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| Journal Article | FZJ-2026-02354 |
; ; ; ; ;
2026
Elsevier Science
Amsterdam [u.a.]
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Please use a persistent id in citations: doi:10.1016/j.tca.2026.180317 doi:10.34734/FZJ-2026-02354
Abstract: This study aims to provide a comprehensive investigation of the reciprocal system Na+, Ca2+// Cl-, SO42- by integrating experimental analysis with thermodynamic modelling. The experimental approach involved the complementary use of Differential Thermal Analysis/Thermogravimetry (DTA/TG), Differential Scanning Calorimetry (DSC), and High-Temperature X-ray Diffraction (HT-XRD). These techniques provided essential experimental evidence for the phase equilibria description and served as a foundation for thermodynamic modelling. The reciprocal system was examined within the framework of phase change material (PCM) screening and identification for thermal energy storage applications. Based on the results obtained in this work, the thermodynamic database was developed for the aforementioned salt system. Notably, experimental findings highlighted significant modifications in the description of the binary system Na2SO4-CaSO4, namely the formation of the solid solution based on the high temperature modification of Na2SO4 and the identification of intermediate compounds Na4Ca(SO4)3, which replaces the previously assumed Na6Ca(SO4)4 compound. Additionally, while Na2Ca(SO4)2 had already been reported in prior studies, this work has provided a more precise definition of its thermal stability window, based on new experimental evidence. Furthermore, the experimental study of the NaCl-CaSO4 and CaCl2-Na2SO4 systems, representing the ionic exchange reaction, enabled a more detailed investigation of the reciprocal system, contributing to an improved thermodynamic description within the current database. This study reports, for the first time, the enthalpy of fusion of the eutectic composition in the NaCl-CaSO4 system, determined to be 39.3 ± 1.7 kJ/mol, with a corresponding melting temperature of 724 °C (997 K). Through the thermodynamic assessment of the sub-systems investigated both in this study and in previous works, an updated thermodynamic database has been developed, providing a comprehensive description of the entire reciprocal system and enabling a more accurate estimation of eutectic compositions within it. These findings enhance the accuracy of phase equilibria modelling and provide valuable insights into the thermal properties of potential PCM candidates.
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