Characterization of Actinide Alloys as Nuclear Transmutation Fuels

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, MCA personnel, FMF personnel
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
8
Powder Metallurgical Approach

• Developed as low temperature fabrication route to
  prevent Am loss. Hot pressing.
• Inhomogeneous microstructure after processing at
  800C
• High impurity content

• Complex process - impractical remote process
  scale-up
• Powder handling
• Material loss
• Time

9
(No Transcript)
10
Americium Retention
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)
  ?-U (? minor)
• 35U-28Pu-7Am-30Zr ?-MZr2 (?-UZr2 hex)
  ?-U (? minor)
• 40U-34Pu-4Am-2Np-20Zr ?-MZr2 (?-UZr2
  hex) ?-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
18
AFC-1F Metal Alloy Fuels XRD Study
19
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.

21
SEM Micrographs of As-Cast 40U-34Pu-4Am-2Np-20Zr
Alloys (MG040)

• Multiphase
• Globule formation (Zr enriched).

22
Differential Scanning Calorimetry of As-Cast
30U-25Pu-3Am-2Np-40Zr Alloy

• Transition from ?-UZr2 to bcc over 565ºC - 600ºC
  range

23
Differential Scanning Calorimetry of As-Cast
40U-34Pu-4Am-2Np-20Zr Alloy

• Transition from ?-UZr2 at 541ºC.
• Transition to bcc at 592ºC.

24
Zr 50U50Pu Vertical Section through U-Pu-Zr
Phase Diagram
25
Laser Flash Diffusivity Measurements
Anter Laser Flash Diffusivity System Modified for
glove-box operation Zero power and finite pulse
width corrected
26
Thermal Conductivity (Clark Taylor Correction)
U-Zr values taken from Takahashi, Yamawaki,
Yamamoto J. Nucl. Mater. 1988, 154, 141.
27
Thermal Diffusivity of Pu-12Am-40Zr
28
Thermal Diffusivity of U-29Pu-4Am-2Np-30Zr
29
Fuel-Cladding Chemical Interaction (fcci)
steel
steel
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
Am
Pu
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