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

Xiaoguang Guo(Dalian Institute of Chemical Physics), Guangzong Fang(Dalian Institute of Chemical Physics), Gang Li(Dalian Institute of Chemical Physics), Hao Ma(Dalian Institute of Chemical Physics), Hongjun Fan(Dalian Institute of Chemical Physics), Liang Yu(Dalian Institute of Chemical Physics), Chao Ma(Chinese Academy of Sciences), Xing‐Long Wu(Southeast University), Dehui Deng(Dalian Institute of Chemical Physics), Mingming Wei(Dalian Institute of Chemical Physics), Dali Tan(Dalian Institute of Chemical Physics), Rui Si(Chinese Academy of Sciences), Shuo Zhang(Chinese Academy of Sciences), Jianqi Li(Chinese Academy of Sciences), Litao Sun(Southeast University), Zichao Tang(Dalian Institute of Chemical Physics), Xiulian Pan(Dalian Institute of Chemical Physics), Xinhe Bao(Dalian Institute of Chemical Physics)
Science
May 8, 2014
Cited by 1,391

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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