Precise Control of Dioxygen Activation by Copper Complexes and Application
| Project/Area Number |
17H03031
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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 | Osaka University |
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Principal Investigator |
Itoh Shinobu 大阪大学, 工学研究科, 教授 (30184659)
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| Project Period (FY) |
2017-04-01 – 2020-03-31
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| Project Status |
Completed (Fiscal Year 2020)
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| Budget Amount *help |
¥18,850,000 (Direct Cost: ¥14,500,000、Indirect Cost: ¥4,350,000)
Fiscal Year 2019: ¥4,550,000 (Direct Cost: ¥3,500,000、Indirect Cost: ¥1,050,000)
Fiscal Year 2018: ¥4,940,000 (Direct Cost: ¥3,800,000、Indirect Cost: ¥1,140,000)
Fiscal Year 2017: ¥9,360,000 (Direct Cost: ¥7,200,000、Indirect Cost: ¥2,160,000)
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| Keywords | 銅錯体 / 酸素の活性化 / 活性酸素錯体 / 酸化反応 / 反応性制御 / 反応機構 / 多座配位子 / 反応制御 / アルカンの触媒的酸化 / 炭化水素の酸化 / 分子状酸素の活性化 / 構造制御 |
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| Outline of Final Research Achievements |
In this study, we have investigated copper-oxygen chemistry systematically by using a variety of supporting ligands in order to accompulish 'precise controlling of dioxygen activation by copper complexes'. The results obtained in this research are as follows.
(1) The reaction control mechanism of copper-oxygen complexes have been elucidated by using an N3- tridentate ligands and N4-tetradentate ligands having a cyclic diamine skeleton. (2) Novel copper complexes having a tetrahedral geometry have been synthesized using a newly designed N3-tridentate ligand and their structure, physiochemical properties, and reactivity have been evaluated to get deeper insights into the role of ligand structures. (3) The structural control mechanism of a copper-active oxygen complex was clarified by employing a tripod-type tetradentate ligand with a bulky substituents. (4) We achieved the ligand design aiming at the creation of a novel mononuclear copper active centers of the copper monooxygenases.
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| Academic Significance and Societal Importance of the Research Achievements |
銅錯体による酸素の活性化は、銅含有酸化酵素や、銅を触媒とする様々な有機合成反応における重要なプロセスであり、錯体化学、生物無機化学、触媒化学、有機合成化学などの広い分野で活発に研究が展開されてきた。各銅－活性酸素錯体の構造、物理化学的特性、反応性などについては生物無機化学や錯体化学の分野で活発に検討が加えられてきたが、それらの生成制御機構に関しては系統的な検討が殆ど成されてきておらず、不明な点が多く残されている。本研究では、様々な配位子を用いて銅－活性酸素錯体の生成機構の解明や反応性の制御を達成するものであり、酵素機能の解明や新しい酸化触媒の開発に繋がるものとしてその意義は大きい。
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Report
(4 results)
Research Products
(38 results)
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[Journal Article] Tetrahedral Copper(II) Complexes with a Labile Coordination Site Supported by a tris-Tetramethylguanidinato Ligand2017
Author(s)
Ikuma Shimizu, Yuma Morimoto, Dieter Faltermeier, Marion Kerscher, Sayantan Paria, Tsukasa Abe, Hideki Sugimoto, Nobutaka Fujieda, Kaori Asano, Takeyuki Suzuki, Peter Comba,* and Shinobu Itoh*
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Journal Title
Inorg. Chem.
Volume: 56
Issue: 16
Pages: 9634-9645
DOI
Related Report
Peer Reviewed / Int'l Joint Research
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