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このアイテムの引用には次の識別子を使用してください:
http://hdl.handle.net/10119/18870
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| タイトル: | Catalytic Oxidation of Methane to Methanol over Cu-CHA with Molecular Oxygen |
| 著者: | Hirayama, Airi
Tsuchimura, Yuka
Yoshida, Hiroshi
Machida, Masato
Nishimura, Shun
Kato, Kazuo
Takahashi, Keisuke
Ohyama, Junya |
| 発行日: | 2021-07-20 |
| 出版者: | Royal Society of Chemistry |
| 誌名: | Catalysis Science & Technology |
| 巻: | 11 |
| 号: | 18 |
| 開始ページ: | 6217 |
| 終了ページ: | 6224 |
| DOI: | 10.1039/D1CY00676B |
| 抄録: | Direct oxidation of CH4 to CH3OH using O2 is challenging because of the high stability of CH4 and the relatively high reactivity of CH3OH. Here, Cu-CHA zeolites are tested for direct oxidation of CH4. Catalytic production of CH3OH in a CH4-O2-H2O flow reaction is improved using CHA type zeolites compared to other zeolites including MOR, BEA, MFI, and FAU zeolites reported previously. In situ X-ray absorption fine structure (XAFS) spectroscopy reveals that high catalytic activity of Cu-CHA is derived from its redox property, particularly, the high reducibility of Cu2+ involved in CH4 activation. The reaction gas concentrations are varied to find optimized reaction conditions on Cu-CHA. In addition, the reaction mechanism of the direct CH4 oxidation on a Cu-CHA is investigated based on not only the effects of gas concentrations but also the isotope gas effects using CD4, 18O2, and D2O. It is suggested that the rate-determining step is C-H activation of CH4, and the selectivity of CH3OH is determined by oxidation rate of CH3OH, which is affected by O2 and OH groups activation rate on Cu-CHA. |
| Rights: | Copyright (C) 2021 Royal Society of Chemistry. Airi Hirayama, Yuka Tsuchimura, Hiroshi Yoshida, Masato Machida, Shun Nishimura, Kazuo Kato, Keisuke Takahashi and Junya Ohyama, Catalysis Science & Technology, 2021, 11(18), 6217-6224. https://doi.org/10.1039/D1CY00676B - Reproduced by permission of the Royal Society of Chemistry |
| URI: | http://hdl.handle.net/10119/18870 |
| 資料タイプ: | author |
| 出現コレクション: | d10-1. 雑誌掲載論文 (Journal Articles)
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