Theoretical and Experimental Studies on Reaction Mechanism for Aerobic Alcohol Oxidation by Supported Ruthenium Hydroxide Catalysts
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- Fumiya Nikaidou
- Department of Chemical System Engineering and Department of Applied Chemistry, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan
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- Hiroshi Ushiyama
- Department of Chemical System Engineering and Department of Applied Chemistry, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan
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- Kazuya Yamaguchi
- Department of Chemical System Engineering and Department of Applied Chemistry, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan
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- Koichi Yamashita
- Department of Chemical System Engineering and Department of Applied Chemistry, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan
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- Noritaka Mizuno
- Department of Chemical System Engineering and Department of Applied Chemistry, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan
書誌事項
- 公開日
- 2010-06-01
- 資源種別
- journal article
- DOI
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- 10.1021/jp101692j
- 公開者
- American Chemical Society (ACS)
この論文をさがす
説明
The experimentally proposed reaction mechanism for the aerobic alcohol oxidation by supported ruthenium hydroxide catalysts (Ru(OH)x/support, support = TiO2 or Al2O3) is theoretically investigated by means of ab initio quantum chemistry calculations with model catalysts “Ru(OH)3(OH2)3” and “RuCl3(OH2)3” for Ru(OH)x/support and RuClx/support, respectively. The experimentally proposed alcoholate formation and β-hydride elimination steps can be verified. In the case of 2-butanol (as a model substrate), the calculated activation energy for the alcoholate formation step with Ru(OH)3(OH2)3 (27.7 kJ mol−1) is much smaller than that with RuCl3(OH2)3 (123.2 kJ mol−1), showing that the alcoholate formation with Ru(OH)x/support much more easily proceeds than that with RuClx/support. The Ru(OH)x/support catalysts possess both Lewis acid (Ru center) and Bronsted base (OH− species) sites on the same metal site. Therefore, the alcoholate formation step can be promoted by the “concerted activation” of an alcohol by the L...
収録刊行物
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- The Journal of Physical Chemistry C
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The Journal of Physical Chemistry C 114 (24), 10873-10880, 2010-06-01
American Chemical Society (ACS)
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詳細情報 詳細情報について
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- CRID
- 1360004233233911552
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- ISSN
- 19327455
- 19327447
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- 資料種別
- journal article
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- データソース種別
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- Crossref
- KAKEN
- OpenAIRE
