甲烷
甲烷厌氧氧化
激进的
光化学
催化作用
电子顺磁共振
密度泛函理论
氧气
乙烯
化学工程
化学
计算化学
工程类
有机化学
物理
核磁共振
作者
Weixin Li,Sun Hee Jun,Mingda Wang,Jiajia Xu,Yanjie Wang,Yahui Li,Yan Ran,Hao He,Shuai Wang,Wei Deng,Zhong‐Qun Tian,Feng Ru Fan
标识
DOI:10.1002/anie.202403114
摘要
The conversion of methane under ambient conditions has attracted significant attention. Although advancements have been made using active oxygen species from photo- and electro- chemical processes, challenges such as complex catalyst design, costly oxidants, and unwanted byproducts remain. This study exploits the concept of contact-electro-catalysis, initiating chemical reactions through charge exchange at a solid-liquid interface, to report a novel process for directly converting methane under ambient conditions. Utilizing the electrification of commercially available Fluorinated Ethylene Propylene (FEP) with water under ultrasound, we demonstrate how this interaction promote the activation of methane and oxygen molecules. Our results show that the yield of HCHO and CH3OH can reach 467.5 and 151.2 μmol ⋅ gcat-1, respectively. We utilized electron paramagnetic resonance (EPR) to confirm the evolution of hydroxyl radicals (⋅OH) and superoxide radicals (⋅OOH). Isotope mass spectrometry (MS) was employed to analyze the elemental origin of CH3OH, which can be further oxidized to HCHO. Additionally, we conducted density functional theory (DFT) simulations to assess the reaction energies of FEP with H2O, O2, and CH4 under these conditions. The implications of this methodology, with its potential applicability to a wider array of gas-phase catalytic reactions, underscore a significant advance in catalysis.
科研通智能强力驱动
Strongly Powered by AbleSci AI