Stubkjær Rasmus Baden, Kløve Magnus, Bertelsen Andreas, Borup Anders Bæk, Roelsgaard Martin, Iversen Bo Brummerstedt
Department of Chemistry and Interdisciplinary Nanoscience Center (iNANO) Aarhus University Langelandsgade 140 Aarhus8000-DK Denmark.
J Appl Crystallogr. 2025 Mar 19;58(Pt 2):495-503. doi: 10.1107/S1600576725001694. eCollection 2025 Apr 1.
and pair distribution function (PDF) studies are becoming commonly used to study chemical reactions, nucleation and growth of nanoparticles, or structural changes during the operation of batteries, catalysts, thermoelectric devices However, repeated time-resolved total scattering experiments and subsequent PDF analysis are often not prioritized due to the scarce synchrotron beam time available. This means that the experimental uncertainty and reproducibility of the experimental methods are unknown, and the full potential of PDF experiments may not be exploited. Here, we quantify the experimental uncertainty of the PDF technique in an study of the hydro-thermal synthesis of ZrO nanoparticles. Systematic variation of the parameters used to obtain the PDF shows that the user-defined parameters can potentially affect the chemical conclusions obtained from the time-resolved experiment. We found that comparable results are best obtained using the same input parameters across different experiments. We also compare different PDF algorithms to examine whether the processing algorithm influences the chemical analysis.
对分布函数（PDF）研究正越来越普遍地用于研究化学反应、纳米颗粒的成核与生长，或电池、催化剂、热电器件运行过程中的结构变化。然而，由于同步加速器束流时间稀缺，重复的时间分辨全散射实验及后续的PDF分析往往未被优先考虑。这意味着实验方法的实验不确定性和可重复性未知，且PDF实验的全部潜力可能未得到充分利用。在此，我们在一项关于ZrO纳米颗粒水热合成的研究中量化了PDF技术的实验不确定性。用于获取PDF的参数的系统变化表明，用户定义的参数可能会影响从时间分辨实验得出的化学结论。我们发现，在不同实验中使用相同的输入参数能最好地获得可比结果。我们还比较了不同的PDF算法，以研究处理算法是否会影响化学分析。
