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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Using Eichrom Resins to Simplify the Analyses for Gallium Content and Atom Percent Fission of Irradiated MOX Fuels
J. M. Giaquinto D. L. Denton
Oak Ridge National Laboratory*Chemical Sciences Division
Oak Ridge, Tennessee 37831-6043
*Oak Ridge National Laboratory is managed by UT-Battelle, LLC, for the U.S. Department of Energy under Contract DE-AC05-00OR22725.
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Presentation Overview
Fissile Materials Disposition Program Mixed Oxide Fuel Assembly Separations for Gallium Analysis Separations for Atom Percent Fission Some Burnup Results vs. Predicted Conclusions
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Fissile Materials Disposition Program (FMDP) International effort to reduce highly enriched uranium and
weapons-grade plutonium stockpiles.
Sep93: Pres. Clinton commits U.S. to eliminate or reduce stockpiles.
Dec96: DOE announces preferred approach for disposal of plutonium will be LWRs.
Dec01: Pres. Bush endorses moving forward with a surplus weapons plutonium program based on using LWRs. ORNL is the lead laboratory for the reactor based initiative.
Mar05: NRC issues licensing amendments for Duke Power to allow the receipt and use of four MOX fuel lead assemblies.
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Why Gallium?
Commercial light water reactors use a zirconium alloy for the fuel clad material.
Gallium will attack zirconium metal. Weapons-grade plutonium contains
gallium. Will gallium migrate from the fuel into the
clad material and cause degradation?
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Why Atom Percent Fission Analysis?
Precise documentation of irradiation period for the various tests (PIEs, gallium, fission gas release, etc.)
Validation of INEL computer codes (Gray Chang)
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
MOX Pellets
Fabricated at LANL ~95% uranium (~99%
U-238) ~5% plutonium
(~94% Pu-239)
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Test Assembly
Stainless Steel outer cladding
Zircaloy inner cladding
15 MOX pellets Irradiated in the
Advanced Test Reactor (INEL)
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Un-irradiated MOX Solution Scan
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Un-irradiated Clad Solution Scan
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
MOX Fuel Fission Products Scan
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
TRU Resin Separation-Conditioned with 4 M
HNO3.-Loaded matrix
exchanged aliquot onto column.- Rinsed with 4 M HNO3.- Rinse collected with
earlier eluant.
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Sr/TRU Resin Separation
Condition with 6M HNO3 (20mL)
Load matrix exchanged aliquots onto columns
Rinse with 6M HNO3 (7-8mL)
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Irradiated MOX Post Sr/TRU Separation
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Irradiated Clad Post Sr/TRU Separation
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Poor Ba and FP Removal in Clads
~6,000 ug Zr in load solution HF complexed with boric acid and matrix
exchange into nitric acid Manageable interferences High Sn in solution has caused flow
problems with some samples
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
ASTM E321 96 Overview
U, Pu, and the Nd fission products are chemically separated and determined by IDMS
Atom fractions are calculated for the dominate contributors and fission product 148Nd
The atom fraction of fuel consumed is equal to the atom fraction of 148Nd/148Nd effective yield
Percent burnup is calculated by dividing the atom fraction of fuel consumed by the unirradiated sum of the dominate fissionable isotopes
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
High Mass Fission Products
Nd Nd Nd Nd Nd Nd
Cs Ba La Ce Pr Ce Ce Sm Sm Sm Sm Eu Sm Eu Sm
Natural Nd check mass
Spike mass
Burnup mass
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
ASTM E321 96 Nd Separations
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Eichrom Technologies Ln Resin
di(2-ethylhexyl) orthophosphoric acid (HDEHP)
Hydrophobic support Resin capacity: 2-4
mg Nd/mL Ln resin
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Ln Resin Simplified Separation
5 mL to 6 mL bed volume Resin conditioned with 0.18
M HCl Sample matrix adjusted to
0.18 M HCl Sample loaded onto column
and rinsed through with 0.18 M HCl. Eluant collected in 5 mL fractions.
Nd fractions combined for MS analysis
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
6mL bed volume Ln column 0.180M HCl load and elution (irradiated MOX fuel)
0
2000
4000
6000
8000
10000
12000
14000
1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20
Fraction
Inte
rgra
ted
Co
un
ts
Ce 140
Ce142
Nd143
Ce/Nd144
Nd145
Nd146
Nd148
Nd150
Sm152
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
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OAK RIDGE NATIONAL LABORATORYU. S. DEPARTMENT OF ENERGY
Conclusions
Combining Eichrom Sr and TRU Resins provide for a simple and effective solution for Ga analysis by ICPMS
Eichrom Ln resin provides for an effective baseline separation of the high mass fission products (REEs)
Data supports FMDP goals for reducing Pu stockpiles by using MOX fuels in commercial LWRs.
Security and waste issues still remain however.