Studies on renewable two-electron reductant and oxidant aimed at water oxidation and CO2 reduction
| Project/Area Number |
26288024
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| Research Category |
Grant-in-Aid for Scientific Research (B)
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| Allocation Type | Partial Multi-year Fund |
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| Section | 一般 |
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| Research Field |
Inorganic chemistry
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| Research Institution | Kyoto University |
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Principal Investigator |
TANAKA KOJI. 京都大学, 物質ー細胞統合システム拠点, 研究員 (00029274)
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| Project Period (FY) |
2014-04-01 – 2017-03-31
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| Project Status |
Completed (Fiscal Year 2016)
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| Budget Amount *help |
¥17,160,000 (Direct Cost: ¥13,200,000、Indirect Cost: ¥3,960,000)
Fiscal Year 2016: ¥3,250,000 (Direct Cost: ¥2,500,000、Indirect Cost: ¥750,000)
Fiscal Year 2015: ¥5,720,000 (Direct Cost: ¥4,400,000、Indirect Cost: ¥1,320,000)
Fiscal Year 2014: ¥8,190,000 (Direct Cost: ¥6,300,000、Indirect Cost: ¥1,890,000)
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| Keywords | water oxidation / CO2 reduction / NAD/NADH model / Renewable reductant / oxyl radical complexes / Amino radical complexes / 二酸化炭素還元反応 / 再生可能有機ヒドリド試薬 / NAD/NADHモデル / 再生可能エネルギー / 再生可能有機ヒドリド / ２電子還元剤 / ２電子酸化剤 / プロトン移動と共役した電子移動 / 二酸化炭素還元 / 光化学的二酸化炭素還元 |
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| Outline of Final Research Achievements |
This study is to construct NADH/NAD redox models as renewable two-electron oxidant and reductant for water oxidation and CO2 reduction. Electrochemical reduction of Ru-NADH model in CO2 saturated aqueous solutions catalytically produced HCOO-. This is the first example of catalytic CO2 reduction mediated with renewable organic hydride donor catalyst.
Ru-dioxolene frameworks exhibit very strong dπ-pπ interaction between Ru t2g and ligand π*. Deprotonation of aqua- and amino-Ru-dioxolene complexes further expands π－electron delocalization, which effectively stabilizes unusual oxyl and amino radicals. Oxidative activation of two oxyl radicals derived from dimeric aqua-Ru-dioxolen complexes resulted in O-O bond formation at the stage prior to O2 evolution in water oxidation. Oxidative activation of the anylinyl radical complex brought about intermolecular N-C bond formation through radical coupling between anilinyl radical and para-position of phenyl ring of aniline.
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Report
(4 results)
Research Products
(33 results)
