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利用飞行时间二次离子质谱和程序升温脱附研究了丙酮在 Ni(111)、表面修饰硅和非晶态水表面的吸附、扩散、去湿和捕获。

Adsorption, diffusion, dewetting, and entrapment of acetone on Ni(111), surface-modified silicon, and amorphous solid water studied by time-of-flight secondary ion mass spectrometry and temperature programmed desorption.

机构信息

International Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan.

出版信息

J Chem Phys. 2011 Oct 28;135(16):164703. doi: 10.1063/1.3656071.

Abstract

Interactions of acetone with the silicon surfaces terminated with hydrogen, hydroxyl, and perfluorocarbon are investigated; results are compared to those on amorphous solid water (ASW) to gain insights into the roles of hydrogen bonds in surface diffusion and hydration of acetone adspecies. The surface mobility of acetone occurs at ∼60 K irrespective of the surface functional groups. Cooperative diffusion of adspecies results in a 2D liquid phase on the H- and perfluorocarbon-terminated surfaces, whereas cooperativity tends to be quenched via hydrogen bonding on the OH-terminated surface, thereby forming residues that diffuse slowly on the surface after evaporation of the physisorbed species (i.e., 2D liquid). The interaction of acetone adspecies on the non-porous ASW surface resembles that on the OH-terminated Si surface, but the acetone molecules tend to be hydrated on the porous ASW film, as evidenced by their desorption during the glass-liquid transition and crystallization of water. The roles of micropores in hydration of acetone molecules are discussed from comparison with the results using mesoporous Si substrates.

摘要

研究了丙酮与氢终止、羟基终止和全氟碳终止的硅表面的相互作用;将结果与非晶态水(ASW)进行比较,以深入了解氢键在表面扩散和丙酮加合物水合作用中的作用。无论表面官能团如何,丙酮的表面迁移率都发生在约 60 K。加合物的协同扩散导致在 H 和全氟碳终止表面上形成 2D 液相,而氢键在 OH 终止表面上趋于猝灭,从而在物理吸附物种蒸发后在表面上形成缓慢扩散的残留物(即 2D 液体)。丙酮加合物在无孔 ASW 表面上的相互作用类似于在 OH 终止的 Si 表面上的相互作用,但丙酮分子在多孔 ASW 膜上倾向于水合,这可以通过它们在玻璃-液体转变期间的脱附和水的结晶来证明。通过与使用中孔 Si 衬底的结果进行比较,讨论了微孔在丙酮分子水合中的作用。

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