Potential-Dependent Adlayer Structure and Dynamics at the Ionic Liquid/Au(111) Interface: A Molecular-Scale In Situ Video-STM Study.

Potential-Dependent Adlayer Structure and Dynamics at the Ionic Liquid/Au(111) Interface: A Molecular-Scale In Situ Video-STM Study.
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DOI:
10.1002/anie.201501715
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发表时间:
2015-05
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影响因子:
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通讯作者:
R. Wen;Björn Rahn;O. Magnussen
R. Wen;Björn Rahn;O. Magnussen
中科院分区:
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文献类型:
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作者:
R. Wen;Björn Rahn;O. Magnussen

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室温离子液体在材料和能源科学中的电化学应用是当前研究的热点。了解这些系统的电化学反应性的关键是这些化合物和金属电极之间的界面的结构和动力学的详细数据,这与传统电解质中的界面明显不同。利用高速扫描隧道显微镜(video-STM)对Au(111)在1-丁基-1-甲基吡咯烷双(三氟甲基磺酰基)酰亚胺([BMP][TFSA])中的电极进行了原位研究。[BMP][TFSA]是最好理解的空气和水稳定的离子液体之一。测量提供了直接的洞察力的电位依赖的分子排列和表面动力学的吸附[BMP](+)阳离子在带负电荷的Au电极表面上的最内层。特别是,两个不同的后续过渡的吸附层结构和横向迁移率观察到降低的潜力。
Room-temperature ionic liquids are of great current interest for electrochemical applications in material and energy science. Essential for understanding the electrochemical reactivity of these systems are detailed data on the structure and dynamics of the interfaces between these compounds and metal electrodes, which distinctly differ from those in traditional electrolytes. In situ studies are presented of Au(111) electrodes in 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide ([BMP][TFSA]) by high-speed scanning tunneling microscopy (video-STM). [BMP][TFSA] is one of the best-understood air and water stable ionic liquids. The measurements provide direct insights into the potential-dependent molecular arrangement and surface dynamics of adsorbed [BMP](+) cations in the innermost layer on the negatively charged Au electrode surface. In particular, two distinct subsequent transitions in the adlayer structure and lateral mobility are observed with decreasing potential.