Charge-transfer rates in thin polyelectrolyte films incorporating a redox molecule with two separate electroactive centers having different redox potentials. An Alizarine Red S-cationic perfluoropolymer film system.
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概要
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The diffusion coefficients for the charge-transport processes through 9,10-dihydro-3,4-dihydroxy-9,10-dioxo-2-anthracenesulfonate (Alizarine Red S, <B>1</B>)-incorporating cationic perfluoropolymer (CPFP) polyelectrolyte films on electrodes undergoing oxidation or reduction of two separate electroactive centers with different redox potentials, i.e., the two-electron reduction of <B>1</B> to 3,4,9,10-tetrahydroxy-2-anthracenesulfonate (<B>2</B>) and the two-electron oxidations of <B>2</B> to <B>1</B> and <B>1</B> to 3,4,9,10-tetrahydro-3,4,9,10-tetraoxo-2-anthracenesulfonate ( <B>3</B>) were measured by potential-step chronoamperometry and chronocoulometry. The apparent diffusion coefficients for <B>1</B> to <B>2</B>, <B>2</B> to <B>1</B>, and <B>1</B> to <B>3</B> processes where the first two processes are reversible and the <B>1</B> to <B>3</B> process is irreversible, represented as <I>D</I><SUB>app</SUB><SUP>rev</SUP>(1→2), <I>D</I><SUB>app</SUB><SUP>rev</SUP>(2→1) and <I>D</I><SUB>app</SUB><SUP>irrrev</SUP> (1→3), respectively, decreased with increasing the concentration (<I>C</I><SUB>film</SUB>) of <B>1</B> (or <B>2</B>) in the CPFP film, and for a given <I>C</I><SUB>film</SUB> they were found to be in the following order: <I>D</I><SUB>s</SUB>′>><I>D</I><SUB>app</SUB><SUP>rev</SUP> (1→2)∼<I>D</I><SUB>app</SUB><SUP>rev</SUP>(2→1)><I>D</I><SUB>app</SUB><SUP>irrev</SUP> (1→3), where <I>D</I><SUB>s</SUB>′ represents the diffusion coefficients corresponding to the diffusion of supporting electrolyte ions coupled to electron transfer and molecular motion of reactant itself. It became apparent that the difference in <I>D</I><SUB>app</SUB><SUP>rev</SUP>(1→2) (or <I>D</I><SUB>app</SUB><SUP>rev</SUP>(2→1)) and <I>D</I><SUB>app</SUB><SUP>irrev</SUP> (1→3) can be attributed to different contributions of electron exchange between electroactive centers to the overall charge-transport rates. The results demonstrate that the contributions from molecular motion of reactant itself and electron exchange between reactants to the overall charge-transport rates can be estimated depending upon which redox center is employed in an electrochemical measurement of diffusional rates.
- 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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Hatozaki Osamu
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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Hatozaki Osamu
Department of Applied Chemistry for Resources, Tokyo University of Agriculture and Technology
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Oyama Noboru
Department of Applied Chemistry for Resources, Tokyo University of Agriculture and Technology
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Takahira Youko
Department of Applied Chemistry for Resources, Tokyo University of Agriculture and Technology
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