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Direct, Nonoxidative Conversion of Methane to Ethylene, Aromatics, and Hydrogen

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Science  09 May 2014:
Vol. 344, Issue 6184, pp. 616-619
DOI: 10.1126/science.1253150

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Upgrading Methane Sans Oxygen

Direct routes to converting methane to higher hydrocarbons can allow natural gas to be used to provide chemical feedstocks. However, the reaction conditions needed to activate the strong C-H bond tend to overoxidize the products. Guo et al. (p. 616) report a high-temperature nonoxidative route that exposes methane to isolated iron sites on a silica catalyst. Methyl radicals were generated and coupled in the gas phase to form ethylene and aromatics along with hydrogen. The isolation of the active sites avoided surface reactions between the radicals that would deposit solid carbon.

Abstract

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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