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Characterization of Actinide Alloys as Nuclear Transmutation Fuels

Characterization of Actinide Alloys as Nuclear Transmutation Fuels

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Characterization of Actinide Alloys as Nuclear Transmutation Fuels

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  1. Characterization of Actinide Alloys as Nuclear Transmutation Fuels J. Rory Kennedy OECD/NEA Eighth Information Exchange Meeting On Partitioning and Transmutation (IEMPT-8) November 10, 2004

  2. Acknowledgements Alloy Fabrication: Mr. Jim Stuart, Mr. Gavin Knighton, Ms. Kaylyne Weatherstone, Mr. Brian Forsmann, Mr. James Sommers Sample Preparation: Mr. Tom DiSanto, Ms. Maryanne Noy, Mr. Brian Forsmann Phase (XRD) measurements: Dr. Steven Frank Microstructure (SEM): Dr. Dennis Keiser Thermal Analysis: Ms. Jennifer Sloppy, Ms. Jacklyn Gates, Ms. Allison Bourke Thermal Diffusivity: Mr. Andrew Maddison, Mr. Samuel Bays, Dr. Marsha Lambregts Chemical Analysis: Dr. Jeffrey Giglio, Mr. Dan Cummings, Mr. Jeffrey Berg, Ms. Pam Crane, Mr. Michael Mitchlik, Material transfer: Mr. Scott Wilde, Mr. Ron Briggs, Mr. Bevin Brush, Health Physics personnel, MC&A personnel, FMF personnel Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  3. Outline • ANL-W Characterization Capabilities • Fuel Fabrication • Am Retention • As-cast Phase Identification • As-cast Microstructure • Thermal Analysis • Differential Scanning Calorimetry (DSC, temps, Cp) • Thermal Mechanical Analysis (TMA, density)) • Thermal Diffusivity (Laser Flash Method, LFD) • Thermal Conductivity • Fuel-Cladding-Chemical-Interaction (FCCI)

  4. ANL-W Fabrication Capabilities • Radioactive isotopes or non-radioactive isotopes • Alloys • Ceramics (oxides, nitrides, carbides, composites, etc.) • Compounds and molecular species

  5. ANL-W Characterization Capabilities • Phase Identification • XRD and elevated variable temperature XRD • Microstructure • SEM, EDS, WDS and TEM • Chemical Analysis • ICP-MS, ICP-AES, gamma spec, LECO, etc • Density • immersion • Thermal Analysis • DSC, TMA, TGA, LFD • Fuel-Cladding-Chemical-Interaction

  6. AFCI Metal Alloy Fuels Under Study • AFC1-B,D Non-fertile (4.0mm diameter; ~83% 239Pu) • 40Pu-60Zr • 60Pu-40Zr • 50Pu-10Np-40Zr • 48Pu-12Am-40Zr • 40Pu-10Am-10Np-40Zr • AFC1-F Low fertile (4.0mm diameter) • 35U-35Pu-30Zr (DU: base composition) • 35U-29Pu-4Am-2Np-30Zr (78% 235U) • 30U-25Pu-3Am-2Np-40Zr (93% 235U) • 40U-34Pu-4Am-2Np-20Zr (33% 235U) • 35U-28Pu-7Am-30Zr (93% 235U) • FUTURIX-FTA (4.9mm diameter) • 35U-29Pu-4Am-2Np-30Zr (78% 235U) • 48Pu-12Am-40Zr

  7. Americium Retention Element Vapor Pressures Am vapor pressure 4-6 orders of magnitude higher than Pu Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  8. Zr rich -(Pu-Zr) Carbon Pu-rich -(Pu-Zr) -Zr Fe Y2O3 Powder Metallurgical Approach • Developed as low temperature fabrication route to prevent Am loss. Hot pressing. • Inhomogeneous microstructure after processing at ~ 800°C • High impurity content • Complex process - impractical remote process scale-up • Powder handling • Material loss • Time Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  9. Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  10. Americium Retention Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  11. AFC1 Metal Alloy Fuels As-Cast Room Temp Phase Results (XRD) 40Pu-60Zr -Zr (hcp) 60Pu-40Zr -Pu (fcc) 48Pu-12Am-40Zr -Pu (fcc) 50Pu-10Np-40Zr -Pu (fcc) + -MZr2 (-UZr2 hex) 40Pu-10Am-10Np-40Zr -Pu (fcc) + -MZr2 (-UZr2 hex) 30U-25Pu-3Am-2Np-40Zr -MZr2 (-UZr2 hex) 35U-29Pu-4Am-2Np-30Zr -MZr2 (-UZr2 hex) + ζ-U (? minor) 35U-28Pu-7Am-30Zr -MZr2 (-UZr2 hex) + ζ-U (? minor) 40U-34Pu-4Am-2Np-20Zr-MZr2 (-UZr2 hex) + ζ-U(?)

  12. AFC1 Metal Alloy Fuels As-Cast Room Temp Phase Results (XRD) Pu-40Zr Pu-12Am-40Zr

  13. AFC1 Metal Alloy Fuels As-Cast Microstructure Results (SEM) Pu-12Am-40Zr Pu-40Zr

  14. AFC1 Metal Alloy Fuels As-Cast Results (DSC, TMA) Pu-40Zr Pu-12Am-40Zr

  15. AFC1 Metal Alloy Fuels As-Cast Room Temp Phase Results (XRD) Pu-10Np-40Zr Pu-10Np-10Am-40Zr

  16. AFC1 Metal Alloy Fuels As-Cast Microstructure Results (SEM) Pu-10Np-10Am-40Zr Pu-10Np-40Zr

  17. DSC/DTA and TMA Heating Curves Pu-10Np-40Zr As-Cast Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  18. AFC-1F Metal Alloy Fuels XRD Study

  19. U-25Pu-3Am-2Np-40Zr (MH036) “30U-30Pu-40Zr” U-29Pu-4Am-2Np-30Zr (MI037) * “36U-34Pu-30Zr” U-34Pu-3Am-2Np-20Zr (MG034) “41U-39Pu-20Zr” U-28Pu-7Am-30Zr (MF032) “35U-35Pu-30Zr”

  20. SEM Micrographs of As-Cast 30U-25Pu-3Am-2Np-40Zr Alloys (MH036) • Even elemental distribution overall. • Some globule formation (oxide enriched). • Few pores. Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  21. SEM Micrographs of As-Cast 40U-34Pu-4Am-2Np-20Zr Alloys (MG040) • Multiphase • Globule formation (Zr enriched). Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  22. Differential Scanning Calorimetry of As-Cast 30U-25Pu-3Am-2Np-40Zr Alloy • Transition from -UZr2 to bcc over 565ºC - 600ºC range Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  23. Differential Scanning Calorimetry of As-Cast 40U-34Pu-4Am-2Np-20Zr Alloy • Transition from -UZr2 at 541ºC. • Transition to bcc at 592ºC. Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  24. Zr – 50U50Pu Vertical Section through U-Pu-Zr Phase Diagram

  25. Instantaneous Laser Pulse Front Face Radiative Heat Loss Back Face Temperature Rise Laser Flash Diffusivity Measurements Anter Laser Flash Diffusivity System Modified for glove-box operation Zero power and finite pulse width corrected Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  26. Thermal Conductivity (Clark & Taylor Correction) U-Zr values taken from Takahashi, Yamawaki, Yamamoto J. Nucl. Mater. 1988, 154, 141. Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  27. Thermal Diffusivity of Pu-12Am-40Zr Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  28. Thermal Diffusivity of U-29Pu-4Am-2Np-30Zr Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  29. Fuel-Cladding Chemical Interaction (fcci) steel steel Characterization Results from AFC1-b,d & f Metal Alloy Fuel Campaigns

  30. FUTURIX-FTA Metal Alloy Fuels FCCI 650ºC 7hrsU-29Pu-4Am-2Np-30Zr – AIM1 SS Diffusion Couple Fe BSE SE Ni Cr Zr

  31. FUTURIX-FTA Metal Alloy Fuels FCCI 650ºC 7hrsU-29Pu-4Am-2Np-30Zr – AIM1 SS Diffusion Couple Np BSE U O Pu Am

  32. FUTURIX-FTA Metal Alloy Fuels FCCI 650ºC 7hrsPu-12Am-40Zr – AIM1 SS Diffusion Couple BSE Pu O SE Am

  33. FUTURIX-FTA Metal Alloy Fuels FCCI 650ºC 7hrsPu-12Am-40Zr – AIM1 SS Diffusion Couple Fe SE BSE Zr Ni Cr

  34. FUTURIX-FTA Metal Alloy Fuels FCCI 650ºC 7hrsPu-12Am-40Zr – AIM1 SS Diffusion Couple BSE – Fe 600 m BSE – Fe 120 m BSE – Fe 1000 m

  35. AFCI Metal Alloy Fuels FCCI 650ºC 200hrsPu-10Am-10Np-40Zr – 422 SS Diffusion Couple 1100 m

  36. Summary • Successfully Arc-Cast Series of Non-fertile and Low-fertile Alloys Composed of Varying Amounts of U, Pu, Np, Am, Zr • Good Retention of Am from Fabrication Process • Continuing the Quantitative Characterization of the Fuels for Phase (XRD), Microstructure (SEM), Thermal Analysis (DSC, TMA, LFD), Thermal Conductivity, and FCCI • Initial PIE looks good