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A fast regression model for the interpretation of electrochemical impedance spectra of intermediate temperature solid oxide fuel cells
Journal of Electroanalytical Chemistry ( IF 4.1 ) Pub Date : 2018-08-01 , DOI: 10.1016/j.jelechem.2018.06.037
Simone Campanella , Mauro Bracconi , Alessandro Donazzi

Abstract A frequency domain transformation method is applied to a physically consistent model of an IT-SOFC with MIEC electrolyte. Fast computation of the impedance spectra is achieved, which allows to apply the model to kinetic studies using traditional regressive techniques. The model includes conservation equations of mass and charge, gas diffusive transport effects and leakage current effects due to the semiconductor electrolyte. Global rate equations for the electrocatalytic semi-reactions guarantee economy of calibrated parameters. Two sets of impedance experiments collected on electrolyte-supported Cu-Pd-CZ80-SDC/SDC/LSCF-GDC cells are analyzed. The description of the H2 oxidation process is improved based on experiments with H2/N2 mixtures at fixed temperature and increasing H2 molar fraction (700 °C, 30–100% H2). The introduction of constant phase elements proves essential to closely predict Nyquist and Bode plots: strong inhomogeneity of the anode structure emerges, while the cathodic determining process is better identified via refinement of the double layer capacitance. Novel impedance experiments, performed with a CO-rich mixture (97% CO, 3% CO2) between 600 °C and 700 °C, allow to estimate the kinetic constant for CO electro-oxidation. The variation of the CPE parameters suggests that carbon deposition during exposure to CO simultaneously reduces the anodic active area and double layer capacitance.

中文翻译:

用于解释中温固体氧化物燃料电池电化学阻抗谱的快速回归模型

摘要 将频域变换方法应用于具有MIEC电解质的IT-SOFC物理一致性模型。实现了阻抗谱的快速计算,这允许使用传统的回归技术将该模型应用于动力学研究。该模型包括质量和电荷守恒方程、气体扩散传输效应和半导体电解质引起的漏电流效应。电催化半反应的全局速率方程保证校准参数的经济性。分析了在电解质支持的 Cu-Pd-CZ80-SDC/SDC/LSCF-GDC 电池上收集的两组阻抗实验。基于在固定温度下使用 H2/N2 混合物和增加 H2 摩尔分数(700 °C,30-100% H2)的实验改进了 H2 氧化过程的描述。恒定相位元素的引入证明对于密切预测 Nyquist 和 Bode 图是必不可少的:阳极结构出现了强烈的不均匀性,而阴极确定过程可以通过双电层电容的细化更好地识别。在 600 °C 和 700 °C 之间使用富含 CO 的混合物(97% CO,3% CO2)进行的新型阻抗实验允许估计 CO 电氧化的动力学常数。CPE 参数的变化表明,暴露于 CO 期间的碳沉积同时降低了阳极活性面积和双层电容。在 600 °C 和 700 °C 之间使用富含 CO 的混合物(97% CO,3% CO2)进行的新型阻抗实验允许估计 CO 电氧化的动力学常数。CPE 参数的变化表明,暴露于 CO 期间的碳沉积同时降低了阳极活性面积和双层电容。在 600 °C 和 700 °C 之间使用富含 CO 的混合物(97% CO,3% CO2)进行的新型阻抗实验允许估计 CO 电氧化的动力学常数。CPE 参数的变化表明,暴露于 CO 期间的碳沉积同时降低了阳极活性面积和双层电容。
更新日期:2018-08-01
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