2016年6月
Catalytic Oxidation of Methane into Methanol over Copper-Exchanged Zeolites with Oxygen at Low Temperature
ACS CENTRAL SCIENCE
- ,
- ,
- ,
- 巻
- 2
- 号
- 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
- ID情報
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- DOI : 10.1021/acscentsci.6b00139
- ISSN : 2374-7943
- eISSN : 2374-7951
- ORCIDのPut Code : 31154222
- Web of Science ID : WOS:000378690000012