Citation: JIANG Tao, WANG Ning, CHENG Chang-Ming, PENG Shu-Ming, YAN Liu-Ming. Molecular Dynamics Simulation on the Structure and Thermodynamics of Molten LiCl-KCl-CeCl₃[J]. Acta Physico-Chimica Sinica, ;2016, 32(3): 647-655. doi: 10.3866/PKU.WHXB201601042 shu

Molecular Dynamics Simulation on the Structure and Thermodynamics of Molten LiCl-KCl-CeCl₃

1.
1 Institute of Nuclear Physics and Chemistry, China Academy of Engineering Physics, Mianyang 621999, Sichuan Province, P. R. China;
2.
2 Department of Chemistry, College of Sciences, Shanghai University, Shanghai 200444, P. R. China

Corresponding author: PENG Shu-Ming,
Received Date: 28 October 2015
Available Online: 31 December 2015
Fund Project: 国家自然科学基金重大研究计划-集成项目(91426302) (91426302)国家自然科学基金(21301163)资助 (21301163)

The structure and thermodynamics of CeCl₃ in molten LiCl-KCl-CeCl₃ mixtures were studied by molecular dynamics simulation. The relationship formulas of temperature and density, and composition and density were obtained. The first peak for the g_Ce-Cl(r) radial distribution function was located at 0.259 nm and the corresponding first coordination number of Ce³⁺ was ~6.9. This inconsistency between molecular dynamics and experimental data could be attributed to the fact that our values were obtained for molten LiCl-KCl-CeCl₃ mixtures, in which the interaction between Ce³⁺ and Cl^- was more powerful than that in pure molten CeCl₃. Regarding self-diffusion coefficients, the activation energy of Ce³⁺ was 22.5 kJ·mol^-1, which is smaller than that of U³⁺ (25.8 kJ·mol^-1). Furthermore, the pre-exponential factors for Ce³⁺ decreased from 31.9×10^-5 to 21.8×10^-5 cm²·s^-1 as the molar fraction of Ce³⁺ increased from 0.005 to 0.05. This means that in the unit volume (ignoring the change of total volume), the diffusion resistance of Ce³⁺ increased, and the self-diffusion ability decreased, which resulted in a decrease of pre-exponential factors.
- LiCl-KCl-CeCl₃,
- Structure,
- Thermodynamics,
- Molecular dynamics,
- Diffusion coefficient
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Molecular Dynamics Simulation on the Structure and Thermodynamics of Molten LiCl-KCl-CeCl3

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Molecular Dynamics Simulation on the Structure and Thermodynamics of Molten LiCl-KCl-CeCl₃