Development of a CALPHAD Thermodynamic Database for Pu-U-Fe-Ga Alloys
Source abstract
Abstract
The interaction of actinides and actinide alloys such as the δ-stabilized Pu-Ga alloy with iron is of interest to understand the impurity effects on phase stability. A newly developed and self-consistent CALPHAD thermodynamic database is presented which covers the elements: Pu, U, Fe, Ga across their whole composition and temperature ranges. The phase diagram and thermodynamic properties of plutonium-iron (Pu-Fe) and uranium-iron (U-Fe) systems are successfully reassessed, with emphasis on the actinide rich side. Density functional theory (DFT) calculations are performed to validate the stability of the stoichiometric (Pu,U)6Fe and (Pu,U)Fe2 compounds by computing their formation enthalpies. These data are combined to construct the Pu-U-Fe ternary phase diagram. The thermodynamic assessment of Fe-Ga is presented for the first time and application to the quaternary Pu-U-Fe-Ga system is discussed.
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Research context
OpenAlex topics: Nuclear Materials and Properties · Rare-earth and actinide compounds · Thermodynamic and Structural Properties of Metals and Alloys
SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.
Affiliations
Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, CA 94550, USA
CEA-Centre de Valduc, 21120 Is sur Tille, France
References (94)
Show source-provided references
1. Thermodynamic re-assessment of the Pu-U system and its application to the ternary Pu-U-Ga system10.1016/j.jnucmat.2014.07.051 ↗
2. Thermodynamic evaluation of the quaternary U-Pu-Zr-Fe system-assessment of cladding temperature limits of metallic fuel in a fast reactor10.1016/S0022-3115(01)00473-1 ↗
3. Kurata, M. (2009, January 12–17). Thermodynamic database on U-Pu-Zr-Np-Am-Fe alloy system II- Evaluation of Np, Am and Fe containing systems. Proceedings of the IOP Conference Series: Material Science and Engineering, San Francisco, CA, USA.10.1088/1757-899X/9/1/012023 ↗
4. Thermodynamic assessment of the Fe-U binary system10.1361/105497103770330730 ↗
5. Thermodynamic calculation of phase equilibria of the U-Ga and U-W systems10.1016/j.jnucmat.2008.07.009 ↗
6. Experimental investigation of the phase equilibria and thermodynamic assessment in the U-Ga and U-Al-Ga systems10.1016/j.jnucmat.2017.11.037 ↗
7. Turchi, P.E.A., Kaufman, L., Liu, Z.-K., and Zhou, S. (2004). Thermodynamics and Kinetics of Phase Transformations in Plutonium Alloys-Part 1, Lawrence Livermore National Lab.. UCRL-TR-206658.10.2172/895082 ↗
8. Lukas, H.L., Fries, S.G., and Sundman, B. (2007). Computational Thermodynamics, The Calphad Method, Cambridge University Press.10.1017/CBO9780511804137 ↗
9. SGTE data for pure elements10.1016/0364-5916(91)90030-N ↗
10. Algebraic representation of thermodynamic properties and the classification of solutions10.1021/ie50458a036 ↗
11. Enthalpies of formation of liquid alloys bismuth-gallium-tin at 723 K—Choice of an analytical representation of integral and partial thermodynamic functions of mixing for this ternary system10.1051/jcp/1975720083 ↗
12. Inhomogeneous Electron Gas10.1103/PhysRev.136.B864 ↗
13. Self-Consistent Equations Including Exchange and Correlation Effects10.1103/PhysRev.140.A1133 ↗
14. Assessing a solids-biased density-gradient functional for actinide metals10.1103/PhysRevB.82.033102 ↗
15. Ziesche, P., and Eschrig, H. (1991). Electronic Structures of Solids, Springer.
16. Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces10.1103/PhysRevLett.100.136406 ↗
17. Ground-State Theory of δ-Pu10.1103/PhysRevLett.84.3670 ↗
18. Density-functional theory for plutonium10.1080/00018732.2019.1599554 ↗
19. Correlation and relativistic effects in U metal and U-Zr alloy: Validation of ab initio approaches10.1103/PhysRevB.88.235128 ↗
20. Comment on “Correlation and relativistic effects in U metal and U-Zr alloy: Validation of ab initio approaches”10.1103/PhysRevB.90.157101 ↗
21. Wills, J.M., Alouani, M., Andersson, P., Delin, A., Eriksson, O., and Grechnev, O. (2010). Full Potential Electronic Structure Method, Springer.10.1007/978-3-642-15144-6 ↗
22. Theory of the crystal structures of cerium and the light actinides10.1080/000187398243492 ↗
23. High-temperature phonon stabilization of γ-uranium from relativistic first-principles theory10.1103/PhysRevB.85.060301 ↗
24. Anisotropic Lattice Distortions in Random Alloys from First-Principals Theory10.1103/PhysRevLett.87.156401 ↗
25. Vitos, L. (2007). Computational Quantum Mechanics for Materials Engineers: The EMTO Method and Application, Springer.
26. Kollar, J., Vitos, L., and Skriver, H.L. (2000). Electronic Structure and Physical Properties in Solids: The Uses of the LMTO Method, Springer.
27. Generalized Gradient Approximation Made Simple10.1103/PhysRevLett.77.3865 ↗
28. Special points for Brillouin-zone integrations10.1103/PhysRevB.13.5188 ↗
29. Density-functional study of the U-Zr system10.1016/j.jallcom.2008.12.052 ↗
30. Density-functional study of Zr-based actinide alloys: 2. U-Pu-Zr system10.1016/j.jnucmat.2009.05.014 ↗
31. Density functional study of Zr-based actinide alloys10.1016/j.jnucmat.2008.09.029 ↗
32. Density-functional study of bcc Pu-U, Pu-Np, Pu-Am, Pu-Cm alloys10.1016/j.jnucmat.2010.10.066 ↗
33. Thermodynamic study of the Np-Zr system10.1016/j.jnucmat.2010.10.085 ↗
34. Density-functional study of bcc U-Mo, Np-Mo, Pu-Mo, and Am-Mo alloys10.1016/j.jnucmat.2012.11.033 ↗
35. Thermodynamic assessment of the Am-Pu system with input from ab initio10.1016/j.jnucmat.2011.06.034 ↗
36. The U-Ti system: Strengths and weaknesses of the CALPHAD method10.1016/j.jnucmat.2011.08.050 ↗
37. The Pu-U-Am system: An ab initio informed CALPHAD thermodynamic study10.1016/j.jnucmat.2014.12.101 ↗
38. Thermostatics and kinetics of transformations in Pu-based alloys10.1016/j.jallcom.2006.10.046 ↗
39. Phase transformations in Pu-Ga alloy: Synergy between simulations and experiments to elucidate direct and indirect reversion competition10.1016/j.actamat.2013.07.060 ↗
40. Phase transformations in PuGa 1 at. % alloy: Study of whole reversion process following martensitic transformation10.1016/j.jallcom.2013.04.142 ↗
41. Phase transformations in PuGa 1 at. % alloy: Influence of stress on δ→α’ martensitic transformation at low temperatures10.1016/j.mtla.2019.100304 ↗
42. Thermodynamic assessments and inter-relationships between systems involving Al, Am, Ga, Pu and U10.1016/j.jnucmat.2016.09.012 ↗
43. Konobeevsky, S.T. Phase Diagram of Some Plutonium Systems, Conference on the Peaceful Use of Atomic Energy, Moscow, Soviet Union.
44. Avivi, E. (1964). Studies of Plutonium-Iron and Uranium-Plutonium-Iron Alloys. [Doctorate Thesis/Dissertation, CEA-Fontenay-aux-Roses, Université de Paris].
45. The Plutonium-Iron system
46. Viscosity-Composition Relationships in Molten Plutonium-Iron Alloys
47. Chiotti, P., Akhachinskij, V.V., Ansara, I., and Rand, M.H. (1981). The Chemical Thermodynamics of Actinide Elements and Compounds, International Atomic Energy Agency.
48. Blanck, H., and Lindner, R. (1976). Plutonium and Other Actinides, North Holland.
49. Akhachinskij, V.V., Koputin, L.M., Ivanov, I., and Podol’skaya, N.S. (1962, January 21–25). Thermodynamics of Nuclear Materials. Proceedings of the Symposium on Thermodynamics of Nuclear Materials, Vienna, Austria.
50. Coffinberry, A.S., and Miner, W.N. (1961). Plutonium Phase Diagrams Studied at Los Alamos, University of Chicago Press.
51. Coffinberry, A.S., and Miner, W.N. (1961). The Metal Plutonium, University of Chicago Press.
52. Schwartz, D.S., Tobash, P.H., and Richmond, S. (2014). Thermal Analysis of Pu6Fe Synthesized from Hydride Precursor, Material Research Society.10.1557/opl.2014.578 ↗
53. Solubility of Plutonium in Iron10.1016/0022-3115(67)90092-X ↗
54. Kassner, M.E., and Peterson, D.E. (1995). Phase Diagrams of Binary Actinide Alloys, ASM International.
55. Uranium-Aluminum and Uranium-Iron
56. The Uranium-Iron System
57. Uranium-Iron Equilibrium Diagram for Dilute Iron Concentration Range
58. Straatman, J.A., and Neumann, N.F. (1964). Equilibrium Structures in the High Uranium-Iron Alloy System, Mallinckrodt Chemical Works. Topical Report. No. MCW-1487 MCW-1487.10.2172/4691350 ↗
59. A study of the iron-rich portion of the Fe-U phase diagram10.1179/cmq.1966.5.4.355 ↗
60. Revision of the Uranium-Iron Phase Diagram10.1016/0022-3115(84)90046-1 ↗
61. Thermodynamics and Phase Equilibria of the Iron-Uranium System10.1016/0022-3115(91)90531-B ↗
62. Thermodynamic Activity Measurements of U-Fe and U-Ga Alloys by Mass Spectrometry10.1016/0022-3115(92)90422-H ↗
63. The Solubility of Iron in Solid Uranium Between 0.003 wt. % and 0.3 wt. % Iron10.1016/0022-3115(66)90167-X ↗
64. Labroche, D. (2000). Contribution a l’etude Thermodynamique du Systeme Ternaire U-Fe-O. [Ph.D. Thesis/Dissertation, Institut National Polytechnique de Grenoble].
65. The system iron-gallium10.1098/rspa.1965.0135 ↗
66. Über den Aufbau des Systems Eisen-Gallium zwischen 10 und 50 At.-% Ga und dessen Abhägigkeit von der Wärmebehandlung, I. Das Diagramm der raumzentrierten Phasen
67. Über den Aufbau des Systems Eisen-Gallium z zwischen 10 und 50 At.-% Ga und dessen Abhägigkeit von der Wärmebehandlung II. Das Gleichgewichtsdiagramm
68. Lattice Parameters of Iron-Rich Iron-Gallium Alloys
69. Structures cristallines des phases Fe6Ge5 et Fe5Ga510.1107/S0567740874006522 ↗
70. Constitution of Some Systems Homologous and Quasihomologous to T5-Ga, II. The Systems Chromium-Gallium, Manganese-Gallium, and Iron-Gallium and some Notes on the Systems Vanadium-Antimony and Vanadium-Arsenic
71. Structural Data on Metallic Phases10.1007/BF00600960 ↗
72. Massalski, T.B., Okamoto, H., Subramnian, P.F., and Kacprzak, L. (1993). Binary Alloy Phase Diagrams, ASM International. [2nd ed.].
73. Reactions between U-Pu-Zr Alloys and Fe at 923 K10.1080/18811248.2000.9714890 ↗
74. Reactions of Uranium-Plutonium Alloys with Iron10.1080/18811248.2001.9715013 ↗
75. Phase Relations in the Fe-Pu-U Ternary System10.1361/105497101770338743 ↗
76. Analysis of metal fuel/cladding metallurgical interaction during off-normal transient events with phase diagram of the U-Pu-Zr-Fe system10.1016/j.jpcs.2004.06.073 ↗
77. Ternary Compounds with the Fe2P type Structure
78. Structural Chemistry and Magnetic Behaviour of Ternary Uranium Gallides U{Fe,Co,Ni,Ru,Rh,Pd,Os,Ir,Pt}Ga510.1016/0022-5088(86)90568-0 ↗
79. Magnetic and Fermi Surface Properties of UFeGa510.1143/JPSJ.70.2982 ↗
80. Magnetic and Fermi surface properties of UTGa5 (T:Fe, Co and Pt)10.1016/S0921-4526(02)02496-1 ↗
81. Thermodynamic and transport properties of single-crystalline UMGa5 (M = Fe, Co, Ni, Ru, Rh)10.1103/PhysRevB.72.035119 ↗
82. Structural and magnetic properties of UFe6Ga6
83. Crystal structure and magnetic properties of UFe5Ga710.1016/j.jnucmat.2009.01.033 ↗
84. Magnetic properties of U2RhGa8 and U2FeGa810.1088/0953-8984/15/28/317 ↗
85. A new family of heavy-fermion compounds10.1016/j.jallcom.2006.06.036 ↗
86. Precipitation dans le system fer-gallium au voisinage de 25 at. % Ga10.1002/pssa.2210410233 ↗
87. Stability of the D03 phase in (FeM1-xMx)3Ga (M = 3d transition metals)10.1016/0956-716X(91)90017-U ↗
88. The Mechanical Behavior of Nonstoichiometric Compounds Ni3Si, Ni3Ge and Fe3Ga10.1007/BF02644399 ↗
89. Structures cristallines des phases Fe3Ga4 et Cr3Ga410.1107/S0567740875003068 ↗
90. FeGa3 and RuGa3: Semiconducting intermetallic Compounds10.1006/jssc.2001.9503 ↗
91. Neutron diffraction studies of the crystalline and magnetic properties of UFe210.1088/0953-8984/1/51/002 ↗
92. Phonon anomalies and local atomic displacements in the exchange-enhanced superconductor U6Fe10.1103/PhysRevB.32.4419 ↗
93. Heats of formation of U6Fe and UFe2 Translated from
94. Hecker, S.S., and Timofeeva, L.F. (2000). A Tale of Two Diagrams, Los Alamos Science.