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1996 Fiscal Year Final Research Report Summary

Development of selective oxygenation of nonactivated hydrocarbons by iron catalysts

Research Project

Project/Area Number 07455322
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field 触媒・化学プロセス
Research InstitutionKYOTO UNIVERSITY

Principal Investigator

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

Co-Investigator(Kenkyū-buntansha) SUGIURA Yukio  Kyoto University, Institute for Chemical Research, Professor, 化学研究所, 教授 (40025698)
TAKANO Mikio  Kyoto University, Institute for Chemical Research, Professor, 化学研究所, 教授 (70068138)
TANAKA Tsunehiro  Kyoto University, Graduated School of Engineering, Associate Professor, 工学研究科, 助手 (70201621)
Project Period (FY) 1995 – 1996
KeywordsNonheme Complex / Oxygenases / Monooxyenases / Dioxyenases / Catechol / Aromatic Ring Cleavage / Chlorocatechol / Development of Enzymatic Function
Research Abstract

Catalytic oxygenation of nonactivated hydrocarbons by oxygenase-model nonheme iron complexes has been studied from the viewpoints of catalysis.
Selective intradiol oxygenation of catechols by iron (III) complexes has been extensively studied. In this project the first example of catalytic oxygenation of chlorocatechols by model iron complexes has been achieved. This is very important result not only as the first model reaction for chlorocatechol dioxygenases, but also for the first step of development of decomposition of haloaromatics which are environmental pollutant. The model intermediate complexes, chlorocateholaoiron - (TPA) complexes have been isolated, and their structures were analyzed by XAFS.Another dioxygenase model reaction, i.e.lipoxygenase model reaction catalyzed by nonheme iron complexes, has been studied. Radical intermediates were detected by ESR,supporting the radical mechanism proposed in the enzymatic systems.
Monooxygenase model reactions have also been studied, specially by using hydroquinones as electron and proton transfer reagents. In this project, selective ortho-hydroxylation of phenols by iron (III) complexes has been developed, as an model reaction for tyrosine hydroxylase. It is specific that substituents on hydroquinones play essential role for controlling reactivity.

  • Research Products

    (10 results)

All Other

All Publications (10 results)

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

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

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

    • Description
      「研究成果報告書概要(欧文)」より
  • [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

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Published: 1999-03-16  

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