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Design and construction of metalloproteins/bilayer film devices and their application

Research Project

Project/Area Number 08455443
Research Category

Grant-in-Aid for Scientific Research (B)

Allocation TypeSingle-year Grants
Section一般
Research Field 高分子合成
Research InstitutionNagasaki University

Principal Investigator

NAKASHIMA Naotoshi  NAGASAKI UNIVERSITY,FACULTY OF ENGINEERING,PROFESSOR, 工学部, 教授 (80136530)

Co-Investigator(Kenkyū-buntansha) MURAKAMI Hiroto  NAGASAKI UNIVERSITY,FACULTY OF ENGINEERING,RESEARCH ASSOCIATE, 工学部, 助手 (30274624)
Project Period (FY) 1996 – 1998
Project Status Completed (Fiscal Year 1998)
Budget Amount *help
¥7,800,000 (Direct Cost: ¥7,800,000)
Fiscal Year 1998: ¥1,500,000 (Direct Cost: ¥1,500,000)
Fiscal Year 1997: ¥2,200,000 (Direct Cost: ¥2,200,000)
Fiscal Year 1996: ¥4,100,000 (Direct Cost: ¥4,100,000)
Keywordsredox protein / artifical lipid / device / electron transfer / phase transition / ferredoxin / mediation / supramolecule / カチオン性人工脂質 / 修飾電極 / 相転移 / 拡散定数 / 分子機能電極 / 二分子膜フィルム / タンパク質 / イオン交換 / 電極デバイス / グルコース酸化酵素
Research Abstract

Results of our research project titled on Design and construction of metalloproteins/bilayer film devices and their application are summarized as follows.
1. A ferrocene with double long chains, 2C16GluFc, was synthesized and regulated mediated electron transfer reactions of glucose oxidase immobilized on a lipid film containing ferrocene was examined. A graphite (BPG) electrode modified with a cast of 2CI6GluFc and a synthetic lipid, dihexadecyldimethylammonium bromide (2C16N^+Br^-) gave phase transition dependent cyclic voltammograms. Normal pulse voltammetry proved that the enhancement of the faradaic current at the electrode at temperatures above the phase transition is ascribable to the increase in the apparent diffusion rate constants. Glucose oxidase was immobilized on the film of 2C16GluFc/2C16N^+Br^- on BPG and ferrocene-mediated catalytic electron transfers in the presence of glucose were explored. Temperature experiment has revealed that the phase transition regulates the catalytic electron transfer reaction.
2. Thermal stability of the [2Fe-2S] cluster structure of ferredoxin embedded in the films of four artificial ammonium lipid was much improved than that of ferredoxin in solution. Artificial cationic ammonium lipid films were found to provide suitable microenvironments for the incorporation of ferredoxin in a way to undergo electrochemical communication with the underlying electrodes. We have demonstrated for the first time that the diffusion constant, D, and the heterogeneous electron transfer rate constant, k^0', for ferredoxin embedded in a cast film of an artificial lipid, 2C18N^+Br^-, are 4 X 10^-^1^0 cm^2 s^-^1 and 1.4 X 10^-^4 cm s^-^1, respectively. D and k^0' values of ferredoxin in the films of the films were close with those of ferredoxin in 2C18N^+r^- films. The experimentally observed voltammograms of ferredoxin in the film fitted well with the simulated voltammograms using the obtained D and k^0'.

Report

(4 results)
  • 1998 Annual Research Report   Final Research Report Summary
  • 1997 Annual Research Report
  • 1996 Annual Research Report
  • Research Products

    (43 results)

All Other

All Publications (43 results)

  • [Publications] A-E.F.Nassar,J.F.Rusling and N.Nakashima: "Electron Transfer between Electrodes and Heme Proteins in Protein-DNA Films" J.Am.Chem.Soc.118. 3043-3044 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Tominaga,H.Yanagimoto,A-E.F.Nassar,J.F.Rusling and N.Nakashima: "Incorporation and Direct Electron Transfer of Chlorella Ferredoxin in the Bilayer Films of Cationic Lipids on Electrodes" Chem.Lett.1996. 523-524 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Nakashima,Y.Miyata and M.Tominaga: "Electrochemical Characterization of an Assembled Monolayer of α-Methoxy-ω-mercapto-poly(ethylene glycol)on Gold and Complex Formation of the Monolayer with α-Cyclodextrin" Chem.Lett.1996. 731-732 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] 中嶋 直敏: "脂質二分子膜修飾電極の設計と電気化学特性の制御" 電気化学. 64. 168-171 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] 冨永昌人,中嶋直敏: "蛋白質/2分子膜フィルムの電極上への固定化と電子移動反応" 蛋白質 核酸 酵素. 41. 1600-1605 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] A-E.F.Nassar,J.F.Rusling,M.Tominaga,J.Yanagimoto and N.Nakashima: "Electrochemistry of Cast films of Ferredoxin and Lipid Bilayers on Electrodes" J.Electroanal.Chem.416. 183-185 (1996)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Tominaga,S.Kusano N.Nakashima: "Tuning of lipid bilayer fluidity regulates mediated electron transfer reactions of glucose oxidase immobilized on lipid bilayer films on an electrode" Bioelectrochemistry and Bioenergetics. 42. 59-62 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Nakashima,T.Tokunaga,T.Nakanishi,Y.Nonaka,H.Murakami,T.Sagara: "A Fullerene/Lipid Electrode Device:Reversible Electron Transfer Reaction of C60 Embedded in a Cast Film of an Artificial Ammonium Lipid on an Electrode in Aqueous Solution" Angew.Chem.Int.Ed.37. 2671-2673 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Nakashima,Y.Nonaka,T.Nakanishi ,T.Sagara,H.Murakami: "A C60-Embedded Artificial Bilayer Membrane Film Electrode Device:Phase Transition Dependent Electrochemistry" J.Phys.Chem.B.102. 7328-7330 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Nakashima,T.Kuriyama,T.Tokunaga,H.Murakami,T.Sagara: "Electrochemistry of a Fullerene/Ammonium Lipid Composite Film on an Electrode in Water. Generation of C603-" Chem.Lett.1998. 633-634 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] 冨永昌人,中嶋直敏: "分子集合系での生体機能分子の電子移動反応制御" 表面. 36. 179-187 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] T.Nakanishi,H.Murakami,T.Sagara,N.Nakashima: "Aqueous Electrochemistry of a C60-Bearing Artificial Lipid Bilayer Membrane Film Immobilized on an Electrode Surface" J.Phys.Chem.B.103. 304-308 (1999)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] 中嶋直敏: "最新の分離・精製・検出法" (株)エヌ・ティー・エス, 1065 (1997)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] 中嶋直敏: "表面技術便覧" 日刊工業新聞社, 1836 (1998)

    • Description
      「研究成果報告書概要(和文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] A-E.F.Nassar: "Electron Transfer between Electrodes and Heme Proteins in Protein-DNA Films" J,Am.Chem.Soc.118. 3043-3044 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Tominaga: "Incorporation and Direct Electron Transfer of Chlorella Ferredoxin in the Bilayer Films of Cationic Lipids on Electrodes" Chem.Lett., 1996. 523-524 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Nakashima: "Electrochemical Characterization of an Assembled Monolayer of alpha-Methoxy-omega-mercapto-poly (ethylene glycol) on Cold and Complex Formation of the Monolayer with alpha-Cyclodextrin" Chem.Lett., 1996. 731-732 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Nakashima: "Design of a Lipid Bilayer-modified Electrode and Regulated Electrochemistry" DENKIKAGAKU. 64. 168-171 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Tominaga: "Immobilization of Protein/Lipid Films on Electrodes and Their Electron Transfer Reactions" Tanpakusitsu, Kouso and Kakusan. 41. 1600-1605 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] A-E.F.Nassar: "Electrochemistry of Cast films of Ferredoxin and Lipid Bilayers on Electrodes" J.Electroanal. Chem.416. 183-185 (1996)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Tominaga: "Tuning of lipid bilayer fluidity regulates mediated electron transfer reactions of glucose oxidase immobilized on lipid bilayer films on an electrode" Bioelectrochemistry and Bioenergetics. 42. 59-62 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Nakashima: "A Fullerene/Lipid Electrode Device : Reversible Electron Transfer Reaction of C60 Embedded in a Cast Film of an Artificial Ammoniun Lipid on an Electrode in Aqueous Solution" Angew.Chem.Int.Ed.37. 2671-2673 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Nakashima: "A C60-Embedded Artificial Bilayer Membrane Film Electrode Device : Phase Transition Dependent Electrochemistry" J.Phys.Chem.B.102. 7328-7330 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Nakashima: "Electrochemistry of a Fullerene/Ammonium Lipid Composite Film on an Electrode in Water. Generation of C603-" Chem.Lett., 1998. 633-634 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] M.Tominaga: "Regulated Electron Transfer Reactions of Biological Molecules in Molecular Assemblies" Hyoumen. 36. 179-187 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] T.Nakanishi: "Aqueous Electrochemistry of a C60- Bearing Aerifical Lipid Bilayer Membrane Film Immobilized on an Electrode Surface" J.Phys.Chem.B. 103. 304-308 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Nakashima: Recent Progress in Separation, Purification and Dedection. NTS Co., 1065 (1997)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] N.Nakashima: Hyoumen Gijyutsu Binran. Nikkankougyousinbunsha, 1836 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
    • Related Report
      1998 Final Research Report Summary
  • [Publications] T.Nakanishi,H.Murakami,T.Sagara,N.Nakashima: "Aqueous Electrochemistry of a C60-Bearing Artificial Lipid Bilayer membrane Film Immobilized on an Electrode Surface" J.Phys.Chem.B. 103. 304-308 (1999)

    • Related Report
      1998 Annual Research Report
  • [Publications] N.Nakashima,T.Tokunaga,T.Nakanishi,Y.Nonaka,H.Murakami,T.Sagara: "A Fullerene/Lipid Electrode Device: Reversible Electron Transfer reaction of C60 Embedded in a cast Film of an Artificial Ammonium Lipid on an Electrode in Aqueous Solution" Angew.Chem.Int.Ed.37. 2671-2673 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] N.Nakashima,Y.Nonaka,T.Nakanishi,T.Sagara,H.Murakami: "A C60-Embedded Artificial Bilayer Membrane Film Electrode Device: Phase Transition Dependent Electrochemistry" J.Phys.Chem.B.102. 7328-7330 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] N.Nakashima,T.Kuriyama,T.Tokunaga,H.Murakami,T.Sagara: "Electrochemistry of a Fullerene / Ammonium Lipid Composite Film on an Electrode in Water.Generation of C603-" Chem.Lett.1998. 633-634

    • Related Report
      1998 Annual Research Report
  • [Publications] 冨永昌人,中嶋直敏: "分子集合系での生体機能分子の電子移動反応制御" 表面. 36. 179-187 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] 中嶋直敏: "表面技術便覧" 日刊工業新聞社, 1836 (1998)

    • Related Report
      1998 Annual Research Report
  • [Publications] M.Tominaga,S.Kusano,N.Nakashima: "Tuning of lipid bilayer fluidity regulates mediated electron transfer reactions of glucose oxidase immobilized on lipid bilayer films on an electrode" Bioelectrochemistry and Bioenergetics. 42. 59-62 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] 富永昌人、中嶋直敏: "分子集合系での生体機能分子の電子移動制御" 表面. 36(印刷中). (1998)

    • Related Report
      1997 Annual Research Report
  • [Publications] 中嶋直敏: "最新の分離・精製・検出法" (株)エヌ・ティー・エス, 1065 (1997)

    • Related Report
      1997 Annual Research Report
  • [Publications] A.-E.F.Nassar,J.F.Rusling,M.Tominaga,J.Yanagimoto and N.Nakashima: "Electrochemistry of Cast films of Ferrdcoxin and Lipid Bilayers on Electrodes" J.Electroanal.Chem.(印刷中). (1997)

    • Related Report
      1996 Annual Research Report
  • [Publications] M.Tominaga,S.Kusano and N.Nakashima: "Tuning of lipid bilayer fluidity regulates mediated electron transfer reactions of glucose oxidase immobilized on lipid bilayer films on an electrode" Bioelectrochem.Bioenerg.(印刷中). (1997)

    • Related Report
      1996 Annual Research Report
  • [Publications] A-E.F.Nassar,J.F.Rusling and N.Nakashima: "Electron Transfer between Electrodes and Heme Proteins in Protein-DNA Films" J.Am.Chem.Soc.118. 3043-3044 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] M.Tominaga,J.Yanagimoto,A-E.F.Nassar,J.F.Rusling and N.Nakashima: "Incorporation and Direct Electron Transfer of Chlorella Ferredoxin in the Bilayer Films of Cationic Lipids on Electrodes" Chem.Lett.1996. 523-524 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] N.Nakashima,Y.Miyata and M.Tominaga: "Electrochemical Characterization of an Assembled Monolayer of α-Methoxy-ω-mercapto-poly(ethylene glycol) on Gold and Complex Formation of the Monolayer with α-Cyclodextrin" Chem.Lett.1996. 731-732 (1996)

    • Related Report
      1996 Annual Research Report
  • [Publications] 中嶋 直敏: "脂質二分子膜修飾電極の設計と電気化学特性の制御" 電気化学. 64. 168-171 (1996)

    • Related Report
      1996 Annual Research Report

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

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