Phase diagrams and thermochemical modeling of salt lake brine systems. IV. Thermodynamic framework and program implementation for multicomponent systems
This paper is part of a series of studies on the development of a multi-temperature thermodynamically consistent model for salt lake brine systems. The objective of this study is to extend the binary thermodynamic models published in our previous studies to multicomponent systems. A revised general...
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| Abstract | This paper is part of a series of studies on the development of a multi-temperature thermodynamically consistent model for salt lake brine systems. The objective of this study is to extend the binary thermodynamic models published in our previous studies to multicomponent systems. A revised general Pitzer–Simonson–Clegg (PSC) gE,∗ equation for multicomponent system is proposed without limitation on the number of components. From the gE,∗ equation, mathematical expressions of the activity coefficient of each component as well as the excess enthalpy and excess heat capacity of the aqueous phase are derived. Based on the multicomponent PSC equations and the CALPHAD-type thermodynamic framework, a generic command-line based program, named ISLEC, was developed for the thermodynamic modeling of aqueous system. The performance of the model and program were tested using three case studies based on typical systems. In the first case study, a temperature-dependent model for a six-component system of Li+-Na+-K+-Mg2+-Ca2+-Cl--H2O was developed based our previous published binary models and the regressed mixing parameters developed in this study. The model well represents the phase equilibrium and activity properties of all 10 sub-ternary systems well over a wide temperature range. These ternary models are generally valid from the lowest eutectic temperature to approximately 373.15 K. For most of the studied ternary systems, the original PSC model is valid for solubility isotherm and phase diagram modeling. However, for the LiCl + KCl + H2O and KCl + CaCl 2+ H2O ternary systems, the revised PSC equations are advantageous in describing the solid-liquid phase equilibria, especially at elevated temperatures. Using the parameters determined in binary and ternary systems, the Li+-Na+-K+-Mg2+-Ca2+-Cl--H2O model system reproduces the phase diagrams of its 10 sub-quaternary and two of its sub-quinary systems (LiCl + NaCl + KCl + MgCl2+H2O and NaCl + KCl + MgCl2+CaCl2+H2O) generally well at various temperatures. However, the reliability of our model predictions of the thermal properties of multicomponent aqueous mixture cannot be assured, and the differences from experimental data are usually large. Thus, the thermal data generated from our model should be used with caution for multicomponent systems. The evaporation and cooling crystallization processes of Dead Sea brine, which is a six-component Li+–Na+–K+–Mg2+-Ca2+-Cl--H2O system, were simulated to test the ISLEC program. The results demonstrate the satisfactory performance of the ISLEC program for solving multiphase equilibria in systems containing at least six components. In the second case study, the PSC equations were applied to model the solubility isotherms in a neutral-solute-containing system: H3BO3+NaCl + H2O. The results are excellent, but additional H3BO3-containing systems should be studied for further validation. In the last case study, mass and energy balance simulations were performed for the process of KCl production using sylvinite as the raw material, thus revealing the applications of ISLEC for process design and simulation. |
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| AbstractList | This paper is part of a series of studies on the development of a multi-temperature thermodynamically consistent model for salt lake brine systems. The objective of this study is to extend the binary thermodynamic models published in our previous studies to multicomponent systems. A revised general Pitzer–Simonson–Clegg (PSC) gE,∗ equation for multicomponent system is proposed without limitation on the number of components. From the gE,∗ equation, mathematical expressions of the activity coefficient of each component as well as the excess enthalpy and excess heat capacity of the aqueous phase are derived. Based on the multicomponent PSC equations and the CALPHAD-type thermodynamic framework, a generic command-line based program, named ISLEC, was developed for the thermodynamic modeling of aqueous system. The performance of the model and program were tested using three case studies based on typical systems. In the first case study, a temperature-dependent model for a six-component system of Li+-Na+-K+-Mg2+-Ca2+-Cl--H2O was developed based our previous published binary models and the regressed mixing parameters developed in this study. The model well represents the phase equilibrium and activity properties of all 10 sub-ternary systems well over a wide temperature range. These ternary models are generally valid from the lowest eutectic temperature to approximately 373.15 K. For most of the studied ternary systems, the original PSC model is valid for solubility isotherm and phase diagram modeling. However, for the LiCl + KCl + H2O and KCl + CaCl 2+ H2O ternary systems, the revised PSC equations are advantageous in describing the solid-liquid phase equilibria, especially at elevated temperatures. Using the parameters determined in binary and ternary systems, the Li+-Na+-K+-Mg2+-Ca2+-Cl--H2O model system reproduces the phase diagrams of its 10 sub-quaternary and two of its sub-quinary systems (LiCl + NaCl + KCl + MgCl2+H2O and NaCl + KCl + MgCl2+CaCl2+H2O) generally well at various temperatures. However, the reliability of our model predictions of the thermal properties of multicomponent aqueous mixture cannot be assured, and the differences from experimental data are usually large. Thus, the thermal data generated from our model should be used with caution for multicomponent systems. The evaporation and cooling crystallization processes of Dead Sea brine, which is a six-component Li+–Na+–K+–Mg2+-Ca2+-Cl--H2O system, were simulated to test the ISLEC program. The results demonstrate the satisfactory performance of the ISLEC program for solving multiphase equilibria in systems containing at least six components. In the second case study, the PSC equations were applied to model the solubility isotherms in a neutral-solute-containing system: H3BO3+NaCl + H2O. The results are excellent, but additional H3BO3-containing systems should be studied for further validation. In the last case study, mass and energy balance simulations were performed for the process of KCl production using sylvinite as the raw material, thus revealing the applications of ISLEC for process design and simulation. This paper is part of a series of studies on the development of a multi-temperature thermodynamically consistent model for salt lake brine systems. The objective of this study is to extend the binary thermodynamic models published in our previous studies to multicomponent systems. A revised general Pitzer–Simonson–Clegg (PSC) gE,∗ equation for multicomponent system is proposed without limitation on the number of components. From the gE,∗ equation, mathematical expressions of the activity coefficient of each component as well as the excess enthalpy and excess heat capacity of the aqueous phase are derived. Based on the multicomponent PSC equations and the CALPHAD-type thermodynamic framework, a generic command-line based program, named ISLEC, was developed for the thermodynamic modeling of aqueous system. The performance of the model and program were tested using three case studies based on typical systems. In the first case study, a temperature-dependent model for a six-component system of Li+-Na+-K+-Mg2+-Ca2+-Cl--H2O was developed based our previous published binary models and the regressed mixing parameters developed in this study. The model well represents the phase equilibrium and activity properties of all 10 sub-ternary systems well over a wide temperature range. These ternary models are generally valid from the lowest eutectic temperature to approximately 373.15 K. For most of the studied ternary systems, the original PSC model is valid for solubility isotherm and phase diagram modeling. However, for the LiCl + KCl + H2O and KCl + CaCl 2+ H2O ternary systems, the revised PSC equations are advantageous in describing the solid-liquid phase equilibria, especially at elevated temperatures. Using the parameters determined in binary and ternary systems, the Li+-Na+-K+-Mg2+-Ca2+-Cl--H2O model system reproduces the phase diagrams of its 10 sub-quaternary and two of its sub-quinary systems (LiCl + NaCl + KCl + MgCl2+H2O and NaCl + KCl + MgCl2+CaCl2+H2O) generally well at various temperatures. However, the reliability of our model predictions of the thermal properties of multicomponent aqueous mixture cannot be assured, and the differences from experimental data are usually large. Thus, the thermal data generated from our model should be used with caution for multicomponent systems. The evaporation and cooling crystallization processes of Dead Sea brine, which is a six-component Li+–Na+–K+–Mg2+-Ca2+-Cl--H2O system, were simulated to test the ISLEC program. The results demonstrate the satisfactory performance of the ISLEC program for solving multiphase equilibria in systems containing at least six components. In the second case study, the PSC equations were applied to model the solubility isotherms in a neutral-solute-containing system: H3BO3+NaCl + H2O. The results are excellent, but additional H3BO3-containing systems should be studied for further validation. In the last case study, mass and energy balance simulations were performed for the process of KCl production using sylvinite as the raw material, thus revealing the applications of ISLEC for process design and simulation. |
| ArticleNumber | 101806 |
| Author | Yin, Xia Li, Dongdong Fan, Yanfei Zeng, Dewen Gao, Dandan |
| Author_xml | – sequence: 1 givenname: Dongdong surname: Li fullname: Li, Dongdong email: ddong_li@hotmail.com, lidongdong@isl.ac.cn organization: Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources, Qinghai Institute of Salt Lakes, Chinese Academy of Sciences, Xining 810008, PR China – sequence: 2 givenname: Dewen surname: Zeng fullname: Zeng, Dewen email: dewen_zeng@hotmail.com organization: Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources, Qinghai Institute of Salt Lakes, Chinese Academy of Sciences, Xining 810008, PR China – sequence: 3 givenname: Xia surname: Yin fullname: Yin, Xia organization: College of Chemistry and Chemical Engineering, Hunan University, Changsha 410082, PR China – sequence: 4 givenname: Dandan surname: Gao fullname: Gao, Dandan organization: Key Laboratory of Comprehensive and Highly Efficient Utilization of Salt Lake Resources, Qinghai Institute of Salt Lakes, Chinese Academy of Sciences, Xining 810008, PR China – sequence: 5 givenname: Yanfei surname: Fan fullname: Fan, Yanfei organization: College of Chemistry of Chemical Engineering, Central South University, Changsha 410083, PR China |
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| CitedBy_id | crossref_primary_10_1016_j_hydromet_2025_106517 crossref_primary_10_1038_s43247_022_00345_5 crossref_primary_10_1134_S0036023622601891 crossref_primary_10_1016_j_chemphys_2022_111538 crossref_primary_10_1007_s10953_021_01077_4 crossref_primary_10_3390_ma14144047 crossref_primary_10_1016_j_jct_2022_106763 crossref_primary_10_1016_j_gca_2024_02_001 crossref_primary_10_1021_acs_jced_5c00120 crossref_primary_10_3390_pr9030525 crossref_primary_10_1016_j_chemgeo_2023_121863 |
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| Keywords | Thermodynamic modeling Salt lake brine ISLEC Li+-Na+-K+-Mg2+-Ca2+-Cl--H2O system Revised pitzer–simonson–clegg equation |
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| SubjectTerms | Activity coefficients Brines Calcium chloride Calcium ions Case studies Crystallization Enthalpy Eutectic temperature Evaporative cooling High temperature ISLEC Isotherms Li+-Na+-K+-Mg2+-Ca2+-Cl--H2O system Liquid phases Lithium chloride Magnesium chloride Parameters Phase diagrams Phase equilibria Potassium chloride Quinary systems Revised pitzer–simonson–clegg equation Salt lake brine Salt lakes Simulation Solubility Temperature Temperature dependence Ternary systems Thermodynamic modeling Thermodynamic models Thermodynamic properties |
| Title | Phase diagrams and thermochemical modeling of salt lake brine systems. IV. Thermodynamic framework and program implementation for multicomponent systems |
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