Electrode kinetics of metal complexes confined in perfluoro polycarboxylate and polysulfonate coatings on graphite electrodes.
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概要
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A heterogeneous electron-transfer process of [Os(bpy)<SUB>3</SUB>]<SUP>2+⁄3+</SUP> (bpy: 2,2′-bipyridine) and [(trimethylammonio)methyl]ferrocene/ferricinium (TAF<SUP>+⁄2+</SUP>) redox couples, which were confined in perfluoro polycarboxylate and polysulfonate polyelectrolyte coatings on graphite electrodes, at the electrode/film interfaces as well as a homogeneous charge-transport process within the coating films were examined by means of potential-step chronoamperometry and chronocoulometry, normal pulse voltammetry and ac impedance measurements. The relevant kinetic parameters (i.e., the standard rate constant <I>k</I><SUP>°</SUP> and the transfer coefficient of the heterogeneous electron-transfer process and the apparent diffusion coefficient <I>D</I><SUB>app</SUB> for the homogeneous charge-transport process) were determined at various concentrations of the redox species in the films at various pH's. The temperature dependences of <I>D</I><SUB>app</SUB>, <I>k</I><SUP>°</SUP> and the formal potentials of the [Os(bpy)<SUB>3</SUB>]<SUP>2+⁄3+</SUP> and TAF<SUP>+⁄2+</SUP> couples confined in the films were also examined and the relevant activation parameters for the heterogeneous electron-transfer and homogeneous charge-transport processes and the reaction entropies of these redox couples were evaluated. On the basis of the kinetic and thermodynamic data obtained, the mechanism of the charge-transport process within the films, the effects of polymer domain and pH on the rates of the heterogeneous electron-transfer and homogeneous charge-transport processes and on the incorporation of the redox species into the films, etc. are discussed.
- 公益社団法人 日本化学会の論文
著者
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Oyama Noboru
Department Of Applied Chemistry Faculty Of Technology Tokyo University Of Agriculture And Technology
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Ohsaka Takeo
Department Of Applied Chemistry Faculty Of Technology Tokyo University Of Agriculture And Technology
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Sanpei Sachiko
Department of Chemistry, Japan Women's University
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Oyama Noboru
Department of Applied Chemistry for Resources, Tokyo University of Agriculture and Technology
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NAKAMURA Sadako
Department of Chemical and Biological Science, Faculty of Science, Japan Women's University
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Ushirogouchi Tooru
Department of Applied Chemistry for Resources, Tokyo University of Agriculture and Technology
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