DEVELOPMENT OF MINOR ACTINIDE TRANSMUTATION BY …DEVELOPMENT OF MINOR ACTINIDE TRANSMUTATION BY...
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DEVELOPMENT OF MINOR ACTINIDE TRANSMUTATION BY CRIEPI
H. Ohta, T. Ogata, K. Nakamura and T. KoyamaCentral Research Institute of Electric Power Industry (CRIEPI)
11IEMPT, San Francisco, U.S.A., November 3, 2010
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Metal Fuel FBR & Pyro-process
11IEMPT, San Francisco, U.S.A., November 3, 2010
Goals:Security of the long-term energy supply,Reduction of the amount and the toxicity of radioactive waste,Improvement of the proliferation resistance.
Innovative fuel cycle system is under development in CRIEPIU-Pu-Zr Fuel FBR : Excellent nuclear performances & safety featuresPyro-reprocessing : Simultaneous recovery of MA with U and Pu
Injection Casting Fuel Fabrication : Simple remote-control operation
Metal Fuel FBR
Pyro-reprocessing
Fuel FabricationReprocessing(PUREX)
LWR
Fuel Fabrication Repository
U mining Enrichment
Reduction to Metal
U
U U
U, Pu,MA, FP
U
FP
U, Pu
Pyro-partitioning
MA, (RE)
U, Pu, MA, (RE)
U, Pu, MA, (RE)
U, Pu,MA, FP
Spent Oxide Fuel
HLLW(MA, FP)
HLLW: High-Level Liquid Waste
MA: Minor ActinidesFP: Fission ProductsRE: Rare Earths
FP
U, Pu, MA, FP
LWR Fuel Cycle FBR Metal Fuel CycleU, Pu, MA, FP
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MA-Containing Metal Fuel Development
• How much content of MA should be loaded in metal fuel FBR?
Evaluation of expected fuel compositions Burnup and recycle calculations of MA & RE in metal fuel FBR cycleMass flow analysis based on the future fuel cycle scenario
• How about the effect of MA addition in metal fuel?Development of MA- and RE-containing U-Pu-Zr alloys
Ex-reactor experimentsIrradiation experiment Characterization of U-Pu-Zr-MA-RE postirradiation examinations
Various experimental studies on U-Pu-Zr-MA(-RE) alloys are performed in cooperation with JRC-ITU.
11IEMPT, San Francisco, U.S.A., November 3, 2010
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MA Burnup Performancein Metal Fuel FBR
OutputCore residence timeCoolant temp.
inlet / outlet Max. cladding temp.Max. linear powerAve. discharge burnup
1,500MWe / 3,900MWt6years
355 / 510ºC650ºC
500W/cm150GWd/t
Large-scale & high-burnup metal fuel core design is assumed as a model of commercial FBR.
No-MA-makeup MA-enrichedMA content, wt%RE content 1, wt%Pu enrichment, wt%Makeup MA ratio 2, %Doppler const., Tdk/dTCoolant coeff., ¢/ºC
0.80.516.6
--2.3×10-3
0.254
2.01.516.437
-2.2×10-3
0.273
5.03.5
15.853
-2.1×10-3
0.310
Feed compositions and core performance parameters
11IEMPT, San Francisco, U.S.A., November 3, 2010
1: D.F. = 10, 2: (MA from LWR) / (MA in FBR fuel)
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Mass Flow Evaluation (1)
11IEMPT, San Francisco, U.S.A., November 3, 2010
Mass Balance of Pu & MA50 400
LWRs FBRs
Cap
acity
[GW
e]
Years
50
0
Transition Scenario from LWRs to FBRs
Years after FBR introduction Years after FBR introduction
Rem
aini
ng T
RUs [
ton]
LWR operation=50yearsMA content=2wt% MA content=5wt%
Assumptions50GWe of LWRs are operated for 50years before FBR introduction,
Reactor lifetime is 40 years,
MA content in the feed is 2 or 5wt%.
0
200
400
600
800
0 10 20 30 40 50 60 70 80
MAsPu+MAs
0
200
400
600
800
0 10 20 30 40 50 60 70 80
MAsPu+MAs
Rem
aini
ng T
RUs [
ton]
MA content of 2wt%: MA & Pu are recycled at the almost same time,5wt%: MA can be consumed in shorter-term.
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Mass Flow Evaluation (2)
MA content of 2wt%: MA & Pu are balanced.11IEMPT, San Francisco, U.S.A., November 3, 2010
Mass Balance of Pu & MA75 400
LWRs FBRs
Cap
acity
[GW
e]
Years
50
0
Transition Scenario from LWRs to FBRs (2)
Years after FBR introduction Years after FBR introduction
Rem
aini
ng T
RUs [
ton]
LWR operation=50years LWR operation=75yearsMA content=2wt%
Assumptions50GWe of LWRs are operated for 75years before FBR introduction,
Reactor lifetime is 40 years,
MA content in the feed is 2wt%.
0
200
400
600
800
0 10 20 30 40 50 60 70 80
MAsPu+MAs
0
200
400
600
800
0 10 20 30 40 50 60 70 80
MAsPu+MAs
Rem
aini
ng T
RUs [
ton]
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Miscibilities among U-Pu-Zr-MA-RE
44U-18Pu-10Zr-9Np-5Am-3Ce-10Nd (wt%)Pu-Am-RE phaseU-Pu-Zr-Np phase
In the alloys of high RE content,→ Matrix segregates into upper
and lower parts.
100µm
U-Pu-Zr-Np phasePu-Am-RE precipitates
39U-22Pu-12Zr-15Np-10Am-0.6Ce-1.8Nd
In the alloys of low RE content (≤5%),→ RE-rich precipitates were
uniformly dispersed.
U-Pu-Zr-MA-RE alloys of different compositions were mixed by arc-melting.
RE ≤ 5% can be mixed in U-Pu-Zr-MA matrix.11IEMPT, San Francisco, U.S.A., November 3, 2010
→ U-Pu-Zr-MA alloys without RE can be blended homogeneously.
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Phase Structures of annealed U-Pu-Zr-MA-RE
50mm
500°C 600°C 700°C 850°C50mm
500°C 600°C 700°C 850°C
Metallography of U-Pu-Zr-2MA-2RE.
Metallography of U-Pu-Zr-5MA-5RE.
U-Pu-Zr-MA-RE alloys were annealed and quenched.
Am & RE-rich precipitates - Uniformly dispersing- Cohesion at grain boundary
(≥700°C)- ~3µm (-2MA-2RE), - ≥10µm (-5MA-5RE)
Matrix phase≤ 600°C: Two phase structures
ζ+δ at 500°Cγ+δ (or ζ+δ) at 600°C
≥ 700°C: Single γ-phase
11IEMPT, San Francisco, U.S.A., November 3, 2010
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Phase transition temperature
200 400 600 800 200 400 600 800 200 400 600 800Temperature [°C]
Expa
nsio
n
Temperature [°C]Temperature [°C]
Expa
nsio
n
Expa
nsio
n
(a) U-Pu-Zr-2MA-2RE (b) U-Pu-Zr-5MA-5RE (c) U-Pu-Zr
Phase transition temperature of U-Pu-Zr(-MA-RE) were measured by dilatometry method.
~580°Cζ+δ↔ γ+δ
~630°Cγ+δ↔ γ
For all samples, two distinctive phase transition temperatures at ~580°C & ~630°C→
Dilatometric curves
Insignificant influence of MA and RE addition up to 5wt%
11IEMPT, San Francisco, U.S.A., November 3, 2010
ζ+δ↔ γ+δ
γ+δ↔ γ
ζ+δ↔ γ+δ
γ+δ↔ γ
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U-19Pu-10Zr-5MA-5RE U-19Pu-10Zr Reported
U-19Pu-10ZrMelting point [°C] 1207±10 1217±10 1214±75 [2]
ElasticityYoung’s modulus [GPa]Shear modulus [GPa]Poisson’s ratio
93.3135.390.32
85.2232.650.31
Compatibility with SS * [1] 920-960 970-990
Thermal conductivity
Rela
tive
ther
ma
l con
duc
tivity
[-]
02468
1012141618
200 300 400 500 600 700Temperature [°C]
U-Pu-Zr-5MA-5REU-Pu-Zr
Other properties
*: Metallurgical reaction temperature between the alloy and stainless steel.
[1] C. Sari, etal, J. Nucl. Mater., 208 (1994) 201. [2] M.C. Billon, etal., Int. Conf. on Reliable Fuels for Liquid Metal Reactors, (1986).
11IEMPT, San Francisco, U.S.A., November 3, 2010
Diffusion couple of U-Pu-Zr-5MA-5RE / SSOptical metallography α-autoradiography
Steel
Steel
Steel
Steel
Influence of MA and RE addition ≤ 5wt% is not significant.
U-Pu-Zr-5MA-5RE
U-Pu-Zr-5MA-5RE
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Fabrication of MA-containing Metal FuelFuel Fabrication:
U-19Pu-10Zr-2MA-2RE, U-19Pu-10Zr-5MA, U-19Pu-10Zr-5MA-5RE and U-19Pu-10ZrMA=60Np-30Am-10Cm, RE=10Y-10Ce-70Nd-10Gd.
Yttria molds used for fuel rod casting Cast fuel rods
Fuel Rod diameterFuel Rod lengthsDensity
U-19Pu-10Zr-2MA-2REU-19Pu-10Zr-5MA-5REU-19Pu-10Zr-5MAU-19Pu-10Zr
4.9 mm20-50 mm
14.73 g/cm3
14.66 g/cm3
15.31 g/cm3
15.77 g/cm3*
11IEMPT, San Francisco, U.S.A., November 3, 2010
*: Reported value =15.8g/cm3,J.H.Kittel, et al., N.E.D. 15 (1971)
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Irradiation ExperimentMA-containing alloys were irradiated in Phénix.
3 metal fuel pins & 16 oxide fuel pinswere arranged in an capsule.
Pin No.1 : U-19Pu-10ZrPin No.2 : U-19Pu-10Zr-2MA-2REPin No.3 : U-19Pu-10Zr-5MA / -5MA-5RE
Cladding material : 15-15TiBurnup goals ~2.5at.% (METAPHIX-1),
~ 7at.% (METAPHIX-2), ~10at.% (METAPHIX-3).
Oxide Fuel Pin (Driver)Metal Fuel Pin
Irradiation Capsule
6.55mm
No.1
No.2 No.3
Unit [mm]
5050
425
1010
010
028
5
1,79
3
Met
al fu
el P
in N
o.1
Met
al fu
el P
in N
o.2
Oxid
e fu
el d
river
pin
Met
al fu
el P
in N
o.3
U-Pu-Zr
U-Pu-Zr-2MA-2RE U-Pu-Zr
-5MA
U-Pu-Zr-5MA-5RE
U-Pu-Zr
U-Pu-ZrU-Pu-Zr
U-Pu-Zr
850
U-Pu-Zr
U-Pu-Zr
Initial bondsodium level
Schematic views of irradiated fuel pins.Fuel pin arrangement in irradiation capsule.
485
11IEMPT, San Francisco, U.S.A., November 3, 2010
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METAPHIX Program’03 ’04 ’05 ’06 ’07 ’08 ’09 ’10 ’11 ’12
Irradiation ExperimentsMETAPHIX-1 (2.5at.% B.U.)METAPHIX-2 (7at.% B.U.)METAPHIX-3 (10at.% B.U.)
Postirradiation ExaminationsMETAPHIX-1 (2.5at.% B.U.)METAPHIX-2 (7at.% B.U.)METAPHIX-3 (10at.% B.U.)
NDT NDT & Destructive PIEsTransport from Phénix to ITUCooling time
- Irradiation experiments were carried out from Dec. 2003 to May 2008 in Phénix.- After cooling, NDT were carried out.
No excessive damage due to neutron irradiation was observed.- Irradiated fuel pins are transported to ITU for nondestructive & destructive PIE.- After the PIE, pyro-reprocessing experiment is planned.
11IEMPT, San Francisco, U.S.A., November 3, 2010
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Irradiation Conditions
Pin No.1U-19Pu-10Zr
Pin No.2U-19Pu-10Zr+2MA+2RE
Pin No.3(lower)U-19Pu-10Zr
+5MA
Pin No.3(upper)U-19Pu-10Zr+5MA+5RE
Begin of IrradiationMax. Linear Power 1 [W/cm]Max. Cladding Temp. 2 [oC]
350581
327581
343581
332←
End of METAPHIX-1 (120EFPD 3)Max. Linear Power 1 [W/cm]Max. Cladding Temp. 2 [oC]Max. Burnup [at.%]
3305722.4
3085722.5
3255722.4
313←
2.6End of METAPHIX-2 (360EFPD 3)Max. Linear Power 1 [W/cm]Max. Cladding Temp. 2 [oC]Max. Burnup [at.%]
2955566.9
2765567.1
2945567.0
282←
7.5End of METAPHIX-3 (900EFPD 3)Max. Linear Power 1 [W/cm]Max. Cladding Temp. 2 [oC]Max. Burnup [at.%]
26854310.9
25154311.2
26954311.2
256←
11.9
Irradiation parameters were analyzed taking account of the operation diagram of the Phénix reactor.
1: Top of the test alloy, 2: Top of the fuel stack, 3: EFPD=Effective Full Power Days.
Projected Irradiation Conditions for METAPHIX Experiment
11IEMPT, San Francisco, U.S.A., November 3, 2010
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1mm1mm
Three concentric regions are formed.γ ↔ γ+ζ ↔ ζ+δ
(center) (periphery)
Two concentric regions are formed.(γ-phase is not observed.)→ Irradiation temperature < 630°C
11IEMPT, San Francisco, U.S.A., November 3, 2010
(a) (b)
Metallography (1)
405m
mU
-Pu-
Zr
440m
mU
-Pu-
Zr
METAPHIX-1, U-19Pu-10Zr
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100μmCentral Zone
Intermediate Zone
1mm
Cross-Sectional Overview
Unirradiated U-Pu-Zr-2MA-2RE
Dense phase→ (γ+ζ)-phases
Matrix morphology is similar to that of U-Pu-Zr fuel (b).Some narrow layered phases (MA-RE inclusions) spread along grain boundaries in
γ+ζ zone.In low-temperature region, some dark spots (MA and RE inclusions) are visible.
100μm
11IEMPT, San Francisco, U.S.A., November 3, 2010
Metallography (2)
370m
mU
-Pu-
ZrU
-Pu-
Zr-2
MA
-2R
E
METAPHIX-1, U-19Pu-10Zr-2MA-2RE
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1mm
Unirradiated U-Pu-Zr-5MA-5RE
Cross-Sectional Overview
Dense phase→ (γ+ζ)-phases
Porous phase→ γ-phase
Matrix morphology is similar to that of U-Pu-Zr fuel (a).Large precipitates (MA and RE inclusions) appear in γ phase zone.Some narrow layered phases (MA-RE inclusions) spread along grain boundaries in
γ+ζ zone.In low-temperature region, small dark spots (MA and RE inclusions) are observed.
100μmCentral Zone
100μm
Peripheral Zone
Intermediate Zone
11IEMPT, San Francisco, U.S.A., November 3, 2010
METAPHIX-1, U-19Pu-10Zr-5MA-5REMetallography (3)
100μm
370m
mU
-Pu-
ZrU
-Pu-
Zr-5
MA
-5M
A-5
RE
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Characteristics of Irradiated MA-Containing Metal Fuel
1. The radial distribution of fuel matrix morphology is similarto that of U-Pu-Zr ternary fuels.
2. Some large precipitates (MA and RE inclusions) appearin the high-temperature phase.
3. In the dense matrix zone, some narrow layered phases (MA and RE inclusions) spread along grain boundaries.
4. In low-temperature region, some dark spots (MA and RE inclusions) are visible.
11IEMPT, San Francisco, U.S.A., November 3, 2010
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SummaryMass flow of Pu and MA was analyzed for future LWR-FBR transition scenario.
MA content in the FBR fuel was estimated to be 2wt%. With using 5wt% MA content fuel, MAs recycling from LWRs can be accelerated for several decades.
Relevant characteristics of U-Pu-Zr-MA-RE were examined.In the case of ≤ 5wt% MA and ≤ 5wt% RE additions,
- Am-RE-rich precipitates are dispersed almost uniformly in the alloy,- Basic properties are practically unchanged.
MA-containing U-Pu-Zr alloys were irradiated in Phénix.o Compositions: U-19Pu-10Zr, U-19Pu-10Zr-2MA-2RE, U-19Pu-10Zr-5MA(-5RE)o Peak burnups: ~2.5at.%, ~7at.% and ~10at.%.
NDT of the METAPHIX-1, -2 & -3 pins- No critical damage had occurred during irradiation.
Metallography of METAPHIX-1- Matrix structure is similar to that of U-Pu-Zr fuels.- Large precipitates appear in γ-phase zone.- Some layered phase spread along grain boundaries in γ+ζ phase region.
Quantitative analyses are being carried out.- Fuel constituent redistribution,- MA transmutation performance
11IEMPT, San Francisco, U.S.A., November 3, 2010
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Thank you for your attention!!
11IEMPT, San Francisco, U.S.A., November 3, 2010
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Compositions of Metal Fuel Alloys
Average Compositions of Fabricated Metal Fuel Alloys [wt%]
4 types of metal fuel alloy were prepared.
Target 71U-19Pu-10Zr 67U-19Pu-10Zr+2MA+2RE
66U-19Pu-10Zr+5MA
61U-19Pu-10Zr+5MA+5RE
U 71.00 66.85 66.30 63.50Pu 18.93 19.80 19.35 19.75Zr 10.19 9.46 8.97 8.19MA
NpAmCm
0.03-
0.03-
2.081.230.670.18
4.742.971.450.32
4.783.041.520.31
REY
CeNdGd
-----
1.730.120.201.250.16
-----
3.400.310.452.300.32
Impurities < 0.3wt%
11IEMPT, San Francisco, U.S.A., November 3, 2010
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Specifications of Metal Fuel PinsFuel pins were manufactured according to Phénix geometry.
Pin length [mm]Outer cladding diameter [mm]Cladding materialFuel length [mm]Fuel diameter [mm]Initial fuel-cladding gap [mm]Fuel smear density [%]Sodium level above fuel* [mm]Plenum length [mm]
1,7936.55
15-15 Ti4854.9
0.37575.2~10464
* : Sodium is filled into fuel‐cladding gap as thermal bonding.
485mm
10mm
1,793mm
Fuel Pin Specifications in this Irradiation Experiments
11IEMPT, San Francisco, U.S.A., November 3, 2010
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Axial Swelling of Fuel alloy
0.0
1.0
2.0
3.0
4.0
5.0
6.0
0 1 2 3 4 5 6 7Peak Burnup [at.%]
Axial Elong
ation [%
]
ALFUS calculation
Pin No.1: U‐Pu‐ZrPin No.2: U‐Pu‐Zr‐2MA‐2REPin No.3: U‐Pu‐Zr‐5MA / ‐5MA‐5RE
Fuel elongation behavior is independent of MA and RE additions.Axial swelling of METAPHIX fuels is within the range of the prediction.
Fuel stack position was estimated by axial gamma-ray distribution from 106Ru.
11IEMPT, San Francisco, U.S.A., November 3, 2010
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Fission Gas Release
[1] : R. G. Pahl, etal., Proc. Int. Fast Reactor Safety Meeting, Session 2 Vol. IV, 129 (1990).
FP gas release fraction of MA & RE‐containing fuel pins isthe same level as that of U‐Pu‐Zr alloy fuel pins, and consistent with EBR‐II ternary test fuel data.
Peak Burnup [at.%]
0
20
40
60
80
100
0 2 4 6 8 10 12 14 16 18 20
Fractio
nal R
elease [%
]
Pin No.1: U‐Pu‐ZrPin No.2: U‐Pu‐Zr‐2MA‐2REPin No.3: U‐Pu‐Zr‐5MA / ‐5MA‐5REEBR‐II Test Fuel (U‐8Pu‐10Zr) [1]
EBR‐II Test Fuel (U‐19Pu‐10Zr) [1]
Trend‐band of EBR‐II Experiment
11IEMPT, San Francisco, U.S.A., November 3, 2010
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Metallography (3’)
1mmIntermediate Zone
Cross-Sectional Overview
Matrix morphology is similar to that of U-Pu-Zr fuel (b).Some narrow layered phases (MA-RE inclusions) spread along grain boundaries in
γ+ζ zone.In low-temperature region, small dark spots (MA and RE inclusions) are dispersed.
100μmCentral Zone
Dense phase→ (γ+ζ)-phases
100μm
11IEMPT, San Francisco, U.S.A., November 3, 2010
METAPHIX-1, U-19Pu-10Zr-5MA
320m
m
U-P
u-Zr
U-P
u-Zr
-5M
A-5
RE
-5M
A
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Irradiation Behavior Analysis-Fuel Temperature Distribution-
420ºC < Temp. < 685ºC
Fig. Evaluated irradiation temperature for METAPHIX‐1 fuel pin at EOI (Pin No.1: U‐19Pu‐10Zr).
0
50
100
150
200
250
300
350
400
450
500
400 450 500 550 600 650 700
γ(γ+ζ)(δ+ζ)(α+δ+ζ)
PeripheryFuel
Fuel Center
Temperature [°C]
Axial Position of F
uel Stack [m
m]
11IEMPT, San Francisco, U.S.A., November 3, 2010
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T (sample #5)
T (sample #1) > T (sample #2)
Upper SideLower Side405mm
370mm
440mm
Sample #2Sample #1Sample #5
Axial position of fuel stack [mm]
Relativ
e γ‐ray intensity from 10
6 Ru
γ‐ray intensity from 106Ru
Fig. 12. Relative γ‐ray intensity emitted from 106Ru in Pin No.1
Axial position of fuel stack [mm]
Relativ
e γ‐ray intensity from 10
6 Ru
Linear Power [W
/cm]
γ‐ray intensity from 106RuEvaluated Linear Power
Fig. Relative γ‐ray intensity emitted from 106Ru and axial power profile of Pin No. 1
Relativ
e γ‐ray intensity from 10
6 Ru
Axial position of fuel stack [mm]
γ‐ray intensity from 106RuEvaluated Linear PowerUncertainty width of Linear Power
Linear Power [W
/cm]
Analyzed Linear Power ~275W/cm (by 104Nd method)
Discussion - Irradiation Temperature -
11IEMPT, San Francisco, U.S.A., November 3, 2010
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Discussion - Irradiation Temperature -
Due to the uncertainty of linear power,
‐Temperature fluctuation for each fuel rodreaches ~20°C at the fuel center, →Irradiation temperature at higher axial level
can be lower than that at lower level,
‐The highest temperature can be ~660°C.→High‐temperature γ‐phase appears at onlylimited fuel rods.
Temperature [°C]
Axial Position of F
uel Stack [m
m]
Fig. Evaluated irradiation temperature for METAPHIX‐1 fuel pins,taking account of the uncertainties of linear power.
Fuel Center
PeripheryFuel
11IEMPT, San Francisco, U.S.A., November 3, 2010