Dynamic Fluctuation of U3+ Coordination Structure in the Molten LiCl–KCl Eutectic via First Principles Molecular Dynamics Simulations

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• 作者：Xuejiao Li ; Jia Song ; Shuping Shi ; Liuming YanZhaochun Zhang ; Tao Jiang ; Shuming Peng
• 刊名：Journal of Physical Chemistry A
• 出版年：2017
• 出版时间：January 26, 2017
• 年：2017
• 卷：121
• 期：3
• 页码：571-578
• 全文大小：473K
• ISSN：1520-5215

文摘

The dynamic fluctuation of the U³⁺ coordination structure in a molten LiCl–KCl mixture was studied using first principles molecular dynamics (FPMD) simulations. The radial distribution function, probability distribution of coordination numbers, fluctuation of coordination number and cage volume, self-diffusion coefficient and solvodynamic mean radius of U³⁺, dynamics of the nearest U–Cl distances, and van Hove function were evaluated. It was revealed that fast exchange of Cl^– occurred between the first and second coordination shells of U³⁺ accompanied with fast fluctuation of coordination number and rearrangement of coordination structure. It was concluded that 6-fold coordination structure dominated the coordination structure of U³⁺ in the molten LiCl–KCl–UCl₃ mixture and a high temperature was conducive to the formation of low coordinated structure.