Publication date: 28th August 2024
Interfacial electric fields play a crucial role in facilitating various electrocatalytic processes. Understanding how these fields emerge from the structure of the electrochemical double layer (EDL), particularly the distribution of ions within the EDL, is essential. In this work, we address this challenge by employing multiple vibrational spectroscopic reporters, which enabled us to simultaneously measure the accumulation of cations in the EDL and the resulting electric field. Specifically, we employed surface-enhanced infrared absorption spectroscopy (SEIRAS) to investigate the accumulation of an infrared-active organic cation, tetramethylammonium, at the aqueous electrolyte/polycrystalline gold (Au) interface as the electrode potential decreases. Additionally, we used vibrational Stark spectroscopy to monitor the resulting interfacial electric field by examining the CO stretch of surface-adsorbed CO. Our findings show a structural change in the EDL at -0.7 V versus the Ag/AgCl electrode. This potential coincides with a change in the Stark tuning slope of the CO stretch, indicating that the structural change in the EDL enhances the interfacial electric field. We will discuss the implications of this finding for electrocatalysis. This study further illustrates how multiple vibrational reporters can be leveraged to gain insights into the connection between interfacial structure and the resulting electric field at catalytic sites.
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