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2005 Fiscal Year Final Research Report Summary

Nanoscale Designing of Iron-Sulfur Active Center in Nitrogenase towards Nano-biomimetic Enzyme

Research Project

Project/Area Number 15550129
Research Category

Grant-in-Aid for Scientific Research (C)

Allocation TypeSingle-year Grants
Section一般
Research Field Functional materials chemistry
Research InstitutionKEIO UNIVERSITY

Principal Investigator

NAKAJIMA Atsushi  Keio University, Faculty of Science and Technology, Professor, 理工学部, 教授 (30217715)

Project Period (FY) 2003 – 2005
KeywordsFunctional Cluster / Enzyme / Soft-landing / Self-assembled Layer / Alkanethiol Molecules / Gold Substrate / Silicon Substrate
Research Abstract

The aim of this research has focused on the creation of nanoscale biomimetic enzyme by unveiling the function and mechanism of an iron-sulfur active center in nitrogenase enzyme. To achieve this research target, two methodologies have been developed ; (1) The production technique of organometallic and molecular clusters has been refined by laser vaporization and molecular beam in order to generate functional cluster efficiently through gas phase reactions. (2) The soft-landing method using self-assembled monolayer on a gold substrate was broadened toward various substrates, and their characteristics were evaluated by infrared reflection absorption spectroscopy (IRAS) and temperature programmed desorption spectroscopy.
Functional clusters, such as organometallic cluster of vanadium-benzene, could be soft-landed efficiently onto the self-assembled monolayer on a gold substrate compared to a bare gold substrate. The adsorption state and thermal stability of V(benzene)_2 sandwich clusters soft-landed onto a self-assembled monolayer of different chain-length n-alkanethiols (C_n-SAM, n = 8, 12, 16, 18, and 22) were studied. The IRAS measurement confirmed that V(benzene)_2 clusters are molecularly adsorbed and maintain a sandwich structure on all of the SAM substrates. In addition, the clusters supported on the SAM substrates are oriented with their molecular axes tilted 70-80° off the surface normal. An Arrhenius analysis of the TPD spectra reveals that the activation energy for the desorption of the supported clusters increases linearly with the chain-length of the SAMs. For the longest chain C_<22>-SAM, the activation energy reaches around 150 kJ/mol, and the thermal desorption of the supported clusters can be considerably suppressed near room temperature, which is superior to a silicon substrate covered with hydrocarbon molecules.

  • Research Products

    (12 results)

All 2006 2005

All Journal Article (12 results)

  • [Journal Article] Soft-Landing Isolation of Vanadium-Benzene Sandwich Clusters on a Room-Temperature Substrate Using n-Alkanethiolare Self-Assembled Monolayer Matrixes2006

    • Author(s)
      Masaaki Mitsui, Shuhei Nagaoka, Takeshi Matsumoto, Atsushi Nakajima
    • Journal Title

      The Journal of Physical Chemistry B 110・7

      Pages: 2968-2971

    • Description
      「研究成果報告書概要(和文)」より
  • [Journal Article] Electronic Properties of Cs-Atom Doped Aluminum and Silicon Clusters : Al_nCs_m and Si_nCs_m2006

    • Author(s)
      Kiichirou Koyasu, Minoru Akutsu, Junko Atobe, Masaki Mitsui, Atsushi Nakajima
    • Journal Title

      Chemistry Physics Letters 421・4-6

      Pages: 534-539

    • Description
      「研究成果報告書概要(和文)」より
  • [Journal Article] Photoelectron Spectroscopy of Binary Au Cluster Anions with A Doped Metal Atom : Au_nM^- (n =2-7), M = pd, Ni, Zn, Cu, and Mg2006

    • Author(s)
      Kiichirou Koyasu, Minoru Akutsu, Junko Atobe, Masaaki Mitsui, Atsushi Nakajima
    • Journal Title

      Chemistry Physics Letters 422・1,2

      Pages: 62-66

    • Description
      「研究成果報告書概要(和文)」より
  • [Journal Article] Classification and characterization of gold and nickel nanoparticles with a differential mobility analyzer2006

    • Author(s)
      Yasutomo Naono, Sayuri Kawabata, Seung H. Huh, Atsushi Nakajima
    • Journal Title

      Science and Technology of Advanced Materials 7・2

      Pages: 209-215

    • Description
      「研究成果報告書概要(和文)」より
  • [Journal Article] Laser Synthesis of Amorphous Iron and Cobalt Carbide Nanoparticles with Carbon Onion : Magnetic Core Shells2006

    • Author(s)
      Seung H.Huh, Atsushi Nakajima
    • Journal Title

      Journal of Applied Physics 99・6

      Pages: 064302(5pages)

    • Description
      「研究成果報告書概要(和文)」より
  • [Journal Article] Soft-Landing Isolation of Vanadium-Benzene Sandwich Clusters on a Room-Temperature Substrate Using n-Alkanethiolate Self-Assembled Monolayer Matrices2006

    • Author(s)
      M.Mitsui, S.Nagaoka, T.Matsumoto, A.Nakajima
    • Journal Title

      J.Phys.Chem.B 110(7)

      Pages: 2968-2971

    • Description
      「研究成果報告書概要(欧文)」より
  • [Journal Article] Electronic properties of Cs-atom doped aluminum and silicon clusters : Al_nCs_m and Si_nCs_m2006

    • Author(s)
      K.Koyasu, M.Akutsu, J.Atobe, M.Mitsui, A.Nakajima
    • Journal Title

      Chem.Phys.Lett. 421(4-6)

      Pages: 534-539

    • Description
      「研究成果報告書概要(欧文)」より
  • [Journal Article] Photoelectron spectroscopy of binary Au cluster anions with doped metal of M = Pd, Ni, Zn, Cu, and Mg : Au_nM- (n = 2-7)2006

    • Author(s)
      K.Koyasu, Y.Naono, M.Akutsu, M.Mitsui, A.Nakajima
    • Journal Title

      Chem.Phys.Lett. 422(1,2)

      Pages: 62-66

    • Description
      「研究成果報告書概要(欧文)」より
  • [Journal Article] Classification and characterization of gold and nickel nanoparticles with a differential mobility analyzer2006

    • Author(s)
      Y.Naono, S.Kawabata, S.H.Huh, A.Nakajima
    • Journal Title

      Science and Technology of Advanced Materials 7(2)

      Pages: 209-215

    • Description
      「研究成果報告書概要(欧文)」より
  • [Journal Article] Laser synthesis and magnetism of amorphous iron and cobalt carbide nanoparticles with carbon onion2006

    • Author(s)
      S.H.Huh, A.Nakajima
    • Journal Title

      J.Appl.Phys. 99(6)

      Pages: 064302(5pages)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Journal Article] Formation and Photoelectron Spectroscopy of Nanoscale Cluster Anions of Biphenyl, (BP)_n (n = 2-100)2005

    • Author(s)
      Masaaki Mitsui, Yukino Matsumoto, Naoto Ando, Atsushi Nakajima
    • Journal Title

      Chemistry Letters 34・9

      Pages: 1244-1245

    • Description
      「研究成果報告書概要(和文)」より
  • [Journal Article] Formation and Photoelectron Spectroscopy of Nanoscale Cluster Anions of Biphenyl, (BP)_n-(n = 2-100)2005

    • Author(s)
      M.Mitsui, Y.Matsumoto, N.Ando, A.Nakajima
    • Journal Title

      Chemistry Letters 34(9)

      Pages: 1244-1245

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

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Published: 2007-12-13  

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