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Empirical Analysis of the Photoelectrochemical Impedance Response of Hematite Photoanodes for Water Photo-oxidation
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2018-03-07 00:00:00 , DOI: 10.1021/acs.jpclett.8b00096
Dino Klotz 1, 2 , Daniel A. Grave 1 , Hen Dotan 1 , Avner Rothschild 1
Affiliation  

Photoelectrochemical impedance spectroscopy (PEIS) is a useful tool for the characterization of photoelectrodes for solar water splitting. However, the analysis of PEIS spectra often involves a priori assumptions that might bias the results. This work puts forward an empirical method that analyzes the distribution of relaxation times (DRT), obtained directly from the measured PEIS spectra of a model hematite photoanode. By following how the DRT evolves as a function of control parameters such as the applied potential and composition of the electrolyte solution, we obtain unbiased insights into the underlying mechanisms that shape the photocurrent. In a subsequent step, we fit the data to a process-oriented equivalent circuit model (ECM) whose makeup is derived from the DRT analysis in the first step. This yields consistent quantitative trends of the dominant polarization processes observed. Our observations reveal a common step for the photo-oxidation reactions of water and H2O2 in alkaline solution.

中文翻译:

赤铁矿光阳极对水光氧化的光电化学阻抗响应的经验分析

光电电化学阻抗谱(PEIS)是用于表征用于太阳能水分解的光电电极的有用工具。但是,PEIS光谱分析通常涉及先验可能会使结果产生偏差的假设。这项工作提出了一种经验方法,该方法可以分析松弛时间(DRT)的分布,松弛时间是直接从模型赤铁矿光电阳极的实测PEIS光谱中获得的。通过遵循DRT如何随控制参数(例如施加的电势和电解质溶液的组成)变化而变化,我们获得了对影响光电流的潜在机制的公正见解。在后续步骤中,我们将数据拟合到面向过程的等效电路模型(ECM),其组成是从第一步的DRT分析得出的。这产生了观察到的主要极化过程的一致的定量趋势。我们的观察结果揭示了水和H 2 O 2的光氧化反应的共同步骤 在碱性溶液中。
更新日期:2018-03-07
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