期刊
SCIENCE
卷 344, 期 6184, 页码 616-619出版社
AMER ASSOC ADVANCEMENT SCIENCE
DOI: 10.1126/science.1253150
关键词
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资金
- Strategic Priority Research Program of the Chinese Academy of Sciences [XDA09030101]
- National Natural Science Foundation of China [21321002, 11079005, 21033009, 21103181]
- Ministry of Science and Technology of China [2011CBA00503, 2013CB933100]
The efficient use of natural gas will require catalysts that can activate the first C-H bond of methane while suppressing complete dehydrogenation and avoiding overoxidation. We report that single iron sites embedded in a silica matrix enable direct, nonoxidative conversion of methane, exclusively to ethylene and aromatics. The reaction is initiated by catalytic generation of methyl radicals, followed by a series of gas-phase reactions. The absence of adjacent iron sites prevents catalytic C-C coupling, further oligomerization, and hence, coke deposition. At 1363 kelvin, methane conversion reached a maximum at 48.1% and ethylene selectivity peaked at 48.4%, whereas the total hydrocarbon selectivity exceeded 99%, representing an atom-economical transformation process of methane. The lattice-confined single iron sites delivered stable performance, with no deactivation observed during a 60-hour test.
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