DFT study of the carbonation on mineral aerosol surface models of olivine: effect of water

Mineral aerosols play a significant role in gas–solid interfacial and atmospheric chemistry. Carbonation of olivine aerosol, which takes place in a multiphase reaction processes, can be an effective means to reduce the concentration of atmospheric carbon dioxide. Due to the presence of a huge reserve of silicate minerals in nature, olivine aerosol could be an ideal potential raw material for mineral carbonation for its higher reactivity with H₂O and CO₂. However, quantitative information about the carbonation process on the surface of natural olivine aerosol is not available. In this paper, calculations on the carbonation reaction processes with and without a H₂O molecule using a periodic olivine model has been carried out via the density functional theory. The pathways and their corresponding energies and structures in the carbonation reactions have been established, and the effect of water as means to reduce the energy barriers and stabilize the carbonated structures by forming hydrogen bonds has been confirmed.