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Development of metal complex/electron-transfer composite system realizing enzyme-like function

Research Project

Project/Area Number 07305062
Research Category

Grant-in-Aid for Scientific Research (A)

Allocation TypeSingle-year Grants
Section総合
Research Field 触媒・化学プロセス
Research InstitutionKYOTO UNIVERSITY

Principal Investigator

FUNABIKI Takuzo  Kyoto University, Faculty of Engineering, Associate Professor, 工学研究科, 助教授 (70026061)

Co-Investigator(Kenkyū-buntansha) WATANABE Yoshihito  Institute for Molecular Science, Professor, 教授 (10201245)
FUKUZUMI Toshikazu  Osaka University, Faculty of Engineering, Professor, 工学研究科, 教授 (40144430)
NARUTA Yoshinori  Kyushu University, Institute for Fundamenatal Research of Organic Chemistry, Pro, 有機化学基礎研究センター, 教授 (00108979)
OKURA Ichiro  Tokyo Institute of Technology, Department of Bioengineering, Professor, 生命理工学部, 教授 (90089821)
UEYAMA Norikazu  Osaka University, Faculty of Science, Associate Professor, 理学研究科, 助教授 (80093376)
Project Period (FY) 1995 – 1996
Project Status Completed (Fiscal Year 1996)
Budget Amount *help
¥2,900,000 (Direct Cost: ¥2,900,000)
Fiscal Year 1996: ¥2,900,000 (Direct Cost: ¥2,900,000)
KeywordsBiofunctional catalysts / Oxygenases / Electron-transfer function / Enzyme model / Nonheme enzyme / Metal complex / Electron-transfer composite / Iron-sulfure cluster / Monooxyenases / 鉄硫黄フラスター / モハオキシゲナーゼ
Research Abstract

In the aim of development of new types homogeneous catalysis by metal complexes which works in the similar fashion to metalloenzymes, the effective combination between metal complexes and electron-transfer systems has been studied. As electron-transfer and electron-donor systems, organic and inorganic reductants, electrochemical and photochemical systems have been used in the various catalytic systems involving oxygenations, oxygen generation from water, etc.in both enzymatic and model systems.
1)Selective oxygenations by metal complexes
Oxygenations by heme and nonheme iron complexes have been extensively studied, and developed new types of oxygenations, e.g., ortho-hydroxylation of phenols in the similar way to tyrosine hydroxylases, aromatic ring cleavage of chlorocatechols as the first model reaction for chlorocatechol dioxygenase, and oxygenation of ortho-aminophenols.
2)Biocatalytic reactions other than oxygenations
Various types of catalytic reactions were performed, e.g.functional catalytic antibody, biological NO generation, oxo-transfer reaction by molybdenum enzymes and model conplexes, modeling of the active center of cytochrome C oxidase and oxygen generation by model complexes.
3)Development of model systems for bioinorganicelectron-transfer process
Modeling of the skillful biological electron-transfer mechanisms has been developed, e.g.photo-excited intramolecular electron-transfer bybiologen-bound porphirins, electron-transfer process by artificial mioglobin, selective oxidation by electrochemical processes.

Report

(3 results)
  • 1996 Annual Research Report   Final Research Report Summary
  • 1995 Annual Research Report
  • Research Products

    (28 results)

All Other

All Publications (28 results)

  • [Publications] Takuzo Funabiki: "ortho-Hydroxylation of 4-tert-butylphenol by nonheme iron(III) complexes as a functional model reaction for tyrosine hydroxylase" J.Chem.Soc.,Chem.Commun. 151-152 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Tadashi Okamoto: "Fundamental studies on the development of lignin-based adhesives.I.Catalytic demethylation of anisole with molecular oxygen" React.Kinet.Catal.Lett.58,2. 237-242 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Morifumi Fujita: "Addition versus oxygenation of alkylbenzenes with 10-methylacridinium ion via photoinduced electron transfer" J.Am.Chem.Soc.118. 8566-8574 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Yutaka Amano: "Effective photoinduced hydrogen evolution with hydrogenase in surfactant micelles" J.Mol.Catal.105. 125-130 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Yoshinori Naruta: "Effective photoinduced hydrogen evolution with hydrogenase in surfactant micelles" J.Mol.Catal.印刷中. (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Norikazu.Ueyama: "Magnetic Properties of Intramolecularly Hydrogen-bonded Carboxylate Copper(II) Dimer Complexes." J.Chem.Soc.,Chem.Commun.,. 1377-1378 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Takuzo Funabiki: "Oxygenases and Model Systems" Kluwer Academic Publishers,Dordrecht/Boston/London, 393 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Takuzo Funabiki: "ortho-Hudroxylation of 4-tert-butylphenol by nonheme iron (nl) complexes as a functional model reaction for tyrosine hydroxylase" J.chem.Soc., Chem.Commun.151-152 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Tadashi Okamoto: "Fundamental studies on the development of lignin-based adhesives. I.Catalytic demethylation of anisole with molecular oxygen" React.Kinet.Catal.Lett.58, (2). 237-242 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Tsunehiro Tanaka: "Photo-assisted Oxidation of 2-Methylpropane over Rb+-Modified V2O5/SiO2. Formation of 2-Methylpropan-2-ol from 2-Methylpropane and O2" J.Chem.Soc., Faraday Trans.1975-1979 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Hisao Yoshida: "Photooxidation of Propylene by O2 over Silica and Mg-loaded Silica" J.Chem.Soc., Chem.Commun.2125-2126 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Morifumi Fujita: "Addition versus oxygenation of alkylbenzenes with 10-methylacridinium ion via photoinduced electron transfer" J.Am.Chem.Soc.118. 8566-8574 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Yutaka Amano: "Effective photoinduced hydrogen evolution with hydrogenase in surfactant micelles" J.Mol.Catal.105. 125-130 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Yoshinori Naruta: "Effectove photoinduced hydrogen evolution with hydrogenase in surfactant micelles" J.Mol.Catal. (in press). (1977)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Norikazu.Ueyama: "Magnetic Properties of Intrmolecularly Hydrogen-bonded Carboxylate Copper (II) Dimer Complexes." J.Chem.Soc., Chem.Commun.1377-1378 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Takuzo Funabiki: Oxygenases and Model Systems. Catalysis by Metal Complexes, No19, Kluwer Academic Publishers, Dordrecht/Boston/London, 1-393 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1996 Final Research Report Summary
  • [Publications] Takuzo Funabiki: "ortho-Hydroxylation of 4-tert-butylphenol by nonheme iron(III)complexes as a functional model reaction for tyrosine hydroxylase" J.Chem.Soc.,Chem.Commun. 151-152 (1997)

    • Related Report
      1996 Annual Research Report
  • [Publications] Tadashi Okamoto: "Fundamental studies on the development of lignin-based adhesives. I.Catalytic demethylation of anisole with molecular oxygen" React.Kinet.Catal.Lett.58,2. 237-242 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] Morifumi Fujita: "Addition versus oxygenation of alkylbenzenes with 10-methylacridinium ion via photoinduced electron transfer" J.Am.Chem.Soc.118. 8566-8574 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] Yutaka Amano: "Effective photoinduced hydrogen evolution with hydrogenase in surfactant micelles" J.Mol.Catal.105. 125-130 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] Yoshinori Naruta: "Effective photoinduced hydrogen evolution with hydrogenase in surfactant micelles" J.Mol.Catal.(印刷中). (1997)

    • Related Report
      1996 Annual Research Report
  • [Publications] Takuzo Funabiki: "Oxygenases and Model Systems" Kluwer Academic Publishers,Dordrecht/Boston/London, 393 (1997)

    • Related Report
      1996 Annual Research Report
  • [Publications] T. Funabiki: "Functional Model Studies for Tyrosine Hydroxylases" J. Inorg. Biochem.59. 584 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] 船引卓三: "錯体材料化学" 月刊「化学工業」. 46. 617-623 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] Y. Watanabe: "Acylperoxo-Iron(III) Porphyrin Complexes : A New Entry of Potent Oxidants for the Alkene Epoxidation" J. Am. Chem. Soc.117. 6691-6697 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] Y. Naruta: "New and Efficient Synthesis of Oligomeric Porphyrins via stepwise Nucleophilic Substitution of Aminoporphyrins to Cyanuric Chloride" Chem. Lett.631-632 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] I. Okura: "Photo-induced Hydrogen Evolution with Hydrogenase and Cytochrome C3" Chem. Lett.33-34 (1995)

    • Related Report
      1995 Annual Research Report
  • [Publications] S. Ito: "A Model Compound of Novel Cofactor TTQ of Bacterial Methylamine Dehydro-genases. Synthesis and Physicohemical Properties" J. Am. Chem. Soc.117. 1485-1493 (1995)

    • Related Report
      1995 Annual Research Report

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Published: 1996-04-01   Modified: 2016-04-21  

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