First-principles study on the adsorption structure of water molecules on a pyrite (100) surface
Yingchao Liu, Jianhua Chen, Yuqiong Li, Junjie Zhang, Duan Kang
Abstract
The hydration structure of water molecule adsorption at different coverages of a monolayer on a pyrite (100) surface were simulated using the density functional theory (DFT) method. The results demonstrate that the Fe-O interaction weakens and the adsorption energy per water molecule decreases with increasing water coverage, except at a monolayer coverage of 12/12 (i.e., full coverage). H-S and H-O hydrogen bonds were formed on the nearest surface layer. When large amounts of water molecules adsorb onto the surface, the adsorbed water molecules can be divided into three layers: the layer nearest to the surface, the second nearest to the surface, and the layer farthest from the surface. The thickness of the former two layers is approximately 5.5 . The three layers have water densities of 1.12 g/cm3, 1.08 g/cm3, and 0.95 g/cm3, respectively, suggesting that there is a strong interaction between the pyrite surface and water molecules and the influence of surface structure on water adsorption reaches a distance of more than 10 . Dynamics simulations suggest that the water molecules close to the mineral surfaces are in an orderly arrangement while those far from the surface are disordered.