Data underlying the publication: Laboratory-based in situ and operando tri-color X-ray photoelectron spectroscopy

Innovative approaches to study buried interfaces and heterogenous interactions under reaction conditions are crucial for advancing energy and catalytic materials. Our Near-Ambient Pressure X-ray Photoelectron Spectroscopy (NAP-XPS) setup is equipped with a novel tri-color X-ray source, with Al Kα, Ag Lα, and Cr Kα excitation energies, enabling information depth-selective operando and in situ analysis of solid-liquid, solid-gas, and solid-solid interfaces. We present three case studies to demonstrate the systems’ capabilities. First, we compare experimental depth profiling of a LaMnO3/LaFeO3/Nb:SrTiO3 multilayer with SESSA simulations. Second, we examine the oxidation and reduction of FexOy as a function of environment and temperature. Finally, the Pt/liquid electrolyte interface is examined, revealing surface oxidation in the absence of bulk oxidation. As our results confirm, the unique combination of a NAP-XPS with the novel tri-color X-ray source empowers laboratory-based in situ and operando XPS characterization of advanced materials under reaction conditions in a wide range of applications.

研究反应条件下掩埋界面与异质相互作用的创新方法，对推动能源与催化材料的发展至关重要。本团队搭建的近常压X射线光电子能谱（Near-Ambient Pressure X-ray Photoelectron Spectroscopy, NAP-XPS）装置搭载新型三色X射线源，激发能量覆盖Al Kα、Ag Lα与Cr Kα波段，可实现固-液、固-气及固-固界面的信息深度选择性原位及工况原位分析。本文展示三项案例研究以验证该系统的性能：其一，将LaMnO3/LaFeO3/Nb:SrTiO3多层膜的实验深度剖析结果与固体电子能谱与散射模拟（SESSA）的计算结果进行对比；其二，探究FexOy的氧化与还原过程随环境及温度的变化规律；其三，对Pt/液态电解质界面开展分析，发现其在本体未发生氧化的情况下出现了表面氧化现象。本研究结果证实，将NAP-XPS与新型三色X射线源相结合的独特方案，可支持实验室环境下，针对多种应用场景中反应条件下先进材料的原位及工况原位X射线光电子能谱表征。