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Nuclear Fuels CRUD Analysis. Analytical S trategies Yannick Suter & Helene Wolleb 24 th September 2013. Table of contents. Nuclear power plant CRUD Sampling Analysis Waste treatment. Operation Mode of a Nuclear Power Plant.

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nuclear fuels crud analysis

NuclearFuelsCRUD Analysis

Analytical Strategies

Yannick Suter & Helene Wolleb

24th September 2013

Yannick Suter & Helene Wolleb

table of contents
Table ofcontents
  • Nuclear power plant
  • CRUD
  • Sampling
  • Analysis
  • Wastetreatment

Yannick Suter & Helene Wolleb

operation mode of a nuclear power plant
Operation Mode of a Nuclear Power Plant
  • Conversionof thermal energyreleasedfromnuclearfission
  • Nuclearandconventionalpart
  • Fissile atomicnuclei: Uranium-235
  • Controlwithneutronmoderators
  • Nuclearchainreaction

Yannick Suter & Helene Wolleb

http://www.kernenergie.ch/de/akw-technik.html#anchor_ZXDVQE, 20.09.2013.

operation mode of a nuclear power plant1
Operation Mode of a Nuclear Power Plant
  • In Switzerland: Light waterreactors
  • Leibstadt: Boilingwaterreactor

Yannick Suter & Helene Wolleb

operation mode of a nuclear power plant2
Operation Mode of a Nuclear Power Plant

Yannick Suter & Helene Wolleb

http://upload.wikimedia.org/wikipedia/commons/1/15/Boiling_water_reactor_english.svg, 20.09.2013.

crud what is it
CRUD – Whatisit?
  • Deposition of solid phaseproducts on thefuelcladding
  • Corrosionproductsandadditionstofeedwater
  • Main expectedelements: Fe, Zn, Ni, Cr, Co, Cu
  • γ-activities: 60Co, 54Mn, 125Sb, 65Zn

Yannick Suter & Helene Wolleb

I. Günther-Leopold et al., Progress Report 2005–2006, Laboratory for Materials Behaviour (LWV), PSI, 13.

crud problems
CRUD – Problems
  • Magnetic CRUD: Interferencewithdeterminationofoxidethicknesslayer
  • Pickup of hydrogen in thecladding material
  • Limitingfactorforthelifetimeoffuelassemblies
  • Radioactivecorrosionproducts: Occupationalradiationexposure

Yannick Suter & Helene Wolleb

S. Abolhassaniet al., Progress Report 2005–2006, Laboratory for Materials Behaviour (LWV), PSI, 12.

radioactivity
Radioactivity
  • Ionizingradiation
  • Eitherparticles (α, β, n, p+) orelectromagneticwaves (hard X-ray, γ)

Yannick Suter & Helene Wolleb

Grundlagen A, Kompetenzzentrum ABC-KAMIR, 30.07.2012.

radioactivity1
Radioactivity
  • Activitygivenbythenumberofdesintegrations per time [Bq = s-1]
  • Radiativeuptakegivenbytheabsorbedenergy dose [Gy = J/kg]
  • Equivalent dose andeffective dose givenasabsorbed dose multipliedwithweightingfactorsfortissueandradiation type [Sv = J/kg]
  • Usuallymeasuredas dose rates [Sv/h]

Yannick Suter & Helene Wolleb

Grundlagen A, Kompetenzzentrum ABC-KAMIR, 30.07.2012.

radioactivity2
Radioactivity
  • Meanannual dose in Switzerland: ~4-5 mSv
  • 1 Svaccountsfor a rise in cancerprobabilityby 4%
  • Fixed limitingvaluesforman-made radiation

Yannick Suter & Helene Wolleb

Grundlagen A, Kompetenzzentrum ABC-KAMIR, 30.07.2012.

sampling general strategy
Sampling – General Strategy
  • Sampling duringannualreactorshutdown
  • Sampling insidethereactorcore
  • Fuel rodshould not bedamaged

Yannick Suter & Helene Wolleb

sampling general strategy1
Sampling – General Strategy
  • Compositionof CRUD
  • Spatialvarianceof CRUD
  • Radioactivityof CRUD

Yannick Suter & Helene Wolleb

sampling general strategy2
Sampling – General Strategy
  • Non-destructive in-situ measurements on CRUD difficult (e.g. EDX or XRF)
  • Howtoget a representative sample of CRUD?
  • Depth-profilingwouldrequire a solid sample

Yannick Suter & Helene Wolleb

sampling risk potential
Sampling – Risk Potential
  • Stronglyradiativeenvironment
  • Sample cancontainvirtuallyanyelement (in theory)

Yannick Suter & Helene Wolleb

sampling risk potential1
Sampling – Risk Potential
  • Release ofradioactivematerial
  • Radiation uptakebyworkingstaff
  • Incorporationorinhalationofradioactive material
  • Productionofradioactivewastewhichneedsfurtherprocessing

Yannick Suter & Helene Wolleb

sampling risk potential2
Sampling – Risk Potential
  • Handling insidehotcells
  • Special requirementsfortransportation

Yannick Suter & Helene Wolleb

http://www.psi.ch/media/knowledge-for-tomorrow-from-hot-cells, 20.09.2013.

sampling sample preparation
Sampling – Sample Preparation
  • CRUD isscraped off thecladdingsurfaceinsidethereactorcore
  • Material collectedbymembranefilters
  • Filters dissolved in concentrated HNO3, H2O2and HF in a microwavedigestionsystem

Yannick Suter & Helene Wolleb

I. Günther-Leopold et al., Progress Report 2005–2006, Laboratory for Materials Behaviour (LWV), PSI, 13.

analysis corrosion layer sims
Analysis – Corrosion Layer (SIMS)
  • Problem: Howtoget a solid sample ofthe wall?
  • A solid sample wouldbemoredifficulttoquantifycorrectly
  • Roughprofilecouldbemadeif CRUD iscollectedfromthe same spot

Yannick Suter & Helene Wolleb

analysis icp ms
Analysis – ICP-MS
  • Liquid sample: Micronebulizer
  • InductivelyCoupled Plasma
  • Interface: Sample coneandskimmercone
  • Quadrupole MS
  • Sectorfield MS
  • Detection: Multiple ioncollector

Yannick Suter & Helene Wolleb

D. Güntheret al., SkriptAnalytischeChemie I + II, ETH Zürich, 2011.

analysis icp ms1
Analysis – ICP-MS

Yannick Suter & Helene Wolleb

http://www.chem.agilent.com/en-US/products-services/Instruments-Systems/Mass-Spectrometry/Pages/gp455.aspx, 20.09.2013.

analysis icp ms2
Analysis – ICP-MS
  • Isotopicdifferentiationpossible
  • Low limitsofdetection (usually ppb)
  • Quantificationpossible

Yannick Suter & Helene Wolleb

http://www.chem.agilent.com/en-US/products-services/Instruments-Systems/Mass-Spectrometry/Pages/gp455.aspx, 20.09.2013.

analysis icp ms3
Analysis – ICP-MS
  • Major problem: Interferences

- Example: Isobaricinterferenceof90Sr with90Zr

  • Solutions:

- Double-focusingsectorfield ICP-MS

- ICP-MS withcollisioncell

- Applicationofcouplingtechniques, e.g. ionchromatography

Yannick Suter & Helene Wolleb

J. S. Becker, International Journal of Mass Spectrometry2005, 242, 183-195.

analysis icp ms4
Analysis – ICP-MS
  • Issues due toradioactivity:

- Nospecialsafetymeasuresforhighlydilutedsamples

- Detectoristreatedasradioactivewaste

Yannick Suter & Helene Wolleb

.

analysis geiger counter
Analysis - Geiger Counter
  • First analysisofγ-radiation
  • Measuresthe dose rate [Sv/h]

Yannick Suter & Helene Wolleb

Automation und Messtechnik GmbH, Gebrauchsanweisung für den Dosis-

leistungsmesser 6150AD, 26.10.2005.

analysis geiger counter1
Analysis - Geiger Counter
  • Countingtube
  • An X-rayorγphotonionizes an argonatom; onlydetectsradiation in a certainenergyrange
  • Noinformationaboutthe radioisotopes

Yannick Suter & Helene Wolleb

Automation und Messtechnik GmbH, Gebrauchsanweisung für den Dosis-

leistungsmesser 6150AD, 26.10.2005.

analysis spectroscopy
Analysis – γ-Spectroscopy
  • Energyofγ-photons characteristicforeachradioisotope

Yannick Suter & Helene Wolleb

analysis spectroscopy1
Analysis – γ-Spectroscopy

Yannick Suter & Helene Wolleb

http://de.wikipedia.org/wiki/Gammaspektroskopie, 20.09.2013.

analysis spectroscopy2
Analysis – γ-Spectroscopy
  • Energymeasurement:- Scintillationdetector (e.g. NaI)- Semiconductor (e.g. pure Ge)

Yannick Suter & Helene Wolleb

http://www.psi.ch/asi/radioanalytik, 20.09.2013.

analysis spectroscopy3
Analysis – γ-Spectroscopy
  • Energycalibrationneeded
  • Quantificationpossibleifcalibrationsourceofknownactivityavailable (detectorefficiency)
  • Usuallysmallmatrixeffects, specially in liquids

Yannick Suter & Helene Wolleb

analysis spectroscopy4
Analysis – γ-Spectroscopy
  • Elements withoutγradiationcannotbemeasured (3H, 14C)
  • Not reallysuitedforactinidesα-spectroscopy
  • High-energyγradiationcannotbemeasured due tothe pair-effect
  • All β+decaysproducetheannihilationlineat 511 keV

Yannick Suter & Helene Wolleb

Grundlagen der γ-Spektroskopie, Kompetenzzentrum ABC-KAMIR, 14.09.2012.

waste treatment
Waste Treatment
  • Strahlenschutzverordnung, Stand 2008

- Short half life: Wastestorageatproductionsite

- Long half life: Collectingpointisthe PSI

- PSI organizes intermediate storage

Yannick Suter & Helene Wolleb

further remarks and summary
Further RemarksandSummary
  • Reductionof CRUD
  • Zincinjection: Preventionofrustformation
  • Analysis of CRUD is essential forqualitycontrol
  • ICP-MS in combinationwithγ-spectroscopy
  • Data validation: Comparison, analysisofreferencesamples

Yannick Suter & Helene Wolleb

G. Ledergerber et al., J. Nuc. Sci. Tech. 2006, 43, 1006-1014.

thank you for your attention
Thankyouforyourattention!

Are thereanyquestions?

Yannick Suter & Helene Wolleb

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