Université de Lyon, CNRS, Ecole Normale Supérieure de Lyon, Institut de Chimie de Lyon, Laboratoire de Chimie, 46 Allée d'Italie, F-69364 Lyon Cedex 07, France.
Phys Chem Chem Phys. 2011 Jul 7;13(25):11827-37. doi: 10.1039/c0cp02285c. Epub 2011 Feb 22.
Understanding the nature of the adhesion of an organic liquid on a metal surface is of paramount importance for elucidating the stability and chemical reactivity at these complex interfaces. However, to date, the morphology, layering and chemical properties at organic liquid metal interfaces have been rarely known. Using semi-empirical dispersion corrected density functional theory calculations and ab initio molecular dynamics simulations, we show that carbon tetrachloride and ethanol films confined to a platinum surface alter their intrinsic properties and exhibit interfacial reactivity. A few interface carbon tetrachloride (ethanol) molecules adsorb dissociatively (molecularly) on platinum thanks to the surrounding medium. The adsorption strength of the interfacial molecules is consequently increased in the condensed phase as compared to the gas phase. This remarkable effect is rationalized by an interaction energy decomposition model and an electrostatic potential analysis.
理解有机液体在金属表面的附着性质对于阐明这些复杂界面的稳定性和化学反应性至关重要。然而,迄今为止,有机液体-金属界面的形态、分层和化学性质还知之甚少。使用半经验色散修正密度泛函理论计算和从头分子动力学模拟,我们表明,四氯化碳和乙醇薄膜被限制在铂表面会改变它们的固有性质,并表现出界面反应性。由于周围介质的存在,一些界面四氯化碳(乙醇)分子在铂上发生离解(分子)吸附。与气相相比,凝聚相中界面分子的吸附强度因此增加。这种显著的效应可以通过相互作用能分解模型和静电势分析来合理化。