Mass transfer at vapor-liquid interfaces of H₂O + CO₂ mixtures studied by molecular dynamics simulation

In many industrial applications as well as in nature, the mass transfer of CO 2 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 + CO 2 was developed that represents both bulk and interfacial equilibrium properties well. This system is characterized by a very large adsorption and enrichment of CO 2 at the vapor-liquid interface. Then, non-equilibrium mass transfer simulations were carried out using a method that was developed recently: CO 2 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 CO 2 particles from the interface and a complex time dependence of the amount of CO 2 adsorbed at the interface.