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首页> 外文期刊>Electroanalysis >Identification and electroanalytical characterization of redox transitions in solid-state Keggin type phosphomolybdic acid
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Identification and electroanalytical characterization of redox transitions in solid-state Keggin type phosphomolybdic acid

机译：固态Keggin型磷钼酸中氧化还原转变的鉴定和电分析特性

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摘要

The tetragonal single crystal, H(3)PMo(12)O(40)center dot 29H(2)O, is considered here as a model system to describe multielectron redox reactions of Keggin type phosphododecamolybdate. Electrochemical experiments have been performed in solid-state, i.e. in the absence of contact with liquid electrolyte phase, and they have utilized a gold wire ultramicrodisk (diameter: 10 mu m) working electrode, a silver disk quasireference electrode, and a glassy carbon counter electrode within all solid cell. The results of voltammetric measurements are explained and verified against the simulated data. The reversible redox reactions of phosphododecamolybdic acid (H3PMo12O40 center dot 29H(2)O) single crystal, that appear at most positive potentials, can be understood in terms of two overlapping one-electron redox processes (separated by only approximate to 50 mV), rather than a single two-electron redox transition, followed by another one-electron process. Comparison is made to the conventional electrochemical behavior of phosphododecamolybdate in solution (0.5 mol dm(-3) H2SO4) as well as to the characteristic of its adsorbate on the electrode surface. The following parameters have been determined from the combination of potential step experiments performed in two limiting (radial and linear) diffusional regimes: the concentration of heteropolymolybdate redox centers, 1.4 mol dm(-3), and the apparent diffusion coefficient for charge propagation, 3.6 x 10(-7) cm(2) s(-1). The result supports the concept of the kinetic control of charge transport by electron hopping (self-exchange) between mixed-valence (Mo-VI/Mo-V) sites.
机译：四方单晶H（3）PMo（12）O（40）中心点29H（2）O在这里被视为描述Keggin型磷酸十二钼酸多电子氧化还原反应的模型系统。电化学实验是在固态下进行的，即在不与液态电解质相接触的情况下进行，他们利用了金线超微盘（直径：10μm）工作电极，银盘准参比电极和玻璃碳计数器。所有固态电池中的电极。解释了伏安测量的结果，并对照模拟数据进行了验证。磷十二烷钼酸（H3PMo12O40中心点29H（2）O）单晶的可逆氧化还原反应最多出现正电位，这可以通过两个重叠的单电子氧化还原过程（仅相隔约50 mV）来理解，而不是单一的两个电子的氧化还原跃迁，然后是另一个单一的电子过程。比较了十二烷基钼酸磷在溶液（0.5 mol dm（-3）H2SO4）中的常规电化学行为，以及在电极表面吸附的特性。根据在两个极限（径向和线性）扩散方案中进行的潜在步骤实验的组合，确定了以下参数：杂多钼酸盐氧化还原中心的浓度为1.4 mol dm（-3），电荷扩散的表观扩散系数为3.6 x 10（-7）cm（2）s（-1）。结果支持了通过混合价（Mo-VI / Mo-V）位之间的电子跳跃（自交换）来动态控制电荷传输的概念。

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