分子动力学方法模拟不同温度下铀酰在叶腊石上的吸附和扩散行为

doi:10.3866/PKU.WHXB201705113

Abstract

Abstract:

In this study, molecular dynamics simulations were performed to gain insight into the adsorption and diffusion behavior of uranyl carbonate species on pyrophyllite basal surface at various temperatures (298.15, 313.15, and 333.15 K). At these temperatures, four kinds of uranium species, i.e. UO₂²⁺, UO₂CO₃, UO₂(CO₃) ₂²^-, UO₂(CO₃) ₃⁴^-, and uranyl oligomers were obtained. According to the atomic density profile of each uranyl species, only UO₂²⁺ and UO₂CO₃ were adsorbed on the pyrophyllite surface. Therefore, due to the strong coordination interaction between carbonate ion and uranyl, the pyrophyllite surface exhibited weak adsorption capacity for uranium after prolonged simulations. Self-diffusion coefficients of water molecules and uranyl species in both the adsorbed layer and the diffuse layer were calculated. With increasing temperature, the diffusion coefficients for all species increased; however, in the adsorbed layer, the diffusion coefficients for UO₂(CO₃) ₂²^- and UO₂(CO₃) ₃⁴^- increased faster than those for UO₂²⁺ and UO₂CO₃. Nonetheless, the diffuse order remained unchanged in both the layers: UO₂²⁺ > UO₂CO₃ > UO₂(CO₃) ₂²^- > UO₂(CO₃) ₃⁴^-. This indicates that UO₂²⁺ is the main diffusing species.

Key words: Pyrophyllite, Uranyl, Molecular dynamic simulation, Temperature, Adsorption, Diffusion

Tao-Na ZHANG,Xue-Wen XU,Liang DONG,Zhao-Yi TAN,Chun-Li LIU. Molecular Dynamics Simulations of Uranyl Species Adsorption and Diffusion Behavior on Pyrophyllite at Different Temperatures[J]. Acta Phys. -Chim. Sin. 2017, 33(10), 2013-2021. doi: 10.3866/PKU.WHXB201705113

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Molecular Dynamics Simulations of Uranyl Species Adsorption and Diffusion Behavior on Pyrophyllite at Different Temperatures

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