| Project/Area Number |
07651006
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| Research Category |
Grant-in-Aid for Scientific Research (C)
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| Allocation Type | Single-year Grants |
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| Section | 一般 |
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| Research Field |
工業物理化学
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| Research Institution | Waseda University |
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Principal Investigator |
YAMAMOTO Kimihisa Advanced Research Institute for Science and Engineering, Associate Professor, 理工学総合研究センター, 助教授 (80220458)
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| Co-Investigator(Kenkyū-buntansha) |
OYAIZU Kenichi School of Science and Engineering, Research Associate, 理工学部, 助手 (90277822)
TSUCHIDA Eishun School of Science and Engineering, Professor, 理工学部, 教授 (90063461)
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| Project Period (FY) |
1995 – 1996
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| Project Status |
Completed (Fiscal Year 1996)
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| Budget Amount *help |
¥2,200,000 (Direct Cost: ¥2,200,000)
Fiscal Year 1996: ¥300,000 (Direct Cost: ¥300,000)
Fiscal Year 1995: ¥1,900,000 (Direct Cost: ¥1,900,000)
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| Keywords | Vanadium Complex / Multi-nuclear Complex / O_24-electron Reduction / X-ray Analysis / mu-Dioxo Complex / One-step Multi-electron Transfer / Electrode Reaction / Planer Ligand / 複核錯体 / 酸素還元 |
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| Research Abstract |
Vanadyl (salen) multi-nuclear complexes act as electron mediators to allow catalytic multi-electron electroeduction of oxygen. By adjusting redox potentials to the value close to the thermodynamic potential for the 4-electron reduction of oxygen using a variety of ligands, the objective of the present study is to establish multi-electron reduction systems of molecular oxygen by the use of these complexes as electron mediators. It is also intended to elucidate novel molecular conversion systems by the use of these complexes as oxidation systems for organic substrates.
It the first year, vanadium complexes with inert ligands were prepared and the redox potentials were determined. Also, the corresponding dinuclear complexes were prepared. X-ray studies of these complexes revealed the structure of the oxygen-binding sites in these complexes. By near-infrared spectrum, the redox state of the complexes were determined. Kinetic analysis for the oxygenation of the catalyst revealed the presence of mu-dioxo intermediate.
In the second year, the selected vanadium complexes were used as electron mediators, and the reduction of oxygen was examined. Koutecky-Levich Plots obtained by the rotating ring-disk voltammetry revealed the 4-electron process and the production of water. The turn-over number of the catalyst was determined to exceed 10. It was concluded that selective 4-electron reduction system of oxygen was established.
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