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Direct, nonoxidative conversion of methane to ethylene, aromatics, and hydrogen.

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... Full description

Journal Title: Science (New York N.Y.), May 9, 2014, Vol.344(6184), pp.616-619
Main Author: Guo, Xiaoguang
Other Authors: Fang, Guangzong , Li, Gang , Ma, Hao , Fan, Hongjun , Yu, Liang , Ma, Chao , Wu, Xing , Deng, Dehui , Wei, Mingming , Tan, Dali , Si, Rui , Zhang, Shuo , Li, Jianqi , Sun, Litao , Tang, Zichao , Pan, Xiulian , Bao, Xinhe
Format: Electronic Article Electronic Article
Language: English
Subjects:
ID: E-ISSN: 1095-9203 ; DOI: 1095-9203 ; DOI: 10.1126/science.1253150
Link: http://search.proquest.com/docview/1523404240/?pq-origsite=primo
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title: Direct, nonoxidative conversion of methane to ethylene, aromatics, and hydrogen.
format: Article
creator:
  • Guo, Xiaoguang
  • Fang, Guangzong
  • Li, Gang
  • Ma, Hao
  • Fan, Hongjun
  • Yu, Liang
  • Ma, Chao
  • Wu, Xing
  • Deng, Dehui
  • Wei, Mingming
  • Tan, Dali
  • Si, Rui
  • Zhang, Shuo
  • Li, Jianqi
  • Sun, Litao
  • Tang, Zichao
  • Pan, Xiulian
  • Bao, Xinhe
subjects:
  • Oxidative Stress
  • Methane
  • Hydrogen
  • Hydrocarbons
ispartof: Science (New York, N.Y.), May 9, 2014, Vol.344(6184), pp.616-619
description: 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. [PUBLICATION ] 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. [PUBLICATION ]
language: eng
source:
identifier: E-ISSN: 1095-9203 ; DOI: 1095-9203 ; DOI: 10.1126/science.1253150
fulltext: fulltext
issn:
  • 10959203
  • 1095-9203
url: Link


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titleDirect, nonoxidative conversion of methane to ethylene, aromatics, and hydrogen.
creatorGuo, Xiaoguang ; Fang, Guangzong ; Li, Gang ; Ma, Hao ; Fan, Hongjun ; Yu, Liang ; Ma, Chao ; Wu, Xing ; Deng, Dehui ; Wei, Mingming ; Tan, Dali ; Si, Rui ; Zhang, Shuo ; Li, Jianqi ; Sun, Litao ; Tang, Zichao ; Pan, Xiulian ; Bao, Xinhe
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descriptionDirect 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. [PUBLICATION ] 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. [PUBLICATION ]
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