| Project/Area Number |
21K14642
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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, 講師 (60801008)
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| Project Period (FY) |
2021-04-01 – 2023-03-31
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| Project Status |
Completed (Fiscal Year 2022)
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| Budget Amount *help |
¥4,550,000 (Direct Cost: ¥3,500,000、Indirect Cost: ¥1,050,000)
Fiscal Year 2022: ¥2,210,000 (Direct Cost: ¥1,700,000、Indirect Cost: ¥510,000)
Fiscal Year 2021: ¥2,340,000 (Direct Cost: ¥1,800,000、Indirect Cost: ¥540,000)
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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 / タングステン / Carbon dioxide / Photoreduction / Photocatalyst / Molybdenum complex / Laser flash photolysis / Photocatalysis / CO2 reduction / Mo complex / laser flash photolysis / mechanism |
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| Outline of Research at the Start |
Converting carbon dioxide (CO2) into carbon-containing value-added produces and feedstocks is extremely important to reduce CO2 emissions. In typical photocatalytic CO2 reduction using single-active-site photocatalysts, noble metal complexes have frequently been used as a photocatalyst for CO2 reduction by virtue of the relatively long-lived excited state under light. The goal of this research is to establish cost-effective and environmental benign systems for selective photocatalytic CO2 reduction using a non-noble metal complex as a photocatalyst under mild conditions.
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| Outline of Final Research Achievements |
Structurally robust, new (PNNP)M (M = Ir, Mo, W, Cr, Mn) complexes were synthesized, and used for photoinduced reduction of carbon dioxide (CO2) under light. The main purpose of this research is to discover non-noble photocatalysts for CO2 reduction by switching the metal center from Ir to a non-noble metal complex and electronic and steric modification of the ligand. Photocatalytic CO2 reduction using a (PNNP)Mo complex continuously gave us formic acid as the main product, reaching the turnover number (TON) of > 440 at 160 h.
A variety of (PNNP)M metal complexes were synthesized by modifying the ligands of the metal complexes, and exploited to catalyze electrocatalytic CO2 reduction in an aqueous solution through heterogenization of the catalyst onto the surface of a carbon paper. The heterogenized molecular complex exhibited outstanding CO2 reduction activity to give formate as the main product with a high Faradaic efficiency of ~86% at a very small overpotential of around 90 mV.
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| Academic Significance and Societal Importance of the Research Achievements |
モリブデン錯体については、貴金属を用いない同様のCO2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を達成した。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還元触媒の開発は金属錯体－半導体ハイブリッド光触媒の最適化によって高効率なCO2還元反応が達成され、人工光合成触媒系へと繋げることができる。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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