Overview of ITU work on inert matrix fuels · 2006-10-02 · Overview of ITU work on inert matrix...
Transcript of Overview of ITU work on inert matrix fuels · 2006-10-02 · Overview of ITU work on inert matrix...
9th IEMPT, 25-26 September 2006 1
Overview of ITU work on inert matrix fuels
A.Fernandez, D. Haas, J.P. Hiernaut, R. KoningsC. Nästren, H. Ottmar ,J. Somers, D. Staicu
Institute for Transuranium Elements (ITU)Karlsruhe, Germanyhttp://www.jrc.org/
http://itu.jrc.cec.eu.int/
9th IEMPT, 25-26 September 2006 2
Outline
1. Fuels for transmutation: state of the art
2. Fabrication process development at ITU
3. Fuel characterization and material properties
4. Fuels and targets irradiation programmes
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Candidate fuels for transmutation
Fuel composition Fuel form Fuel state Oxide Solid Solution Pellet Metal Composite Particle
Nitride Carbide
Solid solution:• Simple fabrication• Low thermal
conductivity (oxides)• Uniform effects
Composite (CERCER and CERMET):• Complex fabrication• Material selection not evident• ‘Tailored’ thermal conductivity• Localised effects
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(Pu0.20Zr0.66Y0.14)O2-x in MgO
CERCER and CERMET : Effect of particle size
Macrodispersed
Microdispersed
0 50 100 150 200 250 300
Particle diameter (æm)
1
10
100
Vol
ume
% d
amag
ed m
atrix
Vf = 0.05
Vf = 0.20
Vf = 0.10
200µm200µm200µm200µm
200µm200µm200µm200µm
9th IEMPT, 25-26 September 2006 5
Outline
1. Fuels for transmutation: state of the art
2. Fabrication process development at ITU
3. Fuel characterization and material properties
4. Fuels and targets irradiation programmes
9th IEMPT, 25-26 September 2006 6
Criteria :
(a) Shielded installations → remote handling(b) Automation → use of robots(c) dust free(c) process simplification : minimises the (active) fabrication steps
hybrid process consisting of a combination of sol gel and infiltration techniques
Fabrication process development
Minor Actinide Laboratory
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HOMOGENEOUS fuels & targets
Pressing
Sintering
Actinide SolutionSolution Infiltration
Zr,Y Nitrate Solution
Droplet to ParticleConversion
Microspheres
ThermalTreatment
Pressing
Sintering
Actinide SolutionSolution Infiltration
Zr,Y Nitrate Solution
Droplet to ParticleConversion
Microspheres
ThermalTreatment
(Zr0.83Y0.17)O1.925
Am0.06Y0.16 Zr 0.78O2-x
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COMPOSITES : CERCER and CERMET
40-60µm
80-100µm
microdispersion
macrodispersion
sieving
MgO/Mo Powder
Granulation
Mixing
Granulation
Mixing
Pressing
Sintering
Actinide SolutionSolution Infiltration
Zr,Y Nitrate Solution
Droplet to ParticleConversion
Microspheres
ThermalTreatment
Blending
Pressing
Sintering
Actinide SolutionSolution Infiltration
Zr,Y Nitrate Solution
Droplet to ParticleConversion
Microspheres
ThermalTreatment
Blending
250 µm
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• Sucessful development of advanced fabrication processes, by a combination of
– sol-gel
– infiltration
– and conventional blending techniques
• For composites, the process has high flexibilities
– to select the size and
– volume of the ceramic phase, and
– the actinide content in the ceramic phase.
• Excellent homogeneous dispersion of the ceramic phase (fuel-bearing phase)in the metal
Summary (I)
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Outline
1. Fuels for transmutation: state of the art
2. Fabrication process development at ITU
3. Fuel characterization and material properties
4. Fuels and targets irradiation programmes
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Calorimetry: Am content determination
Isothermal environ-ment (water bath)ΔT ≤ 100 μK/24h
≤ 10 μK short term
Thermalinsulation
Heat flow sensor(thermocouples)Sensitivity: 157 μV/mW
Sample canister (SS)
ΔT ⇒ ΔV ∝ Q
Thermal resistance
Isothermal environ-ment (water bath)ΔT ≤ 100 μK/24h
≤ 10 μK short term
Thermalinsulation
Heat flow sensor(thermocouples)Sensitivity: 157 μV/mW
Sample canister (SS)
ΔT ⇒ ΔV ∝ Q
Thermal resistance
Isothermal environ-ment (water bath)ΔT ≤ 100 μK/24h
≤ 10 μK short term
Thermalinsulation
Heat flow sensor(thermocouples)Sensitivity: 157 μV/mW
Sample canister (SS)
ΔT ⇒ ΔV ∝ Q
Thermal resistance
5.99
6.00
6.01
6.02
0 5 10 15 20Time (h)
Ther
mal
pow
er (m
W)
1 h
0.12 %
Predicted equilibrium
%weight Americium (gravimetry)
%Am (calorimetry)
Infiltration 1st 2nd 3rd
17.33
30.6927.94
FUTURIX 5PuO2
12.56 17.57
FUTURIX 6Pu0.30Zr0.70O2
15.44 30.07
Excellent agreement between gravimetry and calorimetry!!
H. Ottmar, Nuclear Chemistry Unit
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Laser flash for thermal properties
• high measurement precision for diffusivity (±1%)• simultaneous measurement of α and Cp (±5%)• highly localised measurements possible• samples with irregular shapes can be used
Sample
Laser Beam
Sample Holder
Furnance
Pyrometer
D. Staicu, Materials Research Unit
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Laser flash thermal conductivity measurements
D.Staicu, Materials Research Unit
600 800 1000 1200 1400
2
4
6
8
60
80Th
erm
al c
ondu
ctiv
ity, W
m-1 s
-1
Temperature, K
Homogeneous (6% mol Am)
(20% mol Am-YSZ) microdispersed in MgO
(20% mol Am - YSZ) macrodispersed in MgO
20 % mol Am - PuO2 dipersed in Mo
20% mol Am -PuZrO2 dispersed in Mo
9th IEMPT, 25-26 September 2006 14 J.P Hiernaut, Materials Research Unit
Vaporisation behaviour: Knudsen cell
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2100 2200 2300 2400 2500 2600
1E-12
1E-11
1E-10
M.S
.sig
. (A
)
Temperature (K)
90Zr 90ZrO 90ZrO2
98Mo
1800 1900 2000 2100 2200 2300 2400 2500 26001E-14
1E-13
1E-12
1E-11
1E-10 237Np 237NpO 237NpO2
239Pu 239PuO 239PuO2
241Am 241AmO 241AmO2
Temperature (K)
M.S
. sig
. (A
)
Vaporisation behaviour
CERMET (Pu0.225Am0.240Zr0.534)O2-x-Molybdenum
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Outline
1. Fuels for transmutation: state of the art
2. Fabrication process development at ITU
3. Fuel characterization and material properties
4. Fuels and targets irradiation programmes
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SMART- 1 : (Pu0.090Zr0.757Y0.153)O1.92 Solid Solution
SMART- 2 : SSL + (Pu0.241Zr0.631Y0.128)O2-x Composite, microdispersed (60-80µm)
•
1 mm 1 mm50 µm250 µm
(Pu0.090Zr0.757Y0.153)O1.92SS + (Pu0.241Zr0.631Y0.128)O2-x
SMART irradiation in HFR
End of irradiation: mid 2007PIE in ITU
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FUTURIX irradiation in Phenix(within IP EUROTRANS, US DOE, CEA, JAEA)
• Pu0.8Am0.2O2-x- Molybdenum and (Pu0.225Am0.240Zr0.534)O2-x-Molybdenum
• High quality pellets fabricated: meeting all specifications for Phenix
600 800 1000 1200 14000
10
20
30
40
50
60
70
80
90
Ther
mal
con
duct
ivity
, m2 s
-1
Temperature, K
Futurix 5 Futurix 6
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Homogeneous and CERMET pellets fabricated by a combination of sol-gel, infiltration and mechanical mixing
INNOVATION: Addition of Carbon to the sol-gel feed solution
• improve pellet microstructure• increase porosity (higher Am content by infiltration )
HELIOS irradiation in HFR Petten(within IP EUROTRANS, CEA, NRG)
Fabrication of four fuels and pins for irradiation in HFR-Petten
Fuel Compound Am content* Pu content* Particle size Density
g·cm3 g·cm3 µm
80-100
20-150
%TDHELIOS 2 ZrYAmO2 0.76
HELIOS 3 ZrYPuAmO2 0.76 0.42
HELIOS 4 ZrYAmO2 + Mo 0.76
HELIOS 5 PuAmO2+ Mo 0.32 1.28
90±5
HELIOS 2 pretest
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HELIOS irradiation in HFR Petten(within IP EUROTRANS, CEA, NRG)
0 20 40 60 8016182022242628303234363840424446
Infiltration solution 300gTh/l 1st infiltration 2nd infiltration
ThO
2 infil
trate
d (%
wei
ght)
Carbon content in sol-gel feed solution(g/l)
PuO2 infiltrated with Th
increase porosity (higher Am content by infiltration )
200 µm
94%TD
Addition of Carbon to the sol-gel feed solution
improve pellet microstructure
50 µm
82%TD
Blackberry structure
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Collaborations
Transmutation European Networkswith ITU participation
Integrated projects
• EUROTRANS(FUTURIX, HELIOS) • EUROPART
Shared Cost Actions
P&T Experiments and studies• Nitride fuels experiment (CONFIRM)• Am transmutation in oxides (FUTURE)• Red-Impact• Pu burning in LWR (DEPUTY)
JRC- IRMM
Samples forcross section determination
Concerted Action
P&T roadmap
PATEROS
ACTINET
• AMZrN• EXAFS on EFTTRA
EFTTRACEA,NRG,FZK,EdF, IE
Americium and fission productstransmutation experiments
Third Party Work
CAMIX-COCHIX
GEN IV
IMF Kernels for VHTROxide fuels for FR