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2000 Fiscal Year Final Research Report Summary

Metal Ion Collection Systems Based on the Ligned Basicity Change on Redox Reactions of Some Metal Complexes

Research Project

Project/Area Number 09554037
Research Category

Grant-in-Aid for Scientific Research (B).

Allocation TypeSingle-year Grants
Section展開研究
Research Field Inorganic chemistry
Research InstitutionHOKKAIDO UNIVERSITY

Principal Investigator

SASAKI Yoichi  Hokkaido Univ., Grad.School of Sci., Prof., 大学院・理学研究科, 教授 (30004500)

Co-Investigator(Kenkyū-buntansha) KANESATO Masatoshi  Tohoku National Industrial Research Institute, Functional Molecules Section, Senior Researcher, 東北工業技術研究所・機能化学部, 主任研究官
SUZUKI Toshishige  Tohoku National Industrial Research Institute, Chief Senior Researcher, 東北工業技術研究所, 首席研究官
ABE Masaaki  Hokkaido Univ., Grad.school of Sci., Inst., 大学院・理学研究科, 助手 (90260033)
Project Period (FY) 1997 – 2000
KeywordsMetal-Metal Bond / Transition Metal Elements / Functional Electrode / Enzyme Model Complexes / Metal Cluster Complexes / Redox Reactions / Electrode Reactions / Catalytic Reactions
Research Abstract

Basicity of oxide bridge of dinuclear complexes changes remarkably with the change in the oxidation states of the metal ions. It is thus possible to control the interaction of the oxide bridge with various Lewis acids like metal ions by changing the metal oxidation states. This work aimed at preparing the electrodes with surface self-assembled monolayers of such metal complexes, and use them as reversible metal-ion binder and to establish the method for the step-wise construction of metal-complex oligomers. The results are summarized as follows.
(1)Methods to construct Au self-assembled monolayers of polynuclear metal complexes have been established by using(i)mixed monolayers with alkyl sulfide and(ii)hydrogen bonding between the chains which contain C-CO-NH-groups.
(2)Protoncoupled electron transfer behavior of the oxo-bridged biruthenium complexes on gold surface have been quantitatively investigated. Diiron alnalaogs which are considered as models of biological diiron centers and are unstable towards redox reactions in solution, have been successfully studied in terms of pH-potential profiles over pH range of 1 and 12. The pKa values of the oxidized and reduced forms have been estimated for the first time for the model Fe-O-Fe complexes.
(3)Coupled redox reactions have been studied quantitatively with Lewis acids other than proton for the first time. Thus, for example, interaction of Al^<3+> ions at the oxide bridge is more sensitive to the metal ion oxidation states than protons.
(4)Step-wise oligomerization of the trinuclear oxo-centered Ru complexes on Au electrode has been established by controlling the metal oxidation state. The method is promising in contructing various supramolecular assemblies on electrode surfaces.

  • Research Products

    (12 results)

All Other

All Publications (12 results)

  • [Publications] Hiroshi Kumagai: "Chromatographic Selectivity of Rare Earth Elements on Iminodiacetate-Type Chelating Resins Having Spacer Arms of Different Lengths : Importance of Steric Flexibility of Functional Group in a Polymer Chelating Resin."Analytical Chmeistry. 70(No.1). 19-24 (1998)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] Masaaki Abe: "Synthesis and Electochemical Characterization of Self-Assembled Monolayers of Redox-Active Oxide-Bridged Triruthenium (III) Clusters on Au (111)."Journal of the Electroanalytical Chemistry. 473(No.1-2). 93-98 (1999)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] Pu Quan: "Chiral Molecular Patterns of Self-assembled Ion Pairs Composed of (R,S), (S)-16-Methyloctadecanoic Acid and 4,4'-Bipyridine."Chemical Communications. No.22. 2021-2022 (2000)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] Masaaki Abe: "Characterization of Novel Redox-Active Triruthenium (III) Complexes with a Disulfide-alkyl Ligand. Anion-Dependent Redox Behaviour of Monolayer Assemblies on Gold."Journal of the Chemical Society, Dalton Transactions. No.16. 2693-2701 (2000)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] Zhong-Ning Chen: "Chelate Formation around the Hexarhenium Cluster Center by a Diphosphane Ligand, Ph_2P(CH_2)_6PPh_2."Angewandte Chemie, International Edition in English. 40(No.1). 239-242 (2001)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] Akira Sato: "Cyclic Voltammetric Observation of CO/aqua Terminal Ligand Substitution Reactions for Trinuclear Ruthenium Complexes at Self-Assembled Monolayer Interfaces."Physical Chemistry Chemical Physics. (印刷中). (2001)

    • Description
      「研究成果報告書概要(和文)」より
  • [Publications] Hiroshi Kumagai, et al.: "Chromatographic Selectivity of Rare Earth Elements on Iminodiacetate-Type Chelating Resins Having Spacer Arms of Different Lengths : Importance of Steric Flexibiliy of Functional Group in a Polymer Chelating Resin."Analytical Chmeistry. 70(No.1). 19-24 (1998)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] Masaaki Abe, et al.: "Synthesis and Electochemical Characterization of Self-Assembled Monolayers of Redox-Active Oxide-Bridged Triruthenium(III)Clusters on Au(111)."Journal of the Electroanalytical Chemistry. 473(No.1-2). 93-98 (1999)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] Pu Quan, et al.: "Chiral Molecular Patterns of Self-assembled Ion Pairs Composed of (R, S), (S)-16-Methyloctadecanoic Acid and 4, 4'-Bipyridine."Chemical Communications. No.22. 2021-2022 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] Masaaki Abe, et al.: "Characterization of Novel Redox-Active Triruthenium(III)Complexes with a Disulfide-alky Ligand. Anion-dependent Redox Behavior of Monolayer Assemblies on Gold."Journal of the Chemical Society, Dalton Transactions. No.16. 2693-2701 (2000)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] Zhong-Ning Chen, et al.: "Chelate Formation around the Hexarhenium Cluster Center by a Diphosphane Ligand, Ph_2P(CH_2)_6PPh_2."Angewandte Chemie, International Edition in English. 40(No.1). 239-242 (2001)

    • Description
      「研究成果報告書概要(欧文)」より
  • [Publications] Akira Sato, et al.: "Cyclic Voltammetric Observation of CO/aqua Terminal Ligand Substitution Reactions for Trinuclear Ruthenium Complexes at Self-Assembled Monolayer Interfaces."Physical Chemistry Chemical Physics. (in press). (2001)

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

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Published: 2002-03-26  

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