In many industrial applications as well as in nature, the mass transfer of CO2 at vapor-liquid interfaces in aqueous systems plays an important role. In this work, this process was studied on the atomistic level using non-equilibrium molecular dynamics simulations. In a first step, a molecular model of the system water + CO2 was developed that represents both bulk and interfacial equilibrium properties well. This system is characterized by a very large adsorption and enrichment of CO2 at the vapor-liquid interface. Then, non-equilibrium mass transfer simulations were carried out using a method that was developed recently: CO2 is inserted into the vapor phase of a simulation box which contains a liquid slab. Surprising effects are observed at the interface such as a net repulsion of CO2 particles from the interface and a complex time dependence of the amount of CO2 adsorbed at the interface.

中文翻译：

---

通过分子动力学模拟研究 H2O + CO2 混合物汽液界面的传质


在许多工业应用以及自然界中，CO2 在水系统中汽液界面的传质起着重要作用。在这项工作中，利用非平衡分子动力学模拟在原子水平上研究了这一过程。第一步，开发了水 + CO2 系统的分子模型，该模型很好地代表了体积和界面平衡特性。该系统的特点是在气液界面对CO2有非常大的吸附和富集。然后，使用最近开发的方法进行非平衡传质模拟：将CO2注入包含液体板的模拟箱的气相中。在界面处观察到令人惊讶的效应，例如界面上 CO2 颗粒的净排斥以及界面处吸附的 CO2 量的复杂时间依赖性。