Effects of supporting electrolyte and pH on charge transport within electropolymerized poly(o-phenylenediamine) films deposited on graphite electrodes.
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概要
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The homogeneous charge-transport process within electropolymerized electroactive poly(<I>o</I>-phenylenediamine) (PPD) films on graphite electrodes in various supporting electrolytic solutions (i.e., NaCl, NaClO<SUB>4</SUB>, Na<SUB>2</SUB>SO<SUB>4</SUB>, LiCl, CF<SUB>3</SUB>COONa, tetraethylammonium chloride (TEACl) and sodium <I>p</I>-toluenesulfonate (NaPTS)) at various pH's was examined by potential-step chronoamperometry and chronocoulometry. The overall charge-transport process was found to obey Fick's diffusion laws and thus the apparent diffusion coefficients (<I>D</I><SUB>app</SUB>) for the diffusion-like charge-transport process were estimated. The <I>D</I><SUB>app</SUB> values for the oxidation and reduction processes (i.e., <I>D</I><SUB>app</SUB><SUP>a</SUP> and <I>D</I><SUB>app</SUB><SUP>c</SUP>) were almost the same at pH 1.0 irrespective of the thickness of PPD films and were actually independent of the supporting electrolytes except for NaPTS. As pH was increased from 1 to 7, the <I>D</I><SUB>app</SUB><SUP>a</SUP> values decreased slightly from ca. 5.6×10<SUP>−8</SUP> to 1.6×10<SUP>−8</SUP> cm<SUP>2</SUP> s<SUP>−1</SUP> and the <I>D</I><SUB>app</SUB><SUP>c</SUP> values did more largely from ca. 5.6×10<SUP>−8</SUP> to 2.2×10<SUP>−9</SUP> cm<SUP>2</SUP> s<SUP>−1</SUP>. This behavior was essentially common to all the supporting electrolytes examined. Such pH dependences of <I>D</I><SUB>app</SUB><SUP>a</SUP> and <I>D</I><SUB>app</SUB><SUP>c</SUP> are discussed on the basis of the fact that the charge-transport process within PPD films involves the intrinsic electron-transfer process between adjacent electroactive sites as well as the proton addition–elimination process, the charge-compensating counterion motion, the motion of solvent and the segmental motion of the polymeric chain. Especially, it is demonstrated that in this system the proton addition–elimination process must necessarily occur in order for the charge-transport process to proceed.
- 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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Takahashi Katsuhiko
Department of Applied Chemistry for Resources, Tokyo University of Agriculture and Technology
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Chiba Kazuyuki
Department of Applied Chemistry for Resources, Tokyo University of Agriculture and Technology
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