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/


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


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


(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


Outline






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


HOMOGENEOUS fuels & targets

Pressing

Sintering

Actinide SolutionSolution Infiltration

Zr,Y Nitrate Solution

Droplet to ParticleConversion

Microspheres

ThermalTreatment

Pressing

Sintering




Microspheres

ThermalTreatment

(Zr0.83Y0.17)O1.925

Am0.06Y0.16 Zr 0.78O2-x


COMPOSITES : CERCER and CERMET

40-60µm

80-100µm

microdispersion

macrodispersion

sieving

MgO/Mo Powder

Granulation

Mixing

Granulation

Mixing

Pressing

Sintering




Microspheres

ThermalTreatment

Blending

Pressing

Sintering




Microspheres

ThermalTreatment

Blending

250 µm


• 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)


Outline






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



Thermalinsulation



ΔT ⇒ ΔV ∝ Q

Thermal resistance



Thermalinsulation



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


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


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


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


Outline






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


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


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


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


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

Overview of ITU work on inert matrix fuels · 2006-10-02 · Overview of ITU work on inert matrix...

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