Determining the effects of U/Pu ratio on subsolidus phase transitions in U-Pu-Zr metallic fuel alloys

Middlemas, Scott; Janney, Dawn E.; Adkins, Cynthia; Bawane, Kaustubh

doi:10.1016/j.jnucmat.2024.154909

Determining the effects of U/Pu ratio on subsolidus phase transitions in U-Pu-Zr metallic fuel alloys

Journal Article · Thu Jan 11 23:00:00 EST 2024 · Journal of Nuclear Materials

DOI:https://doi.org/10.1016/j.jnucmat.2024.154909· OSTI ID:2404360

^[1]; Janney, Dawn E. ^[1]; ^[1]; Bawane, Kaustubh ^[1]

Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Here, ternary alloys consisting primarily of uranium, plutonium, and zirconium (U-Pu-Zr) are among the leading candidate fuel systems considered for fast spectrum nuclear reactors. Despite historical operation data from the testing of U-Pu-Zr rods in the Experimental Breeder Reactor-II, considerable uncertainty about the evolution of phases and microstructure across the ternary composition space exists. Due to sluggish kinetics and other difficulties in handling metal actinide specimens, quantitative measurements of phase-transitions in U-Pu-Zr alloys remain sparse in scientific literature, with most investigators reporting either phase-transition temperatures or phase identification data, but not both from the same specimens. The purpose of this paper is to critically compare experimental and calculated phase transition data and correlate with the microstructure and phase characterization data of as-cast and annealed U-Pu-Zr alloys. Phase transition peaks were measured using differential scanning calorimetry in the subsolidus regions (723-948 K) of three ternary U-Pu-Zr alloys with the same zirconium concentration but various U/Pu ratios. Overlapping peaks were deconvoluted using a Frazier-Suzuki peak fitting algorithm, and the critical peak temperatures and enthalpies were calculated. In general, increasing concentrations of Pu were associated with enhanced thermal stability of the body-centered cubic γ phase upon both heating and cooling. Experimental phase transition temperatures in this study tended to agree well with the predictions of the established ternary phase diagrams and other reported phase transition temperatures in literature. Additionally, the TAF-ID thermodynamic database was used to calculate a U-Pu-40 at.% Zr pseudobinary diagram as well as ternary diagrams from 773 to 973 K. The equilibrium phase transition temperatures tended to be considerably lower than measured peak temperatures upon both heating and cooling. Recommendations for improving the quality of data in future U-Pu-Zr characterization studies are also discussed.

View Accepted Manuscript (DOE)

Research Organization:: Idaho National Laboratory (INL), Idaho Falls, ID (United States)

Sponsoring Organization:: USDOE Office of Nuclear Energy (NE), Nuclear Fuel Cycle and Supply Chain. Advanced Fuel Campaign

Grant/Contract Number:: AC07-05ID14517

OSTI ID:: 2404360

Alternate ID(s):: OSTI ID: 2369000

Report Number(s):: INL/JOU--23-74182-Rev001

Journal Information:: Journal of Nuclear Materials, Journal Name: Journal of Nuclear Materials Vol. 591; ISSN 0022-3115

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

References (46)

Fuel constituent redistribution during the early stages of U-Pu-Zr irradiation Porter, D. L.; Lahm, C. E.; Pahl, R. G. Metallurgical Transactions A, Vol. 21, Issue 7 https://doi.org/10.1007/BF02647234	journal	July 1990
Pu-Zr (plutonium-zirconium) Okamoto, H. Journal of Phase Equilibria, Vol. 16, Issue 3 https://doi.org/10.1007/BF02667321	journal	June 1995
Swelling behavior of U-Pu-Zr fuel Hofman, Gerard L.; Pahl, R. G.; Lahm, C. E. Metallurgical Transactions A, Vol. 21, Issue 2 https://doi.org/10.1007/BF02671924	journal	February 1990
Applicability of Fraser–Suzuki function in kinetic analysis of complex crystallization processes Svoboda, Roman; Málek, Jiří Journal of Thermal Analysis and Calorimetry, Vol. 111, Issue 2 https://doi.org/10.1007/s10973-012-2445-9	journal	April 2012
Phase Characteristics of a U-22Pu-4Am-2Np-40Zr Metallic Alloy Containing Rare Earths Burkes, Douglas E.; Kennedy, J. Rory; Hartmann, Thomas Journal of Phase Equilibria and Diffusion, Vol. 30, Issue 4 https://doi.org/10.1007/s11669-009-9556-4	journal	June 2009
The plutonium - uranium system Ellinger, F. H.; Elliott, R. O.; Cramer, E. M. Journal of Nuclear Materials, Vol. 1, Issue 3 https://doi.org/10.1016/0022-3115(59)90019-4	journal	October 1959
Status of LMR fuel development in the United States of America Leggett, R. D.; Walters, L. C. Journal of Nuclear Materials, Vol. 204 https://doi.org/10.1016/0022-3115(93)90195-5	journal	September 1993
Experience with advanced driver fuels in EBR-II Lahm, C. E.; Koenig, J. F.; Pahl, R. G. Journal of Nuclear Materials, Vol. 204 https://doi.org/10.1016/0022-3115(93)90207-F	journal	September 1993
Performance of U-Pu-Zr fuel cast into zirconium molds Crawford, D. C.; Lahm, C. E.; Tsai, H. Journal of Nuclear Materials, Vol. 204 https://doi.org/10.1016/0022-3115(93)90212-H	journal	September 1993
Redistribution behavior of various constituents in U-Pu-Zr alloy and U-Pu-Zr alloy containing minor actinides and rare earths in a temperature gradient Kurata, M.; Inoue, T.; Sari, C. Journal of Nuclear Materials, Vol. 208, Issue 1-2 https://doi.org/10.1016/0022-3115(94)90206-2	journal	January 1994
Temperature gradient driven constituent redistribution in UZr alloys Hofman, G. L.; Hayes, S. L.; Petri, M. C. Journal of Nuclear Materials, Vol. 227, Issue 3 https://doi.org/10.1016/0022-3115(95)00129-8	journal	January 1996
EBR-II driver fuel qualification for loss-of-flow and loss-of-heat-sink tests without scram Lahm, C. E.; Koenig, J. F.; Betten, P. R. Nuclear Engineering and Design, Vol. 101, Issue 1 https://doi.org/10.1016/0029-5493(87)90147-6	journal	April 1987
Metallic fast reactor fuels Hofman, G. L.; Walters, L. C.; Bauer, T. H. Progress in Nuclear Energy, Vol. 31, Issue 1-2 https://doi.org/10.1016/0149-1970(96)00005-4	journal	January 1997
Interdiffusion behavior in UPuZr fuel versus stainless steel couples Keiser, Dennis D.; Petri, Mark C. Journal of Nuclear Materials, Vol. 240, Issue 1 https://doi.org/10.1016/S0022-3115(96)00476-X	journal	December 1996
Analysis of constituent redistribution in the γ (bcc) U–Pu–Zr alloys under gradients of temperature and concentrations Sohn, Y. H.; Dayananda, M. A.; Hofman, G. L. Journal of Nuclear Materials, Vol. 279, Issue 2-3 https://doi.org/10.1016/S0022-3115(99)00290-1	journal	June 2000
Thermodynamic assessment of the Pu-U, Pu-Zr, and Pu-U-Zr systems Kurata, Masaki Calphad, Vol. 23, Issue 3-4 https://doi.org/10.1016/S0364-5916(00)00004-3	journal	September 1999
TAF-ID: An international thermodynamic database for nuclear fuels applications Guéneau, C.; Dupin, N.; Kjellqvist, L. Calphad, Vol. 72 https://doi.org/10.1016/j.calphad.2020.102212	journal	March 2021
Nuclear fuel reprocessing: Can pyro-processing reduce nuclear proliferation risk? Woo, Seung Min; Chirayath, Sunil S.; Fuhrmann, Matthew Energy Policy, Vol. 144 https://doi.org/10.1016/j.enpol.2020.111601	journal	September 2020
Constituent redistribution in U–Pu–Zr fuel during irradiation Kim, Yeon Soo; Hofman, G. L.; Hayes, S. L. Journal of Nuclear Materials, Vol. 327, Issue 1 https://doi.org/10.1016/j.jnucmat.2004.01.012	journal	April 2004
Fuels for sodium-cooled fast reactors: US perspective Crawford, Douglas C.; Porter, Douglas L.; Hayes, Steven L. Journal of Nuclear Materials, Vol. 371, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2007.05.010	journal	September 2007
An approach to fuel development and qualification Crawford, Douglas C.; Porter, Douglas L.; Hayes, Steven L. Journal of Nuclear Materials, Vol. 371, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2007.05.029	journal	September 2007
A US perspective on fast reactor fuel fabrication technology and experience part I: metal fuels and assembly design Burkes, Douglas E.; Fielding, Randall S.; Porter, Douglas L. Journal of Nuclear Materials, Vol. 389, Issue 3 https://doi.org/10.1016/j.jnucmat.2009.02.035	journal	June 2009
Phase characteristics of a number of U–Pu–Am–Np–Zr metallic alloys for use as fast reactor fuels Burkes, Douglas E.; Kennedy, J. Rory; Hartmann, Thomas Journal of Nuclear Materials, Vol. 396, Issue 1 https://doi.org/10.1016/j.jnucmat.2009.10.053	journal	January 2010
Full-length U–xPu–10Zr (x=0, 8, 19wt.%) fast reactor fuel test in FFTF Porter, D. L.; Tsai, Hanchung Journal of Nuclear Materials, Vol. 427, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2012.03.047	journal	August 2012
Crystal structure of high-Zr inclusions in an alloy containing U, Pu, Np, Am, Zr and rare-earth elements Janney, Dawn E.; Kennedy, J. Rory; Madden, J. W. Journal of Nuclear Materials, Vol. 448, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.01.044	journal	May 2014
Thermodynamic re-assessment of the Pu–U system and its application to the ternary Pu–U–Ga system Perron, A.; Turchi, P. E. A.; Landa, A. Journal of Nuclear Materials, Vol. 454, Issue 1-3 https://doi.org/10.1016/j.jnucmat.2014.07.051	journal	November 2014
Am phases in the matrix of a U–Pu–Zr alloy with Np, Am, and rare-earth elements Janney, Dawn E.; Kennedy, J. Rory; Madden, James W. Journal of Nuclear Materials, Vol. 456 https://doi.org/10.1016/j.jnucmat.2014.08.051	journal	January 2015
High- and low-Am RE inclusion phases in a U–Np–Pu–Am–Zr alloy Janney, Dawn E.; Madden, James W.; O’Holleran, Thomas P. Journal of Nuclear Materials, Vol. 458 https://doi.org/10.1016/j.jnucmat.2014.12.016	journal	March 2015
Zr inclusions in actinide–Zr alloys: New data and ideas about how they form Janney, Dawn E.; O’Holleran, Thomas P. Journal of Nuclear Materials, Vol. 460 https://doi.org/10.1016/j.jnucmat.2015.01.065	journal	May 2015
TEM examination of phases formed between U–Pu–Zr fuel and Fe Aitkaliyeva, Assel; Madden, James W.; Miller, Brandon D. Journal of Nuclear Materials, Vol. 467 https://doi.org/10.1016/j.jnucmat.2015.10.043	journal	December 2015
TEM identification of subsurface phases in ternary U–Pu–Zr fuel Aitkaliyeva, Assel; Madden, James W.; Papesch, Cynthia A. Journal of Nuclear Materials, Vol. 473 https://doi.org/10.1016/j.jnucmat.2016.02.022	journal	May 2016
Microstructure changes caused by annealing of U-Pu-Zr alloys Janney, Dawn E.; Sencer, Bulent H. Journal of Nuclear Materials, Vol. 486 https://doi.org/10.1016/j.jnucmat.2017.01.003	journal	April 2017
Behavior of metallic fast reactor fuels during an overpower transient Wachs, Daniel M.; Capriotti, Luca; Porter, Douglas Journal of Nuclear Materials, Vol. 557 https://doi.org/10.1016/j.jnucmat.2021.153304	journal	December 2021
As-cast microstructures in U–Pu–Zr alloy fuel pins with 5–8wt.% minor actinides and 0–1.5wt% rare-earth elements Janney, Dawn E.; Kennedy, J. Rory Materials Characterization, Vol. 61, Issue 11 https://doi.org/10.1016/j.matchar.2010.07.012	journal	November 2010
Phase characteristics of a U–20Pu–3Am–2Np–15Zr metallic alloy containing rare earths Burkes, Douglas E.; Rory Kennedy, J.; Hartmann, Thomas Nuclear Engineering and Design, Vol. 239, Issue 12 https://doi.org/10.1016/j.nucengdes.2009.08.023	journal	December 2009
Preliminary conceptual study of engineering-scale pyroprocess demonstration facility Moon, Seong-In; Chong, Won-Myung; You, Gil-Sung Nuclear Engineering and Design, Vol. 259 https://doi.org/10.1016/j.nucengdes.2013.02.046	journal	June 2013
Resolution of Overlapping Absorption Bands by Least Squares Procedures. Fraser, R. D. B.; Suzuki, Eikichi. Analytical Chemistry, Vol. 38, Issue 12 https://doi.org/10.1021/ac60244a038	journal	November 1966
Kinetic Analysis of Complex Solid-State Reactions. A New Deconvolution Procedure Perejón, Antonio; Sánchez-Jiménez, Pedro E.; Criado, José M. The Journal of Physical Chemistry B, Vol. 115, Issue 8 https://doi.org/10.1021/jp110895z	journal	February 2011
Reprocessing spent nuclear fuel Bodansky, David Physics Today, Vol. 59, Issue 12 https://doi.org/10.1063/1.2435694	journal	December 2006
Fuel-Cladding Chemical Interaction in U-Pu-Zr Metallic Fuels: A Critical Review Matthews, Christopher; Unal, Cetin; Galloway, Jack Nuclear Technology, Vol. 198, Issue 3 https://doi.org/10.1080/00295450.2017.1323535	journal	June 2017
A Critical Review of the Experimentally Known Properties of U-Pu-Zr Alloys. Part 1: Phases and Phase Diagrams Janney, Dawn E.; Hayes, Steven L.; Adkins, Cynthia A. Nuclear Technology, Vol. 205, Issue 11 https://doi.org/10.1080/00295450.2019.1578573	journal	May 2019
A Critical Review of the Experimentally Known Properties of U-Pu-Zr Alloys. Part 2: Thermal and Mechanical Properties Janney, Dawn E.; Hayes, Steven L.; Adkins, Cynthia A. Nuclear Technology https://doi.org/10.1080/00295450.2019.1623617	journal	July 2019
Development of Fast Reactor Metal Fuels Containing Minor Actinides Ohta, Hirokazu; Ogata, Takanari; Papaioannou, Dimitrios Journal of Nuclear Science and Technology, Vol. 48, Issue 4 https://doi.org/10.1080/18811248.2011.9711746	journal	April 2011
The Integral Fast Reactor Chang, Yoon I. Nuclear Technology, Vol. 88, Issue 2 https://doi.org/10.13182/NT88-129	journal	December 1989
Behavior of Modern Metallic Fuel in TREAT Transient Overpower Tests Bauer, Theodore H.; Wright, Arthur E.; Robinson, William R. Nuclear Technology, Vol. 92, Issue 3 https://doi.org/10.13182/NT92-325	journal	December 1990
Pyroprocessing Flowsheets for Recycling used Nuclear fuel Williamson, M. A.; Willit, J. L. Nuclear Engineering and Technology, Vol. 43, Issue 4 https://doi.org/10.5516/NET.2011.43.4.329	journal	August 2011

Similar Records

A critical analysis of U-Pu-Zr phase transitions using calorimetric, microstructural, and phase equilibria data

Journal Article · Tue Apr 01 00:00:00 EDT 2025 · Journal of Nuclear Materials · OSTI ID:2574947

Constituent migration model for U-Pu-Zr metallic fast reactor fuel

Journal Article · Fri Oct 01 00:00:00 EDT 1993 · Nuclear Technology; (United States) · OSTI ID:5889761

Review of the phase equilibria and thermodynamics of binary and ternary systems composed of IFR fuel component metals (U, Pu, and Zr) and nitrogen

Technical Report · Tue Sep 01 00:00:00 EDT 1987 · OSTI ID:713925

Related Subjects

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS
36 MATERIALS SCIENCE
Annealed microstructure
Ternary phase diagrams
U-Pu-Zr alloys
calorimetry
fast reactor fuels
metallic fuels
phase diagram
scanning electron microscopy

Determining the effects of U/Pu ratio on subsolidus phase transitions in U-Pu-Zr metallic fuel alloys

Citation Formats

References (46)

Similar Records

Related Subjects