1 C. Guéneau, 1 S. Gossé, 1 S. Chatain, 1 C. Utton, *2 N. Dupin, 3 B. Sundman, 4 C. Martial, 4 J.C. Dumas, 5 C. Rado. 1 DEN/DANS/DPC/SCP â CEA Saclay ...
FUELBASE : a thermodynamic database for advanced nuclear fuels 1
C. Guéneau, 1 S. Gossé, 1 S. Chatain, 1 C. Utton,
*2
N. Dupin,
3
B. Sundman,
4
C. Martial,
4
J.C. Dumas,
5
C. Rado
1
DEN/DANS/DPC/SCP – CEA Saclay – 91191 Gif-sur-Yvette Cedex, France 2 Calcul Thermo – 3 rue de l’Avenir - 63670 Orcet, France 3 CIRIMAT, ENSIACET, 118 Route de Narbonne, 31077 Toulouse, France 4 DEN/DEC/SESC – CEA Cadarache – 13108 Saint-Paul Lez Durance Cedex 5 DEN/DTEC/SDTC – CEA Valrho – 26702 Pierrelatte Cedex
OBJECTIVE
PROGRESS (2005-2008) Binary systems
To develop a thermodynamic database which will constitute a flexible tool to perform thermodynamic calculations on advanced fuel materials (oxides, carbides, nitrides fuels) for future reactors
C
Mo
N
O
Pu
Si
Ti
U
Zr
W
Re
Nb
C
Andersson 88
SGTE
SGTE
Sundman 05
Grobner 96
Dumitrescu 98
Chevalier 01*
Guillermet 95
Jonsson 93
Dupin 07
Dupin 08
Mo
Frisk 91
Sundman 07
Dupin 05
Liu 05
Chung 99
Dupin 07
Jerlerud 02
N
SGTE
Sundman 05
Hillert 92
Jonsson 96
Chevalier 00*
Ma 04
O
Gueneau 06
Hallstedt 93
Sundman 05
Gueneau 02
Liang 97*
Pu
Dupin 05
Dupin 07
Kurata 99
Kurata 99*
CEA 08
CEA 08
CEA 08
Si
Seifert 00
Gueneau 06
Gueneau 94
Vahlas 89
Dupin 07
Dupin 08
Ti
Rado 06
Kumar 94
U
Chevalier 04
Sundman 07
Guéneau 07
Dupin 08
CONTEXT Gas Fast Reactor High operating temperature ~ 1273 K Fuel kernel
Matrix
Liner
(U,Pu)C ((U,Pu)N)
W-Re (Mo-Re, Nb-Zr )
From the literature * Modified
SiC (TiC, ZrC)
New assessment
Chemical interactions between the fuel components (T< 2273 K) U-Pu-C + W-Re-Mo-Nb-Zr + Si-C phase diagrams Fuel material processing Phase equilibria + vapor partial pressures during processing Ex: (U,Pu)C made by reduction of (U,Pu)O2 by C U-Pu-O-C Incorporation of the Minor actinides Partial press. of MA + µ(C) in (U,Pu,MA)C U-Pu-Am-Np-Cm-C “Chemistry” of the irradiated fuel versus temperature and burnup U-Pu-Am-Np-Cm-C + Fission Products
Np
CEA+I TU 07/08
Sundman 08
Dupin 07
Dupin 07
Ru
Dupin 08
Zr
2008
Am
Dupin 07
Dupin 07
Dupin 08 W
Dupin 07
Ternary systems 2006 2007
C-N-Ti, C-Si-Ti, C-Mo-Ti, C-Mo-Si, U-Pu-Zr U-Pu-O, U-Pu-C, U-O-C, U-Si-C, U-Zr-C, U-C-Mo, U-C-Re, U-C-W
2008
C-Re-W, C-Re-Mo, Pu-C-W, U-Pu-Mo, U-C-Nb, Pu-C-Mo, C-Nb-Zr, Pu-C-Nb, Pu-C-Zr, Pu-O-C, Pu-C-Re
COLLABORATIONS
Sodium Fast Reactor Fuel materials: [(U,Pu)O2,(U,Pu)C] Incorporation of the Minor actinides (MA: Am,Np,Cm) Phase equilibria + Partial pressures of MA + µ(O) in (U,Pu,MA)O2 U-Pu-Am-Np-Cm-O “Chemistry” of the irradiated fuel versus temperature and burnup U-Pu-Am-Np-Cm-O + Fission Products Interaction fuel materials / Na U-Pu-O (C) / Na
FUEL MATERIALS Carbide (U,Pu)C
FUEL / CLADDING INTERACTION
Phase diagram U-Pu-C
C U/(U+Pu)=0.2 1.0
0.6
0.5
0.4 [76BRO/PHI] [76BRO/PHI] [70LOR/DEL] [70LOR/DEL]
0.2 0.1
76 Bro/Phi e(Pu)=0.552 C/M=1.330 76 Bro/Phi e(Pu)=0.316 C/M=1.271 76 Bro/Phi e(Pu)=0.150 C/M=1.076
-6.5
76 Bro/Phi e(Pu)=0.58 C/M=1.94 76 Bro/Phi e(Pu)=0.58 C/M=2.48 76 Bro/Phi e(Pu)=0.33 C/M=2.14 76 Bro/Phi e(Pu)=0.17 C/M=2.10
-7.0
-7.5 4.0
4.2
4.4
4.6
0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0
4.8
5.0
5.2
5.4
5.6
5.8
6.0
10000/T (K-1)
Pu
MOLE_FRACTION PU
UC / SiC
-3.0
log10 [P(Pu(g)) atm]
MC+M2C3
MC
MC+M2C3
UC / W
(U0.8Pu0.2)C1+x
-3.5
L+M2C3
MC
UC / Re
-6.0
0
U
T=1500 K
-5.5
0.3
0
UC / Mo
-5.0
MC2+C
log10 P(Pu(g)atm)
NC CT IO MO LE _F RA
Pu partial pressure in U-Pu-C
-4.5
0.9 0.8 0.7
The FUELBASE database is developed in collaboration with: ITU (R. Konings, D. Manara, P. Gotcu) University of Rennes (H. Noel) University of Sheffield (H. Kinoshita) within the ACTINET network for ACTINIDE SCIENCES
-4.0
-4.5 [76OHS/CAP] Pu/M=0.20 T=2500 K [76OHS/CAP] Pu/M=0.20 T=2400 K [76OHS/CAP] Pu/M=0.20 T=2300 K [76OHS/CAP] Pu/M=0.20 T=2200 K [76OHS/CAP] Pu/M=0.20 T=2200 K [76OHS/CAP] Pu/M=0.20 T=2100 K [76OHS/CAP] Pu/M=0.20 T=2000 K
-5.0 -5.5
-6.0 1.00
1.05
1.10
1.15
1.20
1.25
1.30
C/(U+Pu)
Oxide (U,Pu)O2±x µ(O2) in (U,Pu)O2±x -200
Phase diagram U-Pu-O
(U0,9 Pu0,1)O2±x
-100 -200
U0.8Pu0.2O2 T=2150 K Tetenbaum U0.8Pu0.2O2 T=2250 K Tetenbaum U0.8Pu0.2O2 T=2350 K Tetenbaum U0.8Pu0.2O2 T=2450 K Tetenbaum U0.8Pu0.2O2 T=2550 K Tetenbaum
UO3
∆G(O2) kJ/mol
∆G(O2) kJ/mol
-400 -500 T=1473 T=1373 T=1273 T=1073 T=1223 T=1373
-600 -700 -800 1.95
2.00
K U0.9Pu0.1O2 Woodley81 K U0.9Pu0.1O2 Woodley81 K U0.9Pu0.1O2 Woodley81 K U0.89Pu0.11O2 Markin K U0.89Pu0.11O2 Markin K U0.89Pu0.11O2 Markin
2.05
-300
U3O8
-400
0.70
U4O9 (U0,9 Pu0,2)O2±x
-500
U0.8Pu0.2O2 T=1273 K Javed73 U0.8Pu0.2O2 T=1673 K Javed73 U0.8Pu0.2O2 T=1873 K Javed73 U0.8Pu0.2O2 T=1973 K Javed73
-700
2.10
PuO1,61 Pu2O3
-800 1.90
1.95
2.00
2.05
2.10
0.60
U
0
0.1
0.2 x(Pu)
0.3
0.4
Pu
N(O)
-100
0 U0.69Pu0.31O2 Chilton80 U0.69Pu0.31O2 Chilton80 U0.69Pu0.31O2 Chilton80 U0.7PuO.3O2 Markin U0.7Pu0.3O2 Markin U0.7Pu0.3O2 Markin
-200
3000
T=1473 K U0.6Pu0.4O2 Woodley81 T=1373 K U0.6Pu0.4O2 Woodley81 T=1273 K U0.6Pu0.4O2 Woodley81
Chikalla [12] Martin [13] Boivineau [20] Sari [21] Gardner [23] Besmann [25] Messier [26] Ohse [27] Riley [29] Russel [30] Aitken [40]
liquid (L) 2700 2400
-300 -400 -500
-300 2100
-400
T(K)
T=1815 K T=1713 K T=1810 K T=1073 K T=1223 K T=1373 K
∆G(O2) kJ/mol
-200
PuO 2
0.65
-600
N(O)
-100
T=673 K
0.75
-300
∆G(O2) kJ/mol
ACTINIDE SYSTEMS
0
-100
-500
PuO2-x
1800 1500
PuO1.61
1200
-600 900
-600
(U0,9 Pu0,3)O2±x
-700 -800 1.85
1.90
1.95 N(O)
2.00
2.05
(U0,9 Pu0,4)O2±x 2.10
-700 1.90
1.95
2.00 N(O)
2.05
600
2.10
300 0.58 0.60 0.62 0.64 Pu2O3 PuO 1.52 x(O)
0.66
0.68
