Kinetic study of formic acid oxidation on Ti/IrO2 electrodes prepared using the spin coating deposition technique

Kinetic study of formic acid oxidation on Ti/IrO2 electrodes prepared using the spin coating deposition technique
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DOI:
10.1016/j.electacta.2010.06.066
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发表时间:
2010-09
影响因子:
6.6
通讯作者:
S. Fierro;C. Comninellis
S. Fierro;C. Comninellis
中科院分区:
材料科学2区
文献类型:
--
作者:
S. Fierro;C. Comninellis

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在本文的第一部分中,IrO 2电极由H2 IrCl 6前体的热分解产生的使用旋涂沉积技术,其中离心力传播的前体溶液的同时蒸发的溶剂在旋转的Ti基板上制造。有人发现,使用这种技术,它是可能的,以获得薄而均匀的IrO 2涂层与控制负载。采用伏安法电荷测量研究了前驱体溶液中铱盐浓度(c 0)以及衬底旋转速度(ω)对IrO 2负载量的影响。根据这些结果,提出了一个简单的关系式,用于估计给定c 0和ω的IrO 2负载。在本文的第二部分,并从使用不同的IrO 2负载量和甲酸浓度进行测量,甲酸的氧化的动力学参数已被定量确定使用的模型,涉及氧化还原对IrO 3/IrO 2作为介体的这个反应。利用所获得的动力学参数,结合Nernst方程和支持电解质(1 M HClO 4)的I-V曲线,可以得到不同甲酸浓度和不同IrO 2负载量下的理论I-V曲线。
In the first part of this paper, IrO2electrodes produced by thermal decomposition of H2IrCl6precursor were manufactured using the spin coating deposition technique, where centrifugal forces spread the precursor solution with simultaneous evaporation of the solvent on the rotating Ti substrate. It was found using this technique, that it is possible to obtain thin and uniform IrO2coatings with controlled loadings. The influence of the concentration of iridium salt in the precursor solution (c0) as well as the influence of the rotation speed at which the substrate spins (ω) on the IrO2loading have been studied using voltammetric charge measurements. From these results, a simple relation has been proposed for the estimation of the IrO2loading for a given c0and ω. In the second part of this paper and from measurements performed using different IrO2loadings and formic acid concentrations, the kinetic parameters of the oxidation of formic acid have been quantitatively determined using a model that involves the redox couple IrO3/IrO2as mediator of this reaction. Furthermore, using the kinetic parameters obtained together with the Nernst equation and the I–V curves of the supporting electrolyte (1M HClO4), theoretical I–V curves could be constructed for different concentrations of formic acid and different IrO2loadings.