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

• Published in: Environmental earth sciences 2017-11, Vol.76 (21), p.1-8, Article 732
• Main Authors: Xie, Heping, Jiang, Wen, Hou, Zhengmeng, Xue, Ying, Wang, Yufei, Liu, Tao, Tang, Liang, Wu, Dinglu
• Format: Article
• Language: English
• Subjects: Aerosol effects; Aerosols; Atmospheric chemistry; Atmospheric models; Barriers; Biogeosciences; Carbon dioxide; Carbon dioxide atmospheric concentrations; Carbon dioxide concentration; Carbonation; Chemical bonds; Density functional theory; Earth and Environmental Science; Earth Sciences; Environmental Science and Engineering; Geochemistry; Geology; Hydrogen; Hydrogen bonding; Hydrogen bonds; Hydrology/Water Resources; Information processing; Minerals; Olivine; Original Article; Raw materials; Silicate minerals; Silicates; Structures; Terrestrial Pollution
• ISSN: 1866-6280; 1866-6299
• DOI: 10.1007/s12665-017-6988-8

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 H 2 O and CO 2 . 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 H 2 O 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.