甲烷
沸石
甲醇
甲烷厌氧氧化
催化作用
无机化学
解吸
红外光谱学
化学
铜
部分氧化
氢
氧气
物理化学
有机化学
吸附
作者
Vitaly L. Sushkevich,Dennis Palagin,Marco Ranocchiari,Jeroen A. van Bokhoven
出处
期刊:Science
[American Association for the Advancement of Science]
日期:2017-05-04
卷期号:356 (6337): 523-527
被引量:779
标识
DOI:10.1126/science.aam9035
摘要
Direct functionalization of methane in natural gas remains a key challenge. We present a direct stepwise method for converting methane into methanol with high selectivity (~97%) over a copper-containing zeolite, based on partial oxidation with water. The activation in helium at 673 kelvin (K), followed by consecutive catalyst exposures to 7 bars of methane and then water at 473 K, consistently produced 0.204 mole of CH3OH per mole of copper in zeolite. Isotopic labeling confirmed water as the source of oxygen to regenerate the zeolite active centers and renders methanol desorption energetically favorable. On the basis of in situ x-ray absorption spectroscopy, infrared spectroscopy, and density functional theory calculations, we propose a mechanism involving methane oxidation at CuII oxide active centers, followed by CuI reoxidation by water with concurrent formation of hydrogen.
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