論文

査読有り
2016年6月

Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature

ACS CENTRAL SCIENCE
  • Karthik Narsimhan
  • ,
  • Kenta Iyoki
  • ,
  • Kimberly Dinh
  • ,
  • Yuriy Roman-Leshkov

2
6
開始ページ
424
終了ページ
429
記述言語
英語
掲載種別
研究論文(学術雑誌)
DOI
10.1021/acscentsci.6b00139
出版者・発行元
AMER CHEMICAL SOC

The direct catalytic conversion of methane to liquid oxygenated compounds, such as methanol or dimethyl ether, at low temperature using molecular oxygen is a grand challenge in C-H activation that has never been met with synthetic, heterogeneous catalysts. We report the first demonstration of direct, catalytic oxidation of methane into methanol with molecular oxygen over copper-exchanged zeolites at low reaction temperatures (483-498 K). Reaction kinetics studies show sustained catalytic activity and high selectivity for a variety of commercially available zeolite topologies under mild conditions (e.g., 483 K and atmospheric pressure). Transient and steady state measurements with isotopically labeled molecules confirm catalytic turnover. The catalytic rates and apparent activation energies are affected by the zeolite topology, with caged-based zeolites (e.g., Cu-SSZ-13) showing the highest rates. Although the reaction rates are low, the discovery of catalytic sites in copper-exchanged zeolites will accelerate the development of strategies to directly oxidize methane into methanol under mild conditions.


リンク情報
DOI
https://doi.org/10.1021/acscentsci.6b00139
Web of Science
https://gateway.webofknowledge.com/gateway/Gateway.cgi?GWVersion=2&SrcAuth=JSTA_CEL&SrcApp=J_Gate_JST&DestLinkType=FullRecord&KeyUT=WOS:000378690000012&DestApp=WOS_CPL
URL
http://orcid.org/0000-0002-1111-7111
ID情報
  • DOI : 10.1021/acscentsci.6b00139
  • ISSN : 2374-7943
  • eISSN : 2374-7951
  • ORCIDのPut Code : 31154222
  • Web of Science ID : WOS:000378690000012

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