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首页> 外文期刊>The journal of physical chemistry, C. Nanomaterials and interfaces >Spontaneously Formed Sulfur Adlayers on Gold in Electrolyte Solutions: Adsorbed Sulfur or Gold Sulfide?
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Spontaneously Formed Sulfur Adlayers on Gold in Electrolyte Solutions: Adsorbed Sulfur or Gold Sulfide?

机译：在电解液中的金上自发形成的硫层：吸附的硫还是硫化金？

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摘要

High coverage S phases (surface coverage >0.33), spontaneously formed by immersion of Au(111) in Na2S aqueous solutions at room temperature, have been studied by scanning tunneling microscopy (STM), X-ray photoelectron spectroscopy (XPS), surface enhanced Raman spectroscopy (SERS), electrochemistry, and density functional theory (DFT) calculations. XPS data show no evidence of a AuS phase, as no oxidized gold is detected. Voltammetric data are also inconsistent with the formation of a AuS phase with 0.5 stoichiometry. In situ and ex situ SERS measurements of S-covered nanostructured gold substrates demonstrate that the surface species present at the gold surface consist of a mixture of chemisorbed S and polysulrlde species, as already proposed based on in situ STM images. A DFT surface model that is energetically feasible and reproduces well the experimental STM images is presented. The proposed model involves only a small rearrangement of the upper Au layer and coexistence of monomeric and polymeric S. Therefore, the high coverage S phase should be described as a mixture of monomeric and polymeric chemisorbed sulfur rather than as an extended 2D AuS phase.
机译：通过扫描隧道显微镜（STM），X射线光电子能谱（XPS），表面增强技术研究了室温下Au（111）浸入Na2S水溶液中自发形成的高覆盖率S相（表面覆盖率> 0.33）。拉曼光谱（SERS），电化学和密度泛函理论（DFT）计算。 XPS数据显示没有AuS相的迹象，因为未检测到氧化金。伏安数据也与化学计量比为0.5的AuS相的形成不一致。 S覆盖的纳米结构金基底的原位和异位SERS测量表明，存在于金表面的表面物种由化学吸附的S和多硫化物物种的混合物组成，这已基于原位STM图像提出。提出了一种在能量上可行并且可以很好地再现实验STM图像的DFT表面模型。所提出的模型仅涉及上层Au层的少量重排以及单体和聚合物S的共存。因此，高覆盖率S相应描述为单体和聚合物化学吸附硫的混合物，而不是扩展的2D AuS相。

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