Hydrophobic Water Probed Experimentally at the Gold Electrode/Aqueous Interface

作者：Yujin Tong, François Lapointe, Martin Thämer, Martin Wolf, R. Kramer Campen · 发表于：Angewandte Chemie International Edition · 年份：2017 · DOI：10.1002/anie.201612183 · 被引用次数：138 · 研究领域：Electrochemical Analysis and Applications、Spectroscopy and Quantum Chemical Studies、Electrocatalysts for Energy Conversion

Quantitative description of reaction mechanisms in aqueous phase electrochemistry requires experimental characterization of local water structure at the electrode/aqueous interface and its evolution with changing potential. Gaining such insight experimentally under electrochemical conditions is a formidable task. The potential-dependent structure of a subpopulation of interfacial water with one OH group pointing towards a gold working electrode is characterized using interface specific vibrational spectroscopy in a thin film electrochemical cell. Such free-OH groups are the molecular level observable of an extended hydrophobic interface. This free-OH interacts only weakly with the Au surface at all potentials, has an orientational distribution that narrows approaching the potential of zero charge, and disappears on oxidation of the gold electrode.