| Project/Area Number |
18K14241
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| Research Category |
Grant-in-Aid for Early-Career Scientists
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| Allocation Type | Multi-year Fund |
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| Review Section |
Basic Section 34010:Inorganic/coordination chemistry-related
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| Research Institution | Nagoya University |
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Principal Investigator |
Jung Jieun 名古屋大学, 理学研究科, 助教 (60801008)
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| Project Period (FY) |
2018-04-01 – 2020-03-31
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| Project Status |
Completed (Fiscal Year 2019)
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| Budget Amount *help |
¥4,160,000 (Direct Cost: ¥3,200,000、Indirect Cost: ¥960,000)
Fiscal Year 2019: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000)
Fiscal Year 2018: ¥2,080,000 (Direct Cost: ¥1,600,000、Indirect Cost: ¥480,000)
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| Keywords | 二酸化炭素 / 光触媒 / 光還元 / レーザーフラッシュフォトリシス / 反応機構 / イリジウム / モリブデン / オスミウム / メカニズム / モリブデン錯体 / イリジウム錯体 / ギ酸 / Carbon dioxide / Photoreduction / Photocatalyst / Iridium complex / Laser flash photolysis |
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| Outline of Final Research Achievements |
Structurally robust, new (PNNP)M complexes were synthesized, and used for photoinduced reduction of CO2 under light. The key aspects for the design of the catalysts are (i) the introduction of a bulky PNNP ligand, which has been shown to prevent catalyst deterioration and promote efficient hydrogenation, and (ii) the incorporation of bipyridyl CH2P groups, which could potentially act as proton donors.
Photocatalytic CO2 reduction using a (PNNP)Ir complex continuously gave us formic acid for over 1 week, indicating the Ir complex ligated PNNP ligand is robust enough for the photocatalytic reaction. A variety of new (PNNP)M base metal complexes (M = Mo, Mn, Co, Fe) and (PNNP)M noble metal complexes (M = Ru, Os) were successfully synthesized by modifying the ligands of the metal complexes. The present study has thus provided new insights into the development of efficient catalysts for CO2 reduction reactions and a system for photoinduced CO2 reduction using water to mimic photosynthesis.
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| Academic Significance and Societal Importance of the Research Achievements |
イリジウム錯体(PNNP)Irについては最適反応条件の検討を行った結果、CO2の光還元触媒としてはたらく単核金属錯体としては世界最高の触媒回転数（TON = ~3000）を達成した。(PNNP)Os錯体は既存のOs錯体を遥かに上回る触媒活性を示した。単核のMo錯体がCO2の光還元触媒として単独ではたらくことを示した初めての報告例であるとともに、ギ酸選択的にCO2の光還元反応が進行する数少ない例の一つでもある。
(PNNP)Mを基本骨格構造とした新規CO2光還元触媒の開発および得られた知見は水と太陽光を用いたCO2還元技術の確立と、それに基づく持続可能な循環型社会の実現に貢献することを期待される。
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