2011 Fiscal Year Final Research Report
Construction of highly efficient and highly selective catalytic oxidation systems based on proton-coupled electron transfer
| Project/Area Number |
21350035
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| Research Category |
Grant-in-Aid for Scientific Research (B)
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| Allocation Type | Single-year Grants |
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| Section | 一般 |
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| Research Field |
Inorganic chemistry
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| Research Institution | University of Tsukuba |
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Principal Investigator |
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| Project Period (FY) |
2009 – 2011
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| Keywords | ルテニウム錯体 / 高原子価オキソ錯体 / プロトン共役電子移動 / 環境/エネルギー / 外部基質酸化触媒系 |
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| Research Abstract |
We have established highly efficient and highly selective catalytic oxidation systems for organic substrates using Ru(II)-pyridylamine-aqua complexes as catalysts in aqueous buffer solutions. In those reactions, Ru(IV)-oxo complexes were formed via proton-coupled electron transfer and their characterization were made by spectroscopic and crystallographic methods and DFT calculations. In this research, we have clarified that the spin states of Ru(IV)-oxo complexes do not affect their reactivity. We have also succeeded in the direct observation of the oxygen-rebound mechanism in C-H hydroxylation for the first time and elucidated the reaction mechanism of C-H oxidation in the light of kinetic analysis.
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