Thermodynamic modeling and phase diagram prediction of salt lake brine systems II. Aqueous Li+-Na+-K+-SO42- and its subsystems

doi:10.1016/j.cjche.2020.11.040

Chinese Journal of Chemical Engineering ›› 2021, Vol. 34 ›› Issue (6): 134-149.DOI: 10.1016/j.cjche.2020.11.040

• Chemical Engineering Thermodynamics • Previous Articles Next Articles

Thermodynamic modeling and phase diagram prediction of salt lake brine systems II. Aqueous Li⁺-Na⁺-K⁺-SO₄^2- and its subsystems

Huan Zhou¹, Peng Wu², Wenxuan Li², Xingfan Wang², Kuo Zhou¹, Qing Hao¹

1 College of Chemical Engineering and Materials Science, Tianjin Key Laboratory of Brine Resources and Eco-utilization, Tianjin University of Science and Technology, Tianjin 300457, China;
2 College of Marine and Environmental Sciences, Tianjin Key Laboratory of Brine Resources and Eco-utilization, Tianjin University of Science and Technology, Tianjin 300457, China

Received:2020-04-30 Revised:2020-10-06 Online:2021-08-30 Published:2021-06-28
Contact: Huan Zhou
Supported by:
The authors gratefully thank the financial support of the National Natural Science Foundation of China (U1707602, U1407204) and also thank the Yangtze Scholars and Innovative Research Team in University of Education of China, the Innovative Research Team of Tianjin Municipal Education Commission (TD12-5004).

Thermodynamic modeling and phase diagram prediction of salt lake brine systems II. Aqueous Li⁺-Na⁺-K⁺-SO₄^2- and its subsystems

Huan Zhou¹, Peng Wu², Wenxuan Li², Xingfan Wang², Kuo Zhou¹, Qing Hao¹

1 College of Chemical Engineering and Materials Science, Tianjin Key Laboratory of Brine Resources and Eco-utilization, Tianjin University of Science and Technology, Tianjin 300457, China;
2 College of Marine and Environmental Sciences, Tianjin Key Laboratory of Brine Resources and Eco-utilization, Tianjin University of Science and Technology, Tianjin 300457, China

通讯作者: Huan Zhou
基金资助:
The authors gratefully thank the financial support of the National Natural Science Foundation of China (U1707602, U1407204) and also thank the Yangtze Scholars and Innovative Research Team in University of Education of China, the Innovative Research Team of Tianjin Municipal Education Commission (TD12-5004).

Abstract

Abstract: It is still a challenging task to accurately and temperature-continuously express the thermodynamic properties and phase equilibrium behaviors of the salt-lake brine with multi-component, multi-temperature and high concentration. The essential subsystem of sulfate type brine, aqueous Li⁺-Na⁺-K⁺-SO₄^2- and its subsystems across a temperature range from 250 K to 643 K are investigated with the improved comprehensive thermodynamic model. Liquid parameters (Δg_IJ, Δh_IJ, and ΔC_p,IJ) associated with the contributions of Gibbs energy, enthalpy, and heat capacity to the binary interaction parameters, i.e. the temperature coefficients of eNRTL parameters formulated with a Gibbs Helmholtz expression, are determined via multi-objective optimization method. The solid constants Δ_fG_k^°(298.15) and Δ_fH_k^°(298.15) of 11 solid species occurred in the quaternary system are rebuilt from multi-temperature solubilities. The modeling results show the accurate representation of (1) solution properties and binary phase diagram at temperature ranges from eutectic points to 643 K; (2) isothermal phase diagrams for Li₂SO₄-Na₂SO₄-H₂O, Li₂SO₄-K₂SO₄-H₂O and Na₂SO₄-K₂SO₄-H₂O ternary systems. The predicted results of complete structure and polythermal phase diagram of ternary systems and the isothermal phase diagrams of quaternary system excellently match with the experimental data.

Key words: Aqueous electrolytes, Comprehensive thermodynamic model, Aqueous Li⁺-Na⁺-K⁺-SO₄^2-, Phase diagram, Thermodynamic properties

摘要： It is still a challenging task to accurately and temperature-continuously express the thermodynamic properties and phase equilibrium behaviors of the salt-lake brine with multi-component, multi-temperature and high concentration. The essential subsystem of sulfate type brine, aqueous Li⁺-Na⁺-K⁺-SO₄^2- and its subsystems across a temperature range from 250 K to 643 K are investigated with the improved comprehensive thermodynamic model. Liquid parameters (Δg_IJ, Δh_IJ, and ΔC_p,IJ) associated with the contributions of Gibbs energy, enthalpy, and heat capacity to the binary interaction parameters, i.e. the temperature coefficients of eNRTL parameters formulated with a Gibbs Helmholtz expression, are determined via multi-objective optimization method. The solid constants Δ_fG_k^°(298.15) and Δ_fH_k^°(298.15) of 11 solid species occurred in the quaternary system are rebuilt from multi-temperature solubilities. The modeling results show the accurate representation of (1) solution properties and binary phase diagram at temperature ranges from eutectic points to 643 K; (2) isothermal phase diagrams for Li₂SO₄-Na₂SO₄-H₂O, Li₂SO₄-K₂SO₄-H₂O and Na₂SO₄-K₂SO₄-H₂O ternary systems. The predicted results of complete structure and polythermal phase diagram of ternary systems and the isothermal phase diagrams of quaternary system excellently match with the experimental data.

关键词: Aqueous electrolytes, Comprehensive thermodynamic model, Aqueous Li⁺-Na⁺-K⁺-SO₄^2-, Phase diagram, Thermodynamic properties

Huan Zhou, Peng Wu, Wenxuan Li, Xingfan Wang, Kuo Zhou, Qing Hao. Thermodynamic modeling and phase diagram prediction of salt lake brine systems II. Aqueous Li⁺-Na⁺-K⁺-SO₄^2- and its subsystems[J]. Chinese Journal of Chemical Engineering, 2021, 34(6): 134-149.

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Thermodynamic modeling and phase diagram prediction of salt lake brine systems II. Aqueous Li⁺-Na⁺-K⁺-SO₄^2- and its subsystems

Thermodynamic modeling and phase diagram prediction of salt lake brine systems II. Aqueous Li⁺-Na⁺-K⁺-SO₄^2- and its subsystems

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