论文标题
赤铁矿光抗水光氧化的光电化学阻抗反应的经验分析
Empirical Analysis of the Photoelectrochemical Impedance Response of Hematite Photoanodes for Water Photo-Oxidation
论文作者
论文摘要
光电化学阻抗光谱(PEIS)是用于表征用于太阳能分裂的光电极的有用工具。但是,对PEIS光谱的分析通常涉及可能偏向结果的先验假设。这项工作提出了一种经验方法,该方法分析了直接从模型赤铁矿光阳极的测量的PEIS光谱获得的弛豫时间(DRT)的分布。通过遵循DRT如何演变为控制参数的函数,例如电解质溶液的施加势和组成,我们获得了对塑造光电流的基本机制的无偏见。在随后的步骤中,我们将数据拟合到面向过程的等效电路模型(ECM),该电路模型(ECM)在第一步中源自DRT分析。这产生了观察到的主要极化过程的一致定量趋势。我们的观察结果揭示了碱性溶液中水和H2O2的光氧化反应的共同步骤
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