Overview of ITU work on inert matrix fuels
A.Fernandez, D. Haas, J.P. Hiernaut, R. Konings
C. Nästren, H. Ottmar ,J. Somers, D. Staicu

Institute for Transuranium Elements (ITU)
Karlsruhe, Germany
http://www.jrc.org/
http://itu.jrc.cec.eu.int/
9th IEMPT, 25-26 September 20061

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

2Candidate fuels for transmutation
Fuel composition

Fuel form

Fuel state

Oxide
Metal

Solid Solution
Composite

PelletParticle

NitrideCarbide

Solid solution:• Simple fabrication• Low thermal
conductivity (oxides)• Uniform effects

9th IEMPT, 25-26 September 2006

3Composite (CERCER and CERMET):• Complex fabrication• Material selection not evident• ‘Tailored’ thermal conductivity• Localised effects

CERCER and CERMET : Effect of particle size

Volume % damaged matrix(Pu0.20Zr0.66Y0.14)O2-x in MgOMicrodispersed

10010200µm

Vf = 0.20

Macrodispersed

Vf = 0.10
Vf = 0.051050100150200250

300

Particle diameter (æm)

200µm

9th IEMPT, 25-26 September 2006

4

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

5Fabrication process development
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

Minor Actinide Laboratory
9th IEMPT, 25-26 September 2006

6

HOMOGENEOUS fuels & targets
Zr,Y Nitrate Solution
Droplet to Particle
Conversion
Microspheres
Solution Infiltration
ThermalTreatment
Pressing(Zr0.83Y0.17)O1.925

Am0.06Y0.16 Zr 0.78O2-x

Sintering

9th IEMPT, 25-26 September 2006

Actinide Solution

7

COMPOSITES : CERCER and CERMET
microdispersion
Zr,Y Nitrate Solution
Droplet to Particle
Conversion

40-60µm

sieving

Microspheres
Solution Infiltration
ThermalTreatment

Actinide Solution

macrodispersion

80-100µm

MgO/Mo PowderGranulation

Blending

MixingPressing
Sintering
250 µm

9th IEMPT, 25-26 September 2006

8Summary (I)• 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

9th IEMPT, 25-26 September 2006

9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 200610

Calorimetry: Am content determination
6.02

Thermal resistance

Thermal power (mW)

Predicted equilibrium

ΔT ⇒ ΔV ∝ Q

Isothermal environment (water bath)
ΔT ≤ 100 μK/24h≤ 10 μK short term

Heat flow sensor(thermocouples)
Sensitivity: 157 μV/mW
Sample canister (SS)

FUTURIX 5
PuO2

12.56 17.33

FUTURIX 6
Pu0.30Zr0.70O2

15.44 27.94

2nd6.001h051015
Tim e (h)%weight Americium(gravimetry)
1st0.12 %5.99

Thermalinsulation

Infiltration

6.01%Am(calorimetry)

3rd17.57
30.69

30.07

Excellent agreement between gravimetry and calorimetry!!
9th IEMPT, 25-26 September 2006

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H. Ottmar, Nuclear Chemistry Unit

20

Laser flash for thermal properties
Pyrometer

SampleSample Holder
Furnance• high measurement precision for diffusivity (±1%)• simultaneous measurement of α and Cp (±5%)• highly localised measurements possible• samples with irregular shapes can be used

9th IEMPT, 25-26 September 2006

12D. Staicu, Materials Research Unit

LaserBeamLaser flash thermal conductivity measurements-1

Thermal conductivity, W m s-18060

Homogeneous (6% mol Am)

8(20% mol Am-YSZ) microdispersed in MgO(20% mol Am - YSZ) macrodispersed in MgO
20 % mol Am - PuO2 dipersed in Mo

620% mol Am -PuZrO2 dispersed in Mo

42600

800

1000

Temperature, K

9th IEMPT, 25-26 September 2006

13D.Staicu, Materials Research Unit

12001400

Vaporisation behaviour: Knudsen cell

9th IEMPT, 25-26 September 2006

14J.P Hiernaut, Materials Research Unit

Vaporisation behaviour
CERMET (Pu0.225Am0.240Zr0.534)O2-x-Molybdenum

1E-10237

Np
NpO
237
NpO2
237

1E-1190

Zr
ZrO
90
ZrO2

1E-10

90

239

Pu
PuO
239
PuO2

M.S.sig. (A)

M.S. sig. (A)

239

241

1E-12

Am
AmO
241
AmO2
241

1E-13

1E-14
1800

98

Mo

1E-11

1E-12

1900

2000

2100

2200

2300

Temperature (K)

9th IEMPT, 25-26 September 2006

152400

2500

2600

2100

2200

2300

2400

Temperature (K)

2500

2600

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

16

SMART irradiation in HFRSMART- 1 : (Pu0.090Zr0.757Y0.153)O1.92

Solid Solution

SMART- 2 : SSL + (Pu0.241Zr0.631Y0.128)O2-x Composite, microdispersed (60-80µm)•(Pu0.090Zr0.757Y0.153)O1.92

50 µm

1 mm

End of irradiation: mid 2007
PIE in ITU
9th IEMPT, 25-26 September 2006

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SS + (Pu0.241Zr0.631Y0.128)O2-x1 mm

250 µm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

9070

2Thermal conductivity, m s-1

8060
5040Futurix 5Futurix 63020
100600800

1000

Temperature, K

9th IEMPT, 25-26 September 2006

1812001400

HELIOS irradiation in HFR Petten(within IP EUROTRANS, CEA, NRG)

Fabrication of four fuels and pins for irradiation in HFR-Petten
FuelCompoundAm content*

Pu content*

g·cm3g·cm3

HELIOS 2

ZrYAmO2

0.76

HELIOS 3

ZrYPuAmO2

0.76

HELIOS 4

ZrYAmO2 + Mo

0.76

HELIOS 5

PuAmO2+ Mo

0.32

Particle size

Density

µm%TD

0.42
80-1001.28

90±520-150

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 )9th IEMPT, 25-26 September 200619HELIOS 2 pretest

HELIOS irradiation in HFR Petten(within IP EUROTRANS, CEA, NRG)

Addition of Carbon to the sol-gel feed solution
improve pellet microstructure

increase porosity (higher Am content by infiltration )82%TD

PuO2 infiltrated with Th
46

Infiltration solution 300gTh/lst
1 infiltrationnd
2 infiltration

44
4250 µm

Blackberry structure

94%TD

ThO2 infiltrated (% weight)

40
38
36
34
32
30
28
26
24
2220
18
16020

4060

Carbon content in sol-gel feed solution(g/l)

200 µm
9th IEMPT, 25-26 September 20062080

Collaborations
ACTINET• AMZrN• EXAFS on EFTTRAEFTTRA
CEA,NRG,FZK,EdF, IE

JRC- IRMM

Americium and fission products

Samples forcross section determinationtransmutation experiments

Concerted Action

Third Party Work

Transmutation European Networks
with ITU participation

CAMIX-COCHIX

P&T roadmap
PATEROS

Shared Cost Actions

GEN IVIMF Kernels for VHTR
Oxide fuels for FR

9th IEMPT, 25-26 September 2006

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P&T Experiments and studies• Nitride fuels experiment (CONFIRM)• Am transmutation in oxides (FUTURE)• Red-Impact• Pu burning in LWR (DEPUTY)

Integrated projects• EUROTRANS(FUTURIX, HELIOS)• EUROPART