journal article·2022-05

Development of the Molten Salt Thermal Properties Database − Thermochemical (MSTDB−TC), example applications, and LiCl−RbCl and UF3−UF4 system assessments

Johnathon C. Ard, Jacob A. Yingling, Tristan J. Johnson, Juliano Schorne-Pinto, Mina Aziziha, Clara M. Dixon, Matthew S. Christian, Jacob W. McMurray, Theodore M. Besmann

Publisher page

Abstract

The Molten Salt Thermal Properties Database − Thermochemical ( MSTDB−TC ) has been developed to support thermodynamic modeling of fluoride- and chloride-based systems for molten salt reactors (MSRs). Utilizing data from available literature and original work, the current MSTDB−TC Ver. 1.2 contains models for 96 pseudo-binary systems, 37 pseudo-ternary systems, 42 solid solutions, 229 stoichiometric compounds, and 130 gaseous species. This includes 67 reassessed systems and 13 original system models. The reassessment of the LiCl−RbCl pseudo-binary system and the original assessment of the UF 3−UF 4 pseudo-binary system are included as examples of those efforts and provide improved representations of those systems. The database continues to be expanded, adding systems of relevance to the wide variety of MSR concepts. To illustrate applications for MSTDB−TC, phase equilibria were computed to understand the effect of varying uranium content in the KCl−MgCl 2−NaCl−UCl 3 system. In an example of how such calculations can support corrosion modeling, the control of redox potential by the UF 3:UF 4 ratio in the LiF−BeF 2−UF 3−UF 4 system is demonstrated and used to assess corrosion potential for typical alloy constituents.
Source: expertdata · Quality: candidate unverified · Source record ↗

Research context

OpenAlex topics: Metallurgical Processes and Thermodynamics · Molten salt chemistry and electrochemical processes · Nuclear Materials and Properties

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (95)

Show source-provided references
1. Williams, Technology and Applied R&D for Molten Salt Chemistry, Molten Salt Chemistry Workshop, 2017.
2. A workflow leveraging MOOSE transient multiphysics simulations to evaluate the impact of thermophysical property uncertainties on molten-salt reactors10.1016/j.anucene.2021.108546 ↗
3. Application of NEAMS Codes to Capture MSR Phenomena
4. Engineering scale molten salt corrosion and chemistry code development
5. FactSage thermochemical software and databases, 2010-201610.1016/j.calphad.2016.05.002 ↗
6. The thermochemistry library thermochimica10.1016/j.commatsci.2012.09.011 ↗
7. Saunders · 1998
8. Models for the thermodynamic properties of molten salt systems: perspectives for ionic liquids10.1016/j.fluid.2015.10.031 ↗
9. Pelton · 2018
10. G.N. Haidemenopoulos, Physical Metallurgy: Principles and Design, CNC Press2018, pp. 96–101.10.1201/9781315211220 ↗
11. Rankin · 2019
12. The compound energy formalism10.1016/S0925-8388(00)01481-X ↗
13. Thermodynamic assessment of the LiF-NaF-BeF2-ThF4-UF4 system10.1016/j.jnucmat.2014.03.009 ↗
14. Redlich · Industrial Engineering Chemistry · 1948 · 34510.1021/ie50458a036 ↗
15. The modified quasi-chemical model: part IV. Two-sublattice quadruplet approximation10.1007/s11661-001-0230-7 ↗
16. The modified quasichemical model I - Binary solutions10.1007/s11663-000-0103-2 ↗
17. The modified quasi-chemical model: part II. Multicomponent solutions10.1007/s11661-001-0226-3 ↗
18. The modified quasi-chemical model: Part III. Two sublattices10.1007/s11661-001-0229-0 ↗
19. Molecular dynamics investigation on the local structures and transport properties of uranium ion in LiCl-KCl molten salt10.1016/j.jnucmat.2018.08.052 ↗
20. Dynamic fluctuation of U3+ coordination structure in the molten LiCl-KCl eutectic via first principles molecular dynamics simulations10.1021/acs.jpca.6b10193 ↗
21. Local coordination about La3+ in molten LaCl3 and its mixtures with alkali chlorides10.1021/jp910637p ↗
22. Coordination numbers and physical properties in molten salts and their mixtures10.1039/C5FD00223K ↗
23. Modelling of structure and dynamics of molten NaF using first principles molecular dynamics
24. Overcoming the limitations of cutoffs for defining atomic coordination in multicomponent systems10.1002/jcc.25137 ↗
25. Static and dynamic structure of Pu3+ in molten LiCl-KCl eutectic revealed by first-principles molecular dynamics simulations10.1080/08927022.2018.1506118 ↗
26. Structural investigation of thorium in molten lithium-calcium fluoride mixtures for salt treatment process in molten salt reactor10.1016/j.pnucene.2011.04.026 ↗
27. A new approach for coupled modelling of the structural and thermo-physical properties of molten salts. Case of a polymeric liquid LiF-BeF210.1016/j.molliq.2019.112165 ↗
28. New insights and coupled modelling of the structural and thermodynamic properties of the LiF-UF4 system10.1016/j.molliq.2021.115820 ↗
29. Examination of the short-range structure of molten salts: ThF4, UF4, and related alkali actinide fluoride systems10.1039/D1CP00566A ↗
30. A predictive thermodynamic model for the Al-NaF-AiF3-CaF2-Al2O3 system
31. A thermodynamic database for AlCl3-based molten salt systems
32. Thermodynamic evaluation and optimization of the (NaCl+KCl+AlCl3) system10.1016/j.jct.2004.04.011 ↗
33. Thermodynamic evaluation and optimization of the (NaF + AlF3 + CaF2 + BeF2 + Al2O3 + BeO) system10.1016/j.jct.2012.09.005 ↗
34. Grimvall · 1999
35. Thermodynamics of uranium tri-iodide from density-functional theory10.3390/app10113914 ↗
36. An insight into using DFT data for Calphad modeling of solid phases in the third generation of Calphad databases, a case study for Al10.1016/j.calphad.2019.02.008 ↗
37. New insights and coupled modelling of the structural and thermodynamic properties of the LiF-UF4 system10.1016/j.molliq.2021.115820 ↗
38. Thermodynamic modeling of the K-KCl and Mg-MgCl2 binary systems using the CALPHAD method10.1016/j.solener.2018.06.013 ↗
39. Thermodynamic evaluation of the NaCl-MgCl2-UCl3-PuCl3 system10.1016/j.jnucmat.2008.01.007 ↗
40. Thermodynamic evaluation and optimization of the LiCl-NaCl-KCl-RbCl-CsCl-MgCl2-CaCl2 system using the modified quasi-chemical model10.1007/s11661-001-0227-2 ↗
41. Thermodynamic evaluation of the (LiF + NaF + BeF2 + PuF3) system: an actinide burner fuel10.1016/j.jct.2009.04.016 ↗
42. Thermodynamic evaluation and optimization of the (LiCl plus NaCl plus KCl + MgCl2 + CaCl2 + CeCl3) system10.1016/j.fluid.2018.11.031 ↗
43. Thermodynamic evaluation and optimization of the LiF-NaF-KF-MgF2-CaF2 system using the modified quasi-chemical model10.1007/s11661-001-0228-1 ↗
44. Thermodynamic Investigation of the CaF2-ThF4 and the LiF-CaF2-ThF4 systems10.1021/acs.jced.5b00347 ↗
45. Thermodynamic investigation of the (LiF + NaF + CaF2 + LaF3) system10.1016/j.jct.2011.05.002 ↗
46. Thermodynamic evaluation of the MF-LaF3 (M = Li, Na, K, Rb, Cs) systems10.1016/j.calphad.2007.07.006 ↗
47. A comprehensive study of the heat capacity of CsF from T = 5 K to T = 1400 K10.1016/j.jct.2012.08.003 ↗
48. Modelling and calculation of the phase diagrams of the LiF-NaF-RbF-LaF3 system10.1016/j.calphad.2006.12.004 ↗
49. Actinide burner fuel: Potential compositions based on the thermodynamic evaluation of MF-PuF3 (M = Li, Na, K, Rb, Cs) and LaF3-PuF3 systems10.1016/j.jnucmat.2008.04.004 ↗
50. Experimental determination and thermodynamic optimization of the CuCl-ZnCl2, ZnCl2-FeCl3, CuCl-FeCl3, CuCl-CuCl2, FeCl2-FeCl3, FeCl2-CuCl2 and CuCl-PbCl2 phase equilibria10.1016/j.calphad.2019.101667 ↗
51. Thermodynamic evaluation and optimization of the (NaCl+KCl+MgCl2+CaCl2+MnCl2+FeCl2+COCl2+NiCl2) system10.1016/j.jct.2004.05.005 ↗
52. Thermodynamic evaluation and optimization of the (MgCl2+CaCl2+MnCl2+FeCl2+COCl2+NiCl2) system10.1016/j.jct.2004.05.004 ↗
53. Thermodynamic assessment of the LiF-NiF2, NaF-NiF2 and KF-NiF2 systems10.1016/j.jct.2018.01.023 ↗
54. Thermodynamic assessment of the LiF-ThF4-PuF3-UF4 system10.1016/j.jnucmat.2015.03.042 ↗
55. Modeling and calculation of the LiF-NaF-MF3 (M = La, Ce, Pu) phase diagrams10.1021/cm051531v ↗
56. Thermodynamic assessment of the LiF-CeF3-ThF4 system: prediction of PuF3 concentration in a molten salt reactor fuel10.1016/j.jnucmat.2012.12.005 ↗
57. Thermodynamic assessment of the LiF-NaF-ThF4-UF4 system10.1016/j.jnucmat.2010.08.017 ↗
58. Phase-diagrams and thermodynamic properties of the 70 binary alkali-halide systems having common ions10.1063/1.555803 ↗
59. The melting points of the chlorides of lithium, rubidium and caesium, and the freezing points of binary and ternary mixtures of these salts, including also potassium and sodium chloride10.1021/ja02254a004 ↗
60. Mineral
61. Thermodynamic description of the K, Be//F, Cl salt system with first-principles calculations10.1016/j.molliq.2019.111384 ↗
62. Condensed equilibria in uranium(III)-Uranium(IV) fluoride system10.1016/0022-1902(74)80219-8 ↗
63. Thermodynamic assessment of the (LiF + UF3) and (NaF + UF3) systems10.1016/j.jct.2012.08.001 ↗
64. Experimental investigations and thermodynamic modelling of KCl-LiCl-UCl3 system10.1016/j.calphad.2013.11.001 ↗
65. Phase diagrams of the NaF-RF3 (R = La,Ce,Pr,Nd,Sm) Systems
66. Thermodynamic evaluation and optimization of the LiCl-NaCl-KCl-RbCl-CsCl-MgCl2-CaCl2-SrCl2 system using the modified quasichemical model10.1179/cmq.2000.39.4.405 ↗
67. Exploring crucible designs for differential scanning calorimetry measurements of fluoride salts10.1016/j.tca.2021.178860 ↗
68. Thermodynamic determination and assessment of the CsF-ThF4 system10.1016/j.jct.2017.05.008 ↗
69. Die binaren phasendiagramme KCL-CrCl2 und CsCl-CrCl2
70. Uber die systeme akalimetallchlorid/chrom(2)-chlorid
71. Thermal analysis of the chromous chloride-sodium chloride system10.1021/j100839a056 ↗
72. Microstructure and phase composition OF NaCl-CrCl2 system
73. Phase equilibria in binary systems PuCl3-RbCl and PuCl3-CsCl10.1021/j100826a515 ↗
74. Phase diagrams of systems of uranium trifluoride with fluoride of alkali metal10.1007/BF01123957 ↗
75. Phase equilibria in the alkali fluoride uranium tetrafluoride fused salt systems .2. The systems KF-UF4 and RbF-UF410.1111/j.1151-2916.1958.tb12912.x ↗
76. Thoma · 1965
77. Freezing point depressions in sodium fluoride .4. Effects of trivalent fluorides10.1021/j100806a061 ↗
78. Systems of alkali and rare-earth metal fluorides
79. Thermochemical tables, NIST-JANAF, 1998. doi:https://doi.org/10.18434/t42s31
80. R.J.M. Konings, J.P.M. van der Meer, E. Walle, Chemical aspects of molten salt reactor fuel, Tech. Rep. (2005) ITU-TN 2005/25
81. Thermochemical Databases, Scientific Group Thermodata Europe (SGTE), 2021, Access via FactSage.
82. Barin · 1997
83. Cordfunke · 1990
84. U-S-F system
85. Phase diagrams for uranium-oxygen-fluorine system
86. The UF4-UF3 system
88. High-temperature studies on UF4-UF3 system
89. Molten fluorides for nuclear applications10.1016/S1369-7021(10)70222-4 ↗
90. Corrosion in the molten fluoride and chloride salts and materials development for nuclear applications10.1016/j.pmatsci.2018.05.003 ↗
91. Corrosion phenomena induced by molten salts in generation IV nuclear reactors
92. Method for identification of redox control parameters for corrosion mitigation in molten fluoride salts10.1016/j.jnucmat.2020.152624 ↗
93. Redox potential control in molten salt systems for corrosion mitigation10.1016/j.corsci.2018.08.035 ↗
94. Thermodynamic evaluation and optimization of the Li, Na, K, Mg, Ca, Sr //F, Cl reciprocal system10.1016/j.jct.2011.03.015 ↗
95. Thermodynamic evaluation and optimization of the Li, Na, K, Mg, Ca//F, CI reciprocal system using the modified quasi-chemical model10.1007/s11661-001-0231-6 ↗