Christoph Griesser, Daniel Winkler, Toni Moser, Leander Haug, Marco Thaler, Engelbert Portenkirchner, Bernhard Klötzer, Sergio Diaz-Coello, Elena Pastor, Julia Kunze-Liebhäuser
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引用次数: 0
Abstract
A profound understanding of the solid/liquid interface is central in electrochemistry and electrocatalysis, as the interfacial properties ultimately determine the electro-reactivity of a system. Although numerous electrochemical methods exist to characterize this interface under operating conditions, tools for the in-situ observation of the surface chemistry, that is, chemical composition and oxidation state, are still scarce, and currently exclusively available at synchrotron facilities. Here, we demonstrate the ability of laboratory-based near-ambient pressure X-ray photoelectron spectroscopy to track changes in oxidation states in-situ with respect to the applied potential. In this proof-of-principle study with polycrystalline gold (Au) as the best-studied electrochemical standard, we show that during the oxygen evolution reaction (OER), at high OER overpotentials, Au3+ governs the interfacial chemistry, while, at lower overpotentials, Au+ dominates.
深刻理解固/液界面是电化学和电催化的核心,因为界面特性最终决定了系统的电反应性。虽然有许多电化学方法可以表征工作条件下的这种界面,但用于原位观察表面化学(即化学成分和氧化态)的工具仍然很少,而且目前只能在同步加速器设施中获得。在这里,我们展示了基于实验室的近环境压力 X 射线光电子能谱仪跟踪氧化态随应用电势原位变化的能力。在这项以多晶金(Au)为最佳电化学标准的原理验证研究中,我们发现在氧进化反应(OER)过程中,在高 OER 过电位时,Au3+ 主导界面化学,而在较低的过电位时,Au+ 占主导地位。