Effect of Burn-up and High Burn-up Structure on UO 2 Spent Fuel Matrix Dissolution D. Serrano-Purroy 1 , I. Casas 2 , E. González-Robles 3 , J. P. Glatz 1 , D. Wegen 1 , F. Clarens 3 , J. Giménez 2 , J. de Pablo 2,3 , A. Martínez-Esparza 4 MRS’11, BUENOS AIRES, OCTOBER 2-6, 2011 1 2 3 4
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Effect of Burn-up and High Burn-up Structure on UO2 Spent Fuel Matrix Dissolution
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Effect of Burn-up and High
Burn-up Structure on UO2
Spent Fuel Matrix Dissolution D. Serrano-Purroy1, I. Casas2, E. González-Robles3,
J. P. Glatz1, D. Wegen1, F. Clarens3, J. Giménez2,
•In air PO2 21%•Temperature 25 ± 5 ºC•pHi 8.0 ± 0.2 •pHo 7.2 ± 0.5•Flow rate 0.025-0.1 L/min•Weight of solid 1 g
Experimental conditions
Radionuclide rates normalized to uranium:
Dissolution Rates:
ACQ
rate ii
U
i
i
Uii M
Mmassmass
raterate normalized
CORE
1,E-17
1,E-16
1,E-15
1,E-14
1,E-13
1,E-12
1,E-11
1,E-10
1,E-09
1,E-08
1,E-07
0 50 100 150 200 250 300 350 400 450 500
time (d)
rate
s (
mo
l/m
2. s
)
U Np Pu Am Cm
CORE
1,E-13
1,E-12
1,E-11
1,E-10
1,E-09
1,E-08
0 50 100 150 200 250 300 350 400 450 500
time (d)
no
rm.
rate
s (
mo
l/m
2. s
)
U Np Pu Am Cm
OUT
1,E-16
1,E-15
1,E-14
1,E-13
1,E-12
1,E-11
1,E-10
1,E-09
1,E-08
0 100 200 300 400 500
time (d)
rate
s (m
ol/m
2. s)
U Np Pu Am Cm
OUT
1,E-13
1,E-12
1,E-11
1,E-10
1,E-09
1,E-08
1,E-07
0 100 200 300 400 500
time (d)
norm
. rat
es (m
ol/m
2.s)
U Np Pu Am Cm
60HBU Dissolution & normalized rates for Actinides
48 MBU Dissolution & normalized rates for Actinides
CORE
1.E-15
1.E-14
1.E-13
1.E-12
1.E-11
1.E-10
1.E-09
1.E-08
0 50 100 150 200 250 300 350
time (d)
rate
s (
mo
l m
-2 s
-1)
U Np Pu Am Cm
OUT
1.E-12
1.E-11
1.E-10
1.E-09
1.E-08
1.E-07
1.E-06
0 50 100 150 200 250 300 350
Time (days)
norm
alis
ed r
ate
s (
mol m-2
s-1)
U Np Pu Am Cm
OUT
1.E-15
1.E-14
1.E-13
1.E-12
1.E-11
1.E-10
1.E-09
1.E-08
1.E-07
1.E-06
0 50 100 150 200 250 300 350
time (d)
rate
s (
mol m
-2 s-1
)
U Np Pu Am Cm
CORE60HBU
OUT60HBU
CORE48MBU
OUT48MBU
NORMALIZEDRATE
(mol/m2 s)
U 5.1 10-12 2.1 10-12 8.0 10-11 4.0 10-11
Np 1.6 10-10 5.2 10-11 1.0 10-10 8.0 10-11
Pu 1.0 10-11 5.7 10-12 3.0 10-11 1.4 10-11
Am 3.5 10-12 2.5 10-12 5.0 10-11 2.0 10-11
RATIO
Np/U 11.3 15.2 1.4 2.2
Pu/U 1.2 1.7 0.4 0.4
Am/U 0.4 0.6 0.7 0.7
Results
Some remarks
Uranium and Actinide dissolution rates are twice
faster in the CORE region than in the Periphery
Except for Np in 60HBU fuel, actinides dissolve
congruently with uranium
Uranium dissolution rate is lower in 60HBU fuel than
in 48MBU fuel
60HBU Normalized Rates for Fission Products
CORE
1,E-14
1,E-13
1,E-12
1,E-11
1,E-10
1,E-09
1,E-08
1,E-07
0 100 200 300 400 500
time (d)
no
rma
lize
d r
ate
s (
mo
l/m
2. s
)
Rb Sr Y Zr Mo Tc Ru Rh Cs Nd U
OUT
1,E-14
1,E-13
1,E-12
1,E-11
1,E-10
1,E-09
1,E-08
1,E-07
0 100 200 300 400 500
time (d)n
orm
alize
d r
ate
s (
mo
l/m
2.s
)
Rb Sr Y Zr Mo Tc Ru Rh Cs Nd U
48MBU Normalized Rates for Fission Products
CORE
1.E-13
1.E-12
1.E-11
1.E-10
1.E-09
1.E-08
1.E-07
0 50 100 150 200 250 300 350
time (d)
norm
alised r
ate
s (
mol m
-2 s
-1)
Rb Sr Y Zr Mo Tc Ru Rh Cs La Nd U
OUT
1.E-13
1.E-12
1.E-11
1.E-10
1.E-09
1.E-08
1.E-07
1.E-06
0 50 100 150 200 250 300 350
times (t)
norm
alised r
ate
s (
mol m
-2 s
-1)
Rb Sr Y Zr Mo Tc Ru Rh Cs La Nd U
Ratio CORE60HBU
OUT60HBU
CORE48MBU
OUT48MBU
Rb/U 25.4 113.7 11.0 4.0
Sr/U 7.7 16.2 3.5 1.4
Y/U 1.8 1.7 2.3 3.0
Zr/U 0.02 0.04 0.2 0.1
Mo/U 4.1 29.7 4.2 2.0
Tc/U 0.5 0.5 1.3 1.1
Ru/U 0.3 0.8 0.3 0.7
Rh/U 0.2 0.5 0.3 0.8
Cs/U 2.0 40.2 10.0 3.1
Results
0,00
20,00
40,00
60,00
80,00
100,00
120,00
Rb/U Sr/U Y/U Zr/U Mo/U Tc/U Ru/U Rh/U Cs/U
dis
solu
tio
n r
ate
rat
io
60core
60out
48core
48out
Results: FP rates/ U rate
Some remarks
Fission products normalized dissolution rates are
similar in 48MBU for both core and out samples
Fission products normalized dissolution rates are
higher in out than in core samples in 60HBU
Rb, Sr, Mo, Cs are more segregated from UO2-grains
in 60HBU than in 48MBU
-12.00
-11.50
-11.00
-10.50
-10.00
-9.50
-9.00
-4.50 -4.00 -3.50 -3.00 -2.50 -2.00 -1.50 -1.00
log
rate
log [HCO3-]
Gray_33 MW d/kgU Röllin_43 MW d/kg U this_work_6OHBU_out this_work_60HBU_core
Serrano_53 MW d/kg U this_work_48MBU_core this_work_48MBU_out
Matrix dissolution rate comparison
Conclusions
Rim
Grains
Gap
Grains Boundaries
IRF 2 options:
IRF or matrix
2 options IRF or matrix
This work indicates that High BU Structure (RIM) can not be considered IRF. OUT Dissolution rate (including a percentage of RIM) lower than CORE rate for both HBU and MBU
Congruent dissolution with UO2-matrix: Np, Pu, Am, Cm, except for Np in 60HBU. Rb, Sr, Cs, Mo are more segregated from UO2-grains in 60HBU than in 48MBU
-phase Dissolution lower than UO2-matrix similar in both HBU and MBU fuels
Not studied in detail in
this work, only 3% of
grain boundary present
Not studied in this
work, no gap was
present
UO2-matrix dissolution ratehigher in MBU than in HBU
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