS that drives the partial oxidation of methane (POM). Corresponding experimental results indicate that CH3OH and most HCHO are produced directly from CH4. Furthermore, through in situ characterizations, we have shown that light pretreatment of the catalysts in an oxygenated atmosphere facilitates the forming of more C=O functional groups with strong electron‐withdrawing properties, thereby significantly enhancing overall product yields, particularly for CH3OH. Within two hours, product yields reach 1.5 mmol·gcat−1 for HCHO and 0.9 mmol·gcat−1 for CH3OH. This work introduces a novel approach for efficient POM, while highlighting the distinctive catalytic properties of PDA.
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