稀土卤化物与碱金属卤化物相图的热力学优化与计算
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摘要
本论文运用CALPHAD(Calculation of Phase Diagrams) 技术对NdCl_3—MCl (M=Li, Na, K, Rb, Cs)、LaBr_3—MBr (M=Na, K, Rb, Cs)、TmCl_3—MCl (M= Na, K, Rb, Cs)、DyCl_3-NaCl、LaF_3—NaF、YF_3-LiF 等十六体系的稀土与碱金属卤化物相图进行了系统的优化与计算。研究工作针对所优化计算体系强相互作用的特点,将最新发展的短程有序—扩展似化学模型合理应用于稀土卤化物熔盐体系相图优化计算中。在一些数据库基础上分步应用和编制计算程序,优化计算得到了与上述体系的热力学参数自洽的相图。其中应用短程有序—扩展似化学模型于三价稀土与碱金属溴、氟化物二元体系的相图进行系统的热力学优化具有创新性。
在整个优化过程中,根据体系相图数据与各种热力学参(函)数自洽的原理:首先选择和建立合理的热力学模型;接着将实验相图数据和其他热力学数据结合起来进行热力学优化和评估,再获得合理、可靠、自洽的所研体系的热力学描述。论文通过对计算结果和实验结果的比较,检验了部分实验相图和混合焓;优化预报了TmCl_3-MCl(M=Na, K, Rb, Cs)体系高温混合焓数据和LaF_3—NaF、YF_3-LiF 体系实验未完成部分的混合焓;获得了体系中间化合物的热力学函数。探讨了过剩热力学性质变化的规律和特征,总结了二元体系热力学参数混合焓的变化规律:一、碱金属卤化物与稀土卤化物构成的二元熔盐体系的混合焓数值随碱金属的半径的变大而减小;二、碱金属卤化物与稀土卤化物熔盐体系的混合焓相互作用系数最小值大约出现在稀土卤化物摩尔分数为0.25 处,显现强相互作用的短程有序特征。
By using CALPHAD (Calculation of Phase Diagrams) technique the optimization and calculation of the binary systems related to rare earth halide and the alkali metal one were carried out in this thesis. Due to the characters of stronger interactivities of those systems (NdCl_3—MCl (M=Li, Na, K, Rb, Cs), TmCl_3—MCl (M= Na, K, Rb, Cs), LaBr_3—MBr (M=Na, K, Rb, Cs), DyCl_3-NaCl, LaF_3—NaF, YF_3-LiF), the new modified quasichemical model in the pair-approximation for short-range ordering developed by Pelton et al. was used. And for the first time the model was applied to the systems of REB3-MB (RE=Rare Earth, M=Alkali metal, B=Bromide, Fluoride). The calculated phase diagrams and thermodynamic properties are self-consistent. Based on database and literature data, some basic computer programs were employed in the course of optimization and calculation.
According to the theory of self-consistence between thermodynamic parameters and phase diagrams, some thermodynamic models were chosen and constructed firstly. Then the measured phase equilibria data and experimental thermo-chemical properties were evaluated, at last the phase diagrams were optimized and described rationally. By comparing the calculated results and the experimental ones, we checked up some parts of experimental phase diagrams and mixing enthalpies in this work, and predicted completely mixing enthalpies of TmCl_3-MC(lM=Na, K, Rb, Cs)and parts of LaF_3—NaF, YF_3-LiF systems. Meanwhile the thermodynamic functions of some intermediate compounds were gotten. Further discussions about the calculated and experimental enthalpy of mixing in the systems were made: the enthalpy of mixing decreases with the increasing of the radius of alkali metal ion from Li~+ to Cs~+; moreover, the broad minimum values of the interactive coefficients were found at the 25% mole fraction of rare earths
halides, which represented the characters of short-range ordering.
在整个优化过程中,根据体系相图数据与各种热力学参(函)数自洽的原理:首先选择和建立合理的热力学模型;接着将实验相图数据和其他热力学数据结合起来进行热力学优化和评估,再获得合理、可靠、自洽的所研体系的热力学描述。论文通过对计算结果和实验结果的比较,检验了部分实验相图和混合焓;优化预报了TmCl_3-MCl(M=Na, K, Rb, Cs)体系高温混合焓数据和LaF_3—NaF、YF_3-LiF 体系实验未完成部分的混合焓;获得了体系中间化合物的热力学函数。探讨了过剩热力学性质变化的规律和特征,总结了二元体系热力学参数混合焓的变化规律:一、碱金属卤化物与稀土卤化物构成的二元熔盐体系的混合焓数值随碱金属的半径的变大而减小;二、碱金属卤化物与稀土卤化物熔盐体系的混合焓相互作用系数最小值大约出现在稀土卤化物摩尔分数为0.25 处,显现强相互作用的短程有序特征。
By using CALPHAD (Calculation of Phase Diagrams) technique the optimization and calculation of the binary systems related to rare earth halide and the alkali metal one were carried out in this thesis. Due to the characters of stronger interactivities of those systems (NdCl_3—MCl (M=Li, Na, K, Rb, Cs), TmCl_3—MCl (M= Na, K, Rb, Cs), LaBr_3—MBr (M=Na, K, Rb, Cs), DyCl_3-NaCl, LaF_3—NaF, YF_3-LiF), the new modified quasichemical model in the pair-approximation for short-range ordering developed by Pelton et al. was used. And for the first time the model was applied to the systems of REB3-MB (RE=Rare Earth, M=Alkali metal, B=Bromide, Fluoride). The calculated phase diagrams and thermodynamic properties are self-consistent. Based on database and literature data, some basic computer programs were employed in the course of optimization and calculation.
According to the theory of self-consistence between thermodynamic parameters and phase diagrams, some thermodynamic models were chosen and constructed firstly. Then the measured phase equilibria data and experimental thermo-chemical properties were evaluated, at last the phase diagrams were optimized and described rationally. By comparing the calculated results and the experimental ones, we checked up some parts of experimental phase diagrams and mixing enthalpies in this work, and predicted completely mixing enthalpies of TmCl_3-MC(lM=Na, K, Rb, Cs)and parts of LaF_3—NaF, YF_3-LiF systems. Meanwhile the thermodynamic functions of some intermediate compounds were gotten. Further discussions about the calculated and experimental enthalpy of mixing in the systems were made: the enthalpy of mixing decreases with the increasing of the radius of alkali metal ion from Li~+ to Cs~+; moreover, the broad minimum values of the interactive coefficients were found at the 25% mole fraction of rare earths
halides, which represented the characters of short-range ordering.
引文
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