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Creation of New Chemistry for Energy Conversion from pH gradients

Research Project

Project/Area Number 12440190
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field Inorganic chemistry
Research InstitutionInstitute for Molecular Science

Principal Investigator

TANAKA Koji  Institute for Molecular Science prof, 分子科学研究所, 教授 (00029274)

Project Period (FY) 2000 – 2001
Project Status Completed (Fiscal Year 2001)
Budget Amount *help
¥15,400,000 (Direct Cost: ¥15,400,000)
Fiscal Year 2001: ¥3,800,000 (Direct Cost: ¥3,800,000)
Fiscal Year 2000: ¥11,600,000 (Direct Cost: ¥11,600,000)
KeywordsAqua-RU complex / Oxo-Ru complex / Oxyl radical / dioxygen evolution / energy conversion / pH gradients / エネルギー変換 / 酸化反応 / 水の4電子酸化 / オキソ金属錯体
Research Abstract

Aqua-Ru-quinone complexes, [Ru(trpy)(Q)(OH_2)]^<2+>, dissociate proton to give[Ru(trpy)(Q)(OH^-)]^+ with anionic hydroxy group or [Ru(trpy)(SQ)(HO^-)]+ with hydroxy radical, that is produced by intramolecular electron transfer from hydroxy anion to quinone. Dissociation of hydroxy proton of [Ru(trpy)(Q)(OH^-)]^+ also intramolecula electron transfer from the resultant oxy1 dianion ot quinone. We have successfully isolated [Ru(trpy)(SQ)(O^-)]^0 and determinined the molecular structure of the first Ru-oxo complex with oxyl radical. The fact that Ru-O bound distance of the oxyl radicla complexes is close to that of Ru-OH_2 bond indicates that the multi-bond character is not so high in the Ru-O bond. The Ru-oxo complex with oxyl radicla has essentially no ability to oxidize organic compounds, but one-electron oxidized form of the complex abstract hydrogen atoms of cyclic diens. Compared with monomeric Ru-oxo complexes, dinuclear Ru-oxo one showed high reactivity for hydrogen abstraction of cyclic dienes upon two electron oxidation of the complex. Moreover, the dinuclear complex showed high catalytic ability for four-electron oxidation of water, and the turnover number of dioxygen was 35000 based on the complex. Thus, we succeeded energy conversion from pH gradients to electricity, and also oxidation of not only organic compounds but also water by using unique redox behavior of aqua-Ru-dioxolene complexes.

Report

(3 results)
  • 2001 Annual Research Report   Final Research Report Summary
  • 2000 Annual Research Report
  • Research Products

    (30 results)

All Other

All Publications (30 results)

  • [Publications] Kaname Ito, Toshi Nagata, Koji Tanaka: "Synthesis and Electrochemical Properties of Transition Metal Complexes of 2,2' : 6',2''-Terpyridine 1,1''-Dioxide"Inorganic Chemistry. 40. 6331-6333 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Takashi Tomon, Dai Ooyama, Tohru Wada, Shiren Kazushi, Koji Tanaka: "A Ru-carbene Complex with a metallacycle involving a 1,8-naphthylidine framework"Chemical Communication. 1100-1101 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] H.Sugimoto, K.Tanaka: "Ruthenium Terpyridine Complexes with Mono-and Bidentate Dithiolene Ligands"Journal Chemical Society. Dalton Transaction. 57-63 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T.Wada, K.Tsuge, K.Tanaka: "Synthesis and Redox Propertics of Bis(ruthenium-hydroxo)complexes with Quinone and Bipyridine Ligand as Water-Oxidation Catalysis"Inorganic Chemistry. 40. 329-335 (2001)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] E.Fujita, M.Chou, K.Tanaka: "Chracterization of Ru(bpy)2(CO)(COO) prepared by C02 addition to Ru(bpy)2(CO) in acetonitrile"Applied Organometallics Chemistry. 14. 3515-3521 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.TsugemK, Kurihara, K.Tanaka: "Energy Conversion from Proton Gtradient to Electricity Based on Characteristic Redox Behavior of an Aqua Ruthenium with a WQuinone Ligand"Bulletin of Chemical Society of Japan. 73. 607-614 (2000)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Kaname Ito, Toshi Nagata, Koji Tanaka: "Synthesis and Electrochemical Properties of Transition Metal Complexes of 2,2':6',2"-Terpyridine 1,1 "-Dioxide,"Inorg. Chein. 40. 6331-6333 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Takashi Tonion, Dai Ooyama, Tohru Wada, Shiren Kazushi and Koii Tanaka: "A Ru-carbene Complex with a metallacycle involving a 1,8-naphthylidine framework"Chem. Coinm. 1100-1101 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] H.Sugimoto and K. Tanaka: "Ruthenium Teipyridine Complexes with Mono- and Bidentate Dithiolene Ligands"J. Chem. Soc.. DaltonTrans. 57-63 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T. Wada, K. Tsuge and K. Tanaka: "Synthesis and Redox Properties of Bis(ruthenium-hydroxo)complexe with Quinone and Bipyridine Ligand as a Water-Oxidation Catalysts"Inorg. Chem. 40. 329 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Fujita, Etsuko; Chou, Mei ; Tanaka, Koji: "Characterization of Ru(bpy)2(CO)(COO) prepared by CO2 addition to Ru(bpy)2(CO) in acetonitrile"Appl. Orgauomet. Chem. 14(12). 844-846 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] Toshi Nagata, Koji Tanaka: "Pentadentate Terpyridine-Catechol Linked Ligands and Their Cobalt(II) Complexes"Inorg. Chem. 39. 3515-3521 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Tanaka and T. Mizukawa: "Selective Formation of Ketdnes by Electrochemical Reduction of CO2 Catalyzed by Ruthenium Complexes"Appl. Orgaiiometallic Chem. 14. 863-866 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T. Wada, K. Tsuge and K. Tanaka: "Oxidation of Hydrocarbons by Mono- and Dinuclear Ruthenium Quinone Complexes via Hydrogen Atom Abstraction"Chem. Lett. 910-911 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T. Nagata and K. Tanaka: "Pentadentate Terpyri dine- Catechol Linked Ligands and Their Cobalt(III) Complexes"Inorg. Chem. 39. 3515-3521 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K. Tsuge, M. Kurihara and K. Tanaka: "Energy Conversion from Proton Gradient to Electricity Based on Characteristic Redox Behavior of an Aqua Ruthenium Complex with a Quinone Ligand."Bull. Chem. 73. 607-614 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] T. Wada, K. Tsuge and K. Tanaka: "Electrochemical Water-Oxidation to Dioxygen Catalyzed by Oxidized Form of Bis(ruthenium-hydroxo) - Complex in H2O"Angew. Chem, Int. Ed. 39(8). (2000)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] H. Sugimoto, K. Tsuge and K. Tanaka: "Double Addition of CO2 and CH3OH to Ruthenium Carbonyl Complex with Novel Mono-dentate Dithiolene"Chem. Lett. 1007-1008 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      2001 Final Research Report Summary
  • [Publications] K.Tanaka, D.Ooyama: "Multi-electron reductionof CO2 via Ru-C02, -C(O)OH, -CO, -CHO, and-CH2OH species"Coordination Chemistry Review. 226. 211-218 (2002)

    • Related Report
      2001 Annual Research Report
  • [Publications] Kaname Ito, Toshi Nagata, Koji Tanaka: "Synthesis and Electrochemical Properties of Transition Metal Complexes of 2, 2' : 6', 2"-Terpyridine 1, 1"-Dioxide"Inorganic Chemistry. 40. 6331-6333 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] Takashi Tomon, Dai Ooyama, Tohru Wada, Shiren Kazusbi, Koji Tanaka: "A Ru-carbene Complex wnn a metallacycle involving a 1, 8-naphthylidine framework"Chemical Communication. 1100-1101 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] H.Sugimoto, K.Tanaka: "Ruthenium Terpyridine Complexes with Mono-and Bidentate Dithiolene Ligands"Journal Chemical Society. Dalton Transaction. 57-63 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] T.Wada, K.Tsuge, K.Tanaka: "Synthesis and Redox Properties of Bis(ruthenium-hydroxo)complexes with Quinone and Bipyridine Ligand as a Water-Oxidation Catalysts"Inorganic Chemistry. 40. 329-335 (2001)

    • Related Report
      2001 Annual Research Report
  • [Publications] K.TsugemK.Kurihara, K.Tanaka: "Energy Conversion from Proton Gtradient to Electricity Based on Characteristic Redox Behavior of an Aqua Ruthenium with a Quinone Ligand"Bulletin of Chemical Society of Japan. 73. 607-614 (2000)

    • Related Report
      2001 Annual Research Report
  • [Publications] 田中晃二,水川哲徳: "Selective Formation of Ketones by Electrochemical Reduction of CO2 Catalyzed by Ruthenium Complexes"Applied Organometallic Chemistry. 14. 863-866 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] 杉本秀樹,田中晃二: "Ruthenium Terpyridine Complexes with Mono-and Bidentate Dithiolene Ligands"Journal of Chemical Society, Dalton Transaction. 57-63 (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] 和田亨,柘植清志,田中晃二: "Synthesis and Redox Properties of Bis(ruthenium-hydroxo) complexes with Quinone and Bipyridine Ligand as a Water-Oxidation Catalysts"Inorganic Chemistry. 73. 607-614 (2001)

    • Related Report
      2000 Annual Research Report
  • [Publications] 和田亨,柘植清志,田中晃二: "Oxidation of Hydrocarbons by Mono-and Dinuclear Ruthenium Quinone Complexes via Hydrogen Atom Abstraction"Chemistry Letters. 910-911 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] 永田央,田中晃二: "Pentadentate Terpyridine-Catechol Linked Ligands and Their Cobalt(II) Complexes"Inorganic Chemistrt. 39. 3515-3521 (2000)

    • Related Report
      2000 Annual Research Report
  • [Publications] 柘植清志,栗原正人,田中晃二: "Energy Conversion from Proton Gradient to Electricity Based on Characteristic Redox Behavior of an Aqua Ruthenium Complex with a Quinone Ligand"Bulletin Of Chemical Society of Japan. 73. 607-614 (2000)

    • Related Report
      2000 Annual Research Report

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Published: 2000-04-01   Modified: 2016-04-21  

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