Advanced Fuel Fabrication Processes for Transmutation A. - - PowerPoint PPT Presentation

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Advanced Fuel Fabrication Processes for Transmutation A. - - PowerPoint PPT Presentation

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1 10 IEMPT MITO October 2008 Advanced Fuel Fabrication Processes for Transmutation A. Fernandez-Carretero, C. Nstren, D. Staicu, J. Somers Nuclear Fuels Unit Institute for Transuranium Elements (ITU) Karlsruhe, Germany http://www.jrc.org/

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10 IEMPT MITO October 2008 1

Advanced Fuel Fabrication Processes for Transmutation

  • A. Fernandez-Carretero, C. Nästren, D. Staicu, J. Somers

Nuclear Fuels Unit

Institute for Transuranium Elements (ITU) Karlsruhe, Germany http://www.jrc.org/

http://itu.jrc.cec.eu.int/

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10 IEMPT MITO October 2008 2

The Nuclear Fuel Cycle

Enrichment Fuel Fabrication Reactor SNF Storage Processing High Level Waste Spent Nuclear Fuel Repository Uranium Storage Depleted Uranium Natural Uranium

reprocessin processing p plan ant U mining U mining nuclea nuclear reacto reactor spent fuel storage spent fuel storage repository repository

Fissile and Fertile (U,Pu,MA)

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10 IEMPT MITO October 2008 3

Outline

Introduction Difficulties in Fabricating MA fuels Sol Gel Routes - SUPERFACT Infiltration CERMETS/CERCERS Gen IV Oxides and Nitrides Conclusions

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10 IEMPT MITO October 2008 4

Implications of MA on the fabrication process

  • Shielded installations

→ remote handling

  • Automation → use of robots
  • Dust-free processes → avoid

the use of fine powders that produce dust that accumulates in the production cells

  • Process simplification

→ limit the number of (active) fabrication steps (e.g. vibrocompaction instead of pressing)

Nuclide Specific Activity Alpha Energy Gamma Energy SF (Bq/g) (MeV) (keV)

239Pu

2.29 109 5.156 0.07

237Np

2.610 107 4.79 29.4

241Am

1.271 1011 5.49 59.5

  • 242mAm

3.598 1011 5.20 49.4

243Am

7.391 109 5.28 74.7

  • 243Cm

1.911 1012 5.79 277.6

244Cm

2.997 1012 5.80 42.8

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10 IEMPT MITO October 2008 5

Transmutation Fuels

Fabrication facility: MA LAB

Isotope Limiting mass (g) a Criterion

231Pa

10 Shielding

237Np

  • b

241Am

50 License c

242mAm

0.1 Shielding

243Am

65 License c

244Cm

5 Shielding & licence c

a to yield max 2 µSv/h at 1 metre b no practical limit c corresponding to the dosis equivalent of 200 g Pu in the form of powder

(oxide)

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10 IEMPT MITO October 2008 6

Transmutation Fuels at the ITU MALAB

Since 2004 75 grams Am processed for fuel property and irradiation campaigns CAMIX-COCHIX FUTURE FUTURIX HELIOS Am cross section targets (c.f. Poster V-4 P. Rullhusen)

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10 IEMPT MITO October 2008 7

Transmutation Fuels

Presentation focuses on oxides, but active programmes on MA bearing metal fuels CRIEPI/ITU; INL MA bearing nitride fuels JAEA; LANL

Nitride/Carbide Fuel FabricationA

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10 IEMPT MITO October 2008 8

Transmutation Fuel Fabrication: Strategic choice at conversion step

Individual An Separation and Conversion (e.g. today at Sellafield and La Hague) U, Pu, Np, Am, Cm streams Group An Conversion Single U/Pu/Np/Am/Cm stream Selected An Separation and Conversion e.g. U, Pu/Np, Am/Cm Streams POWDER Metallurgy (LANL c.f. Pasemehmethogolu JAEA c.f Tanaka / Kato)) Sol Gel/Infiltration (ITU) Ox Precipitation (CEA c.f Poster III-1 Grandjean) Sol Gel (ITU)

(U0.65Pu0.30Am00.5)O2 fuel (Tanaka Global 2007)

Low dust routes

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10 IEMPT MITO October 2008 9

Outline

Introduction Difficulties in Fabricating MA fuels Sol Gel Routes - SUPERFACT Infiltration CERMETS/CERCERS Gen IV Oxides and Nitrides Conclusions

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10 IEMPT MITO October 2008 10

  • Fuel restructuring similar to standard fuel

irradiated under similar conditions

  • U and Pu did not show significant radial

re-distribution

  • Nodular oxide layer (few tens of microns)
  • n inner cladding
  • Reprocessing demonstrated

Typical observations for (U0.74Pu0.24Am00.2)O2 fuel:

SUPERFACT – As yet unsurpassed irradiation test (CEA/ITU)

Sol Gel conversion of (U,Pu,Am,Np solutions

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10 IEMPT MITO October 2008 11

Outline

Introduction Difficulties in Fabricating MA fuels Sol Gel Routes - SUPERFACT INFILTRATION CERMETS Gen IV Oxides and Nitrides Conclusions

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10 IEMPT MITO October 2008 12

Fuel Compound Am content* Pu content* Particle size Density g·cm3 g·cm3 µm %TD HELIOS 1 Am2Zr2O2-MgO 0.76 90 ± 5 HELIOS 2 ZrYAmO2 0.76 HELIOS 3 ZrYPuAmO2 0.76 0.42 HELIOS 4 ZrYAmO2 + Mo 0.76 80-100 HELIOS 5 PuAmO2+ Mo 0.32 1.28 20-150

HELIOS FUELS FABRICATED USING Sol Gel /Infiltration processes CEA ITU Sol Gel precursors (prepared in inactive

  • r Pu facilities)

(Zr,Y)O2 (Zr,Y,Pu)O2 (Zr,Y)O2 PuO2

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10 IEMPT MITO October 2008 13

Carbon addition improve microstructure improve infiltration behaviour YZrAmO2-x

HELIOS FUELS INFILTRATION ROUTE OPTIMISATION

Good visual aspect But microstructure→ cracks and large localised porosity

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10 IEMPT MITO October 2008 14

Droplet to Particle Conversion Calcination 20-225 µm Microspheres Thermal Treatment Actinide Solution Solution Infiltration Pressing Sintering Characterization Zr, Y solution (Helios 2,4) Zr, Y, Pu (Helios 3) Pu (Helios 5)

C

(Zr0.83Y0.17)O1.925

Helios 2

PuO2

Helios 5

Ma-Lab Mo powder

HELIOS 4 & 5

HELIOS FUELS: Fabrication Process Optimisation

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10 IEMPT MITO October 2008 15

Non uniform shrinkage cracks

CARBON ADDITION: Surface spalling, higher than normal mass loss Outgassing during sintering (Ar/H2) HELIOS FUELS INFILTRATION ROUTE OPTIMISATION Process modification Calcine 800 C (air) Infiltartion Calcine 800C (air) Pellet compaction Heat 1000 C (air) Sinter Ar/H2 CH4 or ???

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10 IEMPT MITO October 2008 16

HELIOS 2 Zr0.800Y0.134Am0.066O2-x 0.70 gAm•cm-3 92.6 ± 1.2 %TD 90.9 ± 0.3 %TD HELIOS 3 Zr0.767Y0.127Pu0.038Am0.068O2-x 0.74 gAm•cm-3 0.41 gPu•cm-3 89.7± 0.4 %TD 89.1 ± 1.1 %TD

HELIOS FUELS INFILTRATION ROUTE OPTIMISATION

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10 IEMPT MITO October 2008 17

CAMIX 1 HELIOS 2 Carbon addition

0,0 0,5 1,0 1,5 2,0 2,5 500 700 900 1100 1300 1500 Temperature (K) Thermal conductivity (W/m/K)

Thermal conductivity Helios 2 Thermal conductivity Camix 1

+ 40%

1 measured by Dragos Staicu (MR)

Carbon addition → improve microstructure → Improve Thermal Conductivity1

HELIOS FUELS: Characterization

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10 IEMPT MITO October 2008 18

New Design Transport carousel 5 pins Transport to HFR-Petten 11.10.2007 Beginning of Irradiation – October 2008

HELIOS FUELS: Pin fabrication & Transport

Contact (mSv/h) 1m (µSv/h) 1

175 105

2

66 42

3

58 43

4

36 22

5

12 6

Measured dose rate

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10 IEMPT MITO October 2008 19

Outline

Introduction Difficulties in Fabricating MA fuels Sol Gel Routes - SUPERFACT INFILTRATION CERMETS Gen IV Oxides and Nitrides Conclusions

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10 IEMPT MITO October 2008 20

Zr0.666Y0.111Am0.223O2-x + 71.3 %vol Mo 0.69 gAm•cm-3 94.2 ± 0.4 %TD HR = 4.83 HELIOS 4 Pu0.801Am0.199O2-x + 84.2 %vol Mo 0.295 gAm•cm-3 , 1.24 gPu•cm-3 95.9 ± 0.4 %TD HELIOS 5 HR = 12.01

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10 IEMPT MITO October 2008 21

Fabrication of porous PuO2 and (Zr0,705Pu0.295)O2 beads (100-200µm)

Conventional rotating cup

  • Pu concentration
  • Denitration
  • Viscosity
  • Rotating cup (rpm, height, etc)
  • Polydisperse size distribution

25%

FUTURIX fuels

PuO2 beads

FUTURIX CERMET fabrication (II): Sol-gel

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10 IEMPT MITO October 2008 22

Calculated from measured thermal diffusivity and specific heat. CERCER compared to CERMET

Thermal conductivity

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10 IEMPT MITO October 2008 23

CERMETS – cladding compatibility tests

Mo- (Pu,Am)O2-x (FX 5) Mo- (Zr,Pu,Am)O2-x (FX 6) Cladding

Compatibility test- T91

Cladding

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10 IEMPT MITO October 2008 24

Outline

Introduction Difficulties in Fabricating MA fuels Sol Gel Routes - SUPERFACT INFILTRATION CERMETS Gen IV Oxides and Nitrides Conclusions

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10 IEMPT MITO October 2008 25

U Pu C External Gelation Calcination Am Infiltration Calcination Carbothermal Reduction Sintering Pressing Conventional Gloveboxes Conventional Gloveboxes with Purified Atmospheres MALAB (U,Pu)O2 + AmO2 + C (U,Pu)O2 + C (U,Pu,Am)N

FR Nitride (Carbide) Fuel Production

Nitride/Carbide Fuel Fabrication

U0,805Pu0,175Am0,02N

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10 IEMPT MITO October 2008 26

NIMPHE Pu Isotopes 239 241 Am/(Pu+Am) % as starting material Pu as delivered 74,6 2,62 0,365 MA Production Losses : Particularly for carbides but also known for nitrides (LANL) Experience in NIMPHE2 Nitride 2pin 3 74,7 2,573 0,436 seems ok Carbide 2 pin 4 74,7 2,58 0,112 75% Am Losses!!

Nitride/Carbide Fuel Fabrication

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10 IEMPT MITO October 2008 27

Production Losses : Needs Vapor Pressure determination of Am over (U,Pu,Am)C New Lower Temperature Fabrication Routes Precursor to carbide or nitride directly Pyrochemistry through azide precipitation from molten salt Alternatives to carbothermal reduction?

Nitride/Carbide Fuel Fabrication

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10 IEMPT MITO October 2008 28

Outline

Introduction Difficulties in Fabricating MA fuels Sol Gel Routes - SUPERFACT Infiltration CERMETS Gen IV Oxides and Nitrides Conclusions

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10 IEMPT MITO October 2008 29

Transmutation Fuel Fabrication:

Options today Reprocessing: Aqueous or Pyro (potential for “and/or” especially of MC and MN) Fabrication: Separation strategy influences fabrication options (Homogeneous vs heterogeneous recycling)

  • Individual An Separation & Conversion
  • Partial An Separation & Conversion
  • Grouped An Separation & Conversion
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10 IEMPT MITO October 2008 30

Transmutation Fuel Fabrication:

Decisions must include plant concept Dust or not Production Scrap recycling Primary and secondary waste issues

Powder metallurgy -

Very flexible; dust

Grouped Oxalate precipitation - limited flexibility; dust Sol Gel - flexible if partial separation; limited flexibility for grouped separation; no dust Infiltration – Medium flexibility, partial separation needed, no dust

Microstructure attributes for Hi BU, He MGT, swelling……..

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10 IEMPT MITO October 2008 31

Outlook for the Future

Gen IV Fast Reactors and ADS Demo with MOX cores R&D for advanced MA bearing fuels Oxide, nitride, carbide Three Pillars for Fuel R&D recognised in the SNETP Strategic Research Agenda 1. Fabrication and basic properties of advanced fuels 2. Integral irradiation testing of fuel in appropriate advanced cladding materials 3. Separate effect studies and multiscale modelling approach Goals to be reached via National, European, Global research programmes

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10 IEMPT MITO October 2008 32

Fuels Research

2008 2020 2044

Decisions DEMO operating (1st Load MOX) Prototype DEMO with full MA compliment

  • Fab. and Prop MA fuels and targetsl

In DEMO testing MC, MN, MA Fuels Separate effects and multiscale modelling & simulation with integration in engineering codes

2020 2008 2044 2032 2032

Integral Testing MA fuels + Adv Cladding