Effect of water on carbonation of mineral aerosol surface models of kaolinite: a density functional theory study

摘要

Gas-solid interfacial phenomena always play a significant role in the multiphase process in atmospheric chemistry. The mineral aerosols have desirable interfacial reactivity on the carbonation of kaolinite. In addition, carbonation of kaolinite may play a role in carbon dioxide capture. It is not well-known about the mechanisms of this reaction. In this paper, the carbonation of kaolinite cluster models with or without water on the atomic scale is studied. We simulate the corresponding reaction paths and accurately calculate the transition states with the homologous enthalpies via using the density functional theory (DFT) method. The study shows that the reaction barriers are lowered down seriously with the existence of water. In addition, water can help stabilize the reaction regions thereby firming the structure of carbonated product.