Skip to main content
SpringerLink
Log in

Experimental and Modeling Review of the Plutonium-Zirconium (Pu-Zr) System: Lost in Translation and Over Time?

  • Published:
Journal of Phase Equilibria and Diffusion Aims and scope Submit manuscript

Abstract

This article presents a review of the phase equilibria of the Pu-Zr system and discusses the contradictory reports on the experimental phase diagram and misinterpretations that have led to confusion over time. In addition, a review of the few Pu-Zr CALculation of PHAse Diagrams (CALPHAD) assessments is presented with emphasis on the heat of formation of the bcc phase, highlighting a disagreement between CALPHAD and ab initio calculations. Based on the information gathered in this study, a critical re-assessment of the Pu-Zr system involving the ζ (Pu28Zr), θ (Pu4Zr), kinetically hindered κ (PuZr2), and once observed ι phases is called for.

This is a preview of subscription content, log in via an institution to check access.

Access this article

Log in via an institution

Price excludes VAT (USA)
Tax calculation will be finalised during checkout.

Instant access to the full article PDF.

Institutional subscriptions

Fig. 1
Fig. 2
Fig. 3
Fig. 4
Fig. 5
Fig. 6
Fig. 7

Similar content being viewed by others

References

  1. R. Agarwal and V. Venugopal, Thermodynamics and phase diagrams of the plutonium-uranium, uranium-zirconium, plutonium-zirconium and plutonium-uranium-zirconium systems, Technical Report, Bhabha Atomic Research Centre, Mumbai, India; BARC-2004/E/009, 2004, 65 p.

  2. D.E. Janney, S.L. Hayes, and C.A. Adkins, A critical review of the experimentally known properties of U-Pu-Zr alloys. Part 1: phases and phase diagrams, Nucl. Technol., 2019, https://doi.org/10.1080/00295450.2019.1578573

    Article  Google Scholar 

  3. A.A. Bochvar, S.T. Konobeevskii, V.I. Kutaitsev, T.S. Men’shikova, and N.T. Chebotarev, Interaction of plutonium and other metals in relation to their arrangement in Mendeleev’s periodic table. in Proceedings of the Second International Conference on the Peaceful Uses of Atomic Energy, United Nations: Geneva, Switzerland, 1958; vol. 6, pp. 184–193.

  4. J.A.C. Marples, The Plutonium-Zirconium phase diagram, J. Less-Common Met., 1960, 2, p 331-351. https://doi.org/10.1016/0022-5088(60)90042-4

    Article  Google Scholar 

  5. F.H. Ellinger, C.C. Land, and K.A. Gschneidner, Alloying behavior of plutonium, Plutonium Handbook: A Guide to the Technology, Vol 1, O.J. Wick, Ed., American Nuclear Society, La Grange Park, 1967, p 191-247

    Google Scholar 

  6. F.H. Ellinger, Discussion of plutonium-zirconium alloys. in Plutonium 1960, Proceedings of the Second International Conference on Plutonium Metallurgy, Grenoble, France, April 19–22, 1960; ed. by E. Grison, W.B.H. Lord, R.D. Fowler (Cleaver-Hume Press, London, 1961), pp. 318–319

  7. A. Robillard, discussion of plutonium-zirconium alloys. in Plutonium 1960, Proceedings of the Second International Conference on Plutonium Metallurgy, Grenoble, France, April 19–22, 1960; ed. by E. Grison, W.B.H. Lord, R.D. Fowler, (Cleaver-Hume Press, London, 1961), pp. 320–327.

  8. F.H. Ellinger and C.C. Land, Plutonium 1970 and Other Actinides, W.N. Miner, Ed., AIME, New York, 1970, p 686

    Google Scholar 

  9. F.H. Ellinger, W.N. Miner, D.R. O’Boyle, and F.W. Schonfeld, Constitution of Plutonium Alloys; Report LA-3870, Los Alamos Scientific Laboratory, Los Alamos, 1968

    Book  Google Scholar 

  10. D.F. Bowersox and J.A. Leary, The solubilities of selected elements in liquid plutonium. XI. Zirconium; Report LA-3742, Los Alamos, Los Alamos National Laboratory, 1967

    Book  Google Scholar 

  11. D.F. Bowersox and J.A. Leary, Solubilities of selected elements in liquid plutonium. 2. Titanium vanadium chromium manganese zirconium niobium molybdenum and thulium, J. Nucl. Mater., 1968, 27, p 181-186. https://doi.org/10.1016/0022-3115(68)90121-9

    Article  ADS  Google Scholar 

  12. A.F. Berndt, The theta phase in the plutonium-zirconium system, J. Less-Common Met., 1967, 12, p 82-83. https://doi.org/10.1016/0022-5088(67)90076-8

    Article  Google Scholar 

  13. V.I. Kutaitsev, N.T. Chebotarev, I.G. Lebedev, M.A. Andrianov, V.N. Konev, and T.S. Menshikova, Phase diagrams of plutonium with the metals of groups IIA, IVA, VIIIA, and IB. in Plutonium 1965, Proceedings of the Third International Conference on Plutonium, London, United Kingdom, November 22–26, 1965; ed. by A.E. Kay, M.B. Waldron, (Chapman and Hall, London, 1967), pp. 420–457

  14. V.I. Kutaitsev, N.T. Chebotarev, M.A. Andrianov, V.N. Konev, I.G. Lebedev, V.I. Bagrova, A.V. Beznosikova, A.A. Kruglov, P.N. Petrov, and E.S. Smotriskaya, Phase diagrams of plutonium with metals of groups IIA, IVA, VIII, and IB, Soviet Atomic Energy, 1967, 23, p 1279-1287. https://doi.org/10.1007/BF01162033

    Article  Google Scholar 

  15. J.M. Taylor, The plutonium-zirconium equilibrium diagram from 0 to 10 at% Zr, J. Nucl. Mater., 1969, 30, p 346-350. https://doi.org/10.1016/0022-3115(69)90253-0

    Article  ADS  Google Scholar 

  16. W.H. Zachariasen and F.H. Ellinger, Unit Cell of the Zeta Phase of the Plutonium Zirconium and the Plutonium Hafnium Systems; Report LA-4367, Los Alamos National Laboratory, Los Alamos, 1970

    Book  Google Scholar 

  17. D.T. Cromer, The crystal structure of ζ-Pu-Zr, ideal formula Pu28Zr, Acta Crystallogr. B, 1979, 35, p 14-19. https://doi.org/10.1107/S0567740879002430

    Article  Google Scholar 

  18. H.J. Okamoto, Pu-Zr (plutonium-zirconium), Phase Equilib., 1993, 14, p 400-401. https://doi.org/10.1007/BF02668249

    Article  Google Scholar 

  19. H.J. Okamoto, Pu-Zr (plutonium-zirconium), Phase Equilib., 1995, 16, p 287-288. https://doi.org/10.1007/BF02667321

    Article  Google Scholar 

  20. M.E. Kassner and D.E. Peterson, Phase Diagrams of Binary Actinide Alloys, Materials Park, OH, ASM International, 1995

    Google Scholar 

  21. D.E. Janney, Metallic Fuels Handbook, Part 1 and Part 2, Idaho National Lab, Idaho, 2018, https://doi.org/10.2172/1469797

    Book  Google Scholar 

  22. J.C. Lauthier, N. Housseau, A. Van Craeynest, and D.J. Calais, Contribution a l’etude du diagramme de phases plutonium-zirconium, J. Nucl. Mater., 1967, 23, p 313-319. https://doi.org/10.1016/0022-3115(67)90164-X

    Article  ADS  Google Scholar 

  23. F.W. Schonfeld, The Metal Plutonium, A.S. Coffinberry and W.N. Miner, Ed., University of Chicago Press, Chicago, 1961, p 255-264

    Google Scholar 

  24. M.B. Waldron, Phase Diagrams of Plutonium Alloys Studied at Harwell, The Metal Plutonium, A.S. Coffinberry and W.N. Miner, Ed., University of Chicago Press, Chicago, 1961, p 225-239

    Google Scholar 

  25. M.B. Waldron, J. Garstone, J. J.A. Lee, P.G. Mardon, J.A.C. Marples, O.M. Poole, G.K. Williamson, The physical metallurgy of plutonium. in Proceedings of the Second United Nations International Conference on the Peaceful Uses of Atomic Energy, Geneva, Switzerland, September 1–13, 1958; United Nations: Geneva; vol. 6, pp. 162–169

  26. H. Okamoto, Pu-Zr (Plutonium-Zirconium). In Binary Alloy Phase Diagrams, II Ed., Ed. T.B. Massalski, Vol. 3, 1990; pp 3185-3186

  27. Y. Suzuki, A. Maeda, and T. Ohmichi, Phase diagram of the Pu-Zr system in the Zr-rich region, J. Alloys Compd., 1992, 182, p L9-L14. https://doi.org/10.1016/0925-8388(92)90590-6

    Article  Google Scholar 

  28. D.R. O’Boyle and A.E. Dwight, in Plutonium 1970, Proceedings of the Fourth International Conference on Plutonium and Other Actinides, Santa Fe, NM, October 5–9, 1970; ed. by W.N. Miner, (Metallurgical Society of the AIME, Englewood), vol. 2, pp. 720–732.

  29. F.H. Ellinger and C.C. Land, On the Plutonium-Zirconium Phase Diagram, Nucl. Metall., 1971, 17, p 686-698

    Google Scholar 

  30. A. Maeda, Y. Suzuki, Y. Okamoto, and T. Ohmichi, Vaporization behavior of plutonium-zirconium binary alloy, J. Alloys Compd., 1994, 205, p 35-38. https://doi.org/10.1016/0925-8388(94)90761-7

    Article  Google Scholar 

  31. L. Leibowitz, E. Veleckis, R.A. Blomquist, and A.D. Pelton, Solidus and liquidus temperatures in the uranium-plutonium-zirconium system, J. Nucl. Mater., 1988, 154, p 145-153. https://doi.org/10.1016/0022-3115(88)90128-6

    Article  ADS  Google Scholar 

  32. M. Kurata, Thermodynamic assessment of the Pu-U, Pu-Zr, and Pu-U-Zr systems, Calphad, 1999, 23(3–4), p 305-337. https://doi.org/10.1016/S0364-5916(00)00004-3

    Article  ADS  Google Scholar 

  33. M. Kurata, Thermodynamic database on U-Pu-Zr-Np-Am-Fe alloy system I—Re-evaluation of U-Pu-Zr alloy system. in IOP Conference Series: Materials Science and Engineering, vol. 9, pp. 012022-1–8. https://doi.org/10.1088/1757-899x/9/1/012022

  34. A. Landa, P. Söderlind, P.E.A. Turchi, L. Vitos, and A. Ruban, Density-functional study of Zr-based actinide alloys: 2. U-Pu–Zr system, J. Nucl. Mater., 2009, 393, p 141-145. https://doi.org/10.1016/j.jnucmat.2009.05.014

    Article  ADS  Google Scholar 

  35. P.E.A. Turchi, P. Söderlind, and A.I. Landa, From electronic structure to thermodynamics of actinide-based alloys, JOM, 2014, 66(3), p 375-388. https://doi.org/10.1007/s11837-014-0882-6

    Article  Google Scholar 

  36. A. Perron, P.E.A. Turchi, A. Landa, P. Söderlind, B. Oudot, B. Ravat, F. Delaunay, and M. Kurata, Thermodynamic re-assessment of the Pu-U system and its application to the ternary Pu-U-Ga system, J. Nucl. Mater., 2014, 454, p 81-95. https://doi.org/10.1016/j.jnucmat.2014.07.051

    Article  ADS  Google Scholar 

  37. A. Perron, P. Turchi, A. Landa, P. Söderlind, B. Ravat, B. Oudot, and F. Delaunay, The Pu-U-Am system: An ab initio informed CALPHAD thermodynamic study, J. Nucl. Mater., 2015, 458, p 425-441. https://doi.org/10.1016/j.jnucmat.2014.12.101

    Article  ADS  Google Scholar 

  38. A. Perron, P.E.A. Turchi, A. Landa, B. Oudot, B. Ravat, and F. Delaunay, Thermodynamic assessments and inter-relationships between systems involving Al, Am, Ga, Pu, and U, J. Nucl. Mater., 2016, 482, p 187-200. https://doi.org/10.1016/j.jnucmat.2016.09.012

    Article  ADS  Google Scholar 

  39. E.E. Moore, P.E.A. Turchi, A. Landa, P. Söderlind, B. Oudot, J.L. Belof, S.A. Stout, and A. Perron, Development of a CALPHAD Thermodynamic Database for Pu-U-Fe-Ga Alloys, Appl. Sci., 2019, 9, p 5040. https://doi.org/10.3390/app9235040

    Article  Google Scholar 

  40. P.E.A. Turchi and A.P.P. Perron, Alloyed plutonium: thermodynamics and application to transformations, Chapter 8 in Plutonium Handbook, Vol 1, 2nd ed., D.L. Clark, D.A. Geeson, and R.J. Hanrahan, Jr., Ed., American Nuclear Society, La Grange Park, 2019, p 333-639

    Google Scholar 

Download references

Acknowledgements

This work is performed under the auspices of the US Department of Energy by the Lawrence Livermore National Laboratory under Contract No. DE-AC52-07NA27344. A.P. thanks the dedication, responsiveness, and expertise of the staff of the LLNL Research Library.

Author information

Authors and Affiliations

  1. Lawrence Livermore National Laboratory, 7000 East Avenue, Livermore, CA, 94550, USA

    Aurélien Perron & Patrice E. A. Turchi

Authors
  1. Aurélien Perron
    View author publications

    You can also search for this author in PubMed Google Scholar

  2. Patrice E. A. Turchi
    View author publications

    You can also search for this author in PubMed Google Scholar

Corresponding author

Correspondence to Aurélien Perron.

Additional information

Publisher's Note

Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.

This article is an invited paper selected from presentations at “PSDK XIV: Phase Stability and Diffusion Kinetics—Gibbs: Phase Equilibria, Diffusion and Materials Design” held during MS&T’19, September 29–October 3, 2019, in Portland, Oregon. The special sessions were dedicated to honor Dr. Patrice Turchi, recipient of the ASM International 2019 J. Willard Gibbs Phase Equilibria Award “for outstanding and pioneering contributions in the application of first-principles, quantum–mechanical calculations to the modeling of phase equilibria and thermodynamic behavior of alloys.” It has been expanded from its original presentation.

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Perron, A., Turchi, P.E.A. Experimental and Modeling Review of the Plutonium-Zirconium (Pu-Zr) System: Lost in Translation and Over Time?. J. Phase Equilib. Diffus. 41, 756–763 (2020). https://doi.org/10.1007/s11669-020-00845-x

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1007/s11669-020-00845-x

Keywords

Search

Navigation