Labonet Inaugural Meeting short presentation of concerned CEA/DEN teams. Jean-Philippe DANCAUSSE

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1 Labonet Inaugural Meeting short presentation of concerned CEA/DEN teams Jean-Philippe DANCAUSSE 1

2 Localization of concerned solid waste characterization laboratories and facilities Facilities Hot cells Glove boxes Equipments Neutron and gamma sources, Analytic instruments Code development Nuclear Energy Units based at SACLAY MARCOULE CADARACHE DEN

3 General scheme of solid waste characterization Radioactive solid waste package Non destructive characterizations Radiological (gamma spectro., passive imaging, Active and passive neutron measurement, Physical (active imaging, radiography and tomography) Elemental (neutron interrogation or activation) Gas measurements (radiolysis GPC, volatile RN) Sampling Inventory, cutting out, dry or wet drilling, Destructive characterizations Chemical and radio-chemical measurements (α, β and γ LLRN, actinides, water content, ) Physical measurements (resistance to compression, traction, water diffusion coefficient, gas permeability, density, porosity, leaching rate, ) 3

4 Non destructive characterization Research & Development Coupling measurement methods REGAIN Matrix characterisation by neutron activation ECT & TCT coupling Gamma radiography VANPIR interactive visualisation radio / tomo Measurements and Expertise PROMETHEE 6 Active neutron interrogation for waste drums TEMISEC Gamma emission tomography SYMETRIC Gamma spectrometry TRANSEC Radiography & Tomography SYMETRIC Active and passive neutron measurements 4

5 Non destructive characterization HE imagery with MINILINATRON: Expertise of bituminised packages on the BELGOPROCESS site EMECC Component contamination measurement by Under-water measurement spectrometry Leaktight shielded spectrometer holder BANGA : underwater gammaray spectroscopy on nuclear propulsion spent fuel (in the pool of the RES testing reactor) COQUINA: portable active neutron measurement unit MECANO Neutron measurement of residual uranium for the decommissioning of enrichment plants 5

6 Non destructive characterization Emission gas measurement from packages or samples Radiolysis gases ( H ( H,CO, CO, CH 4, )) = > gas chromatography measurement; ; (HCl( HCl) trapping in aqueous solution and chlorides chemical measurement Volatile radionuclides ( 3 H ( H H ( H et H O) et 14 C ) = > trapping in aqueous solutions and measurements in spectrometry beta 6

7 Sampling ALCESTE shielded cell Dry sampling of cores- Inventory Waste packages type A or B, up to m 3 Weigth < 10 ton, Activity < 7.4 TBq éq. To group 1 in radiotoxicity & Dose rate up to 10 Gy/h Inventory facilities Inventory, gas measurement,.. Waste packages type A or B, up to 5 ton Dose rate <mgy/h Activity < 4 GBq éq. To groupe 1in radio toxicity 7

8 GENERAL TREATEMENT OF THE SAMPLE DEVICES : - Dissolution Reactors; - Assisted digestion through microwave (open or closed systems) - Burn up under oxygen pressure; Alkaline melting, etc... TECHNIQUES: DESTRUCTION OF THE MATRIX SELECTIVE SEPARATION - Precipitation; Liquid-liquid extraction; - Ion exchange chromatography; Electro-chemistry; Addition of a tracer DETERMINATION OF THE YIELD TECHNIQUES: Analysis of the natural tracer with ICP-MS, ICP-AES or Radiochemical analysis TECHNIQUES: RADIOMETRIC ANALYSES - SPECTROMETRY : α, γ and X - LIQUID SCINTILLATION MASS SPECTROMETRY TECHNIQUES and COUPLING METHODS: - ICP-Q-MS; - ETV-ICP-Q-MS; - ICP-SF-MS in white room DEVELOPEMENT OF ONE METHOD FOR EACH MATRIX AND EACH RADIONUCLIDE 8

9 Some of the destructive techniques Mass Spectrometry ICP-MS-Q- analyse = 1 nuclearised + 3 ICP-MS-MC ( x1 nuclearised) Thermoionisation (x3 nuclearised) ICP-MS-HR : couplage microhplc x1 LC-ESI-MS Separative methods gravimetric chromatography x5 glove box dedicated HPLC with UV and liquid scintillation detection x1 glove box ionic chromatography (anions, cations) micro, nano- chromatography Capillary electrophoresis Elemental analysis Atomic Absorption ICP-AES Hg Analyser Radiometric detection α spectrometry, γ-x spectrometry, αβ counting, Liquid scintillation 9

10 Destructive characterization Radio - Hal-life Methods nuclides (years) 10 Be, ICP/MS 14 C 5, L.S 36 Cl 3, L.S 59 Ni 7, X 63 Ni 1,0.10 L.S. 79 Se 3, ETV -ICP/MS 93 Zr 1, ICP/MS complementary techniques α, γ Spectrometry, liquid scintillation ICP/MS, ICP/MS-ETV, ICP/SFMS 93 Mo 3, X 94 Nb, γ 99 Tc, ICP/MS 107 Pd 6, ETV -ICP/MS 108m Ag 4,4.10 γ 11m Sn 55 L.S 16 Sn, ICP/MS 19 I 1, ICP/MS 135 Cs, ETV -ICP/MS 151 Sm 90 L.S Half time (years) 1,E+08 1,E+07 1,E+06 1,E+05 1,E+04 1,E+03 1,E+0 1,E+01 1,E+00 Radiochemistry ICP/MS 11mSn 151Sm 63Ni 108mAg 93Mo 14C 94Nb 79Se 59Ni 16Sn Radionuclide 99Tc 36Cl 93Zr 135Cs 10Be 107Pd 19I 10

11 Destructive characterization Preparation Analytical processes for the radionucléides measurement (A~100mBq.g -1 ) RN : 3 H, 14 C, 59 Ni, 90 Sr, 41 Pu, Pu, 38 Pu, 108m Ag, 43 Am, 41 Am, 3 U, 34 U, 35 U, 38 U, 10 Be, 36 Cl, 55 Fe, 63 Ni, 93 Mo, 93 Zr, 94 Nb, 19 I, 107 Pd, 151 Sm. Fractionning Grinding Drying Dilution Medium Change Spiker/Carrier addition From 10 4 to 10 8 Bq/g Dissolution Pyrolysis Alcalin Fusion Nitric Attack Mineralisation under micro-wave flux Parr Bomb Combustion Separation/ Extraction/ Purification Co-precipitation Specific column Chromatography HPLC Specific molecules spiking liquid/liquid extraction Measurement Ionic Chromatography AAS, ICP-AES ICP-MS Gravimetry Alpha, bêta counting Alpha, gamma spectrometry Liquid Scintillation Counting 0.01 to 1 Bq/g 11

12 Destructive characterization Nitrogen permeability = > gas exhaust from waste packages QLPµ 0 k= S( P P) 1 k : le coefficient de perméabilité intrinsèque du matériau (m²), av L épaisseur du matériau (m) µ viscosité dynamique du gaz (Pa.s) P1 pression appliquée en entrée (Pa) P pression en sortie (Pa) P0 pression atmosphérique (Pa) S surface (m²) Q débit mesuré en m 3 /s perméabilité K=f(taux de saturation S) échantillons coques et bouchons p erm éab ilité K (m ²) E-16 1,5E-16 1E-16 5E taux de saturation S (%) 0 CV1a CV1g CVa CV1 coque Permeability measurements according to several level of moisture of the porous solid 1

13 Destructive characterization Resistance to compression = > Resistance to the stacking of waste packages AFNOR norm NF-P with sulfuring ajustment AFNOR norm NF-P Power press 100 ton in a nuclear glove box Power press 50 kn in a shielded cell 13

14 Destructive characterization Water diffusion coefficient (D e ) (mortar, concrete,..) => containment in wet medium of waste packages Upper compartment tritiated water D e Downstream compartment Q( t). L C 0 α. L = De. t 6 α. L π n= 1 ( 1) n n e n π t De α. L C 0 Q(t) (3, Bq/m 3 ) Transfert Activity (Bq/m 3 ) Balance mass transfer L 1,6E-05 1,4E-05 1,E-05 1,0E-05 8,0E-06 Q(t)L/Co (m²) Modèle Expérience Régime transitoire Régime permanent 6,0E-06 4,0E-06,0E temps (j) 0,0E+00 14

15 Destructive characterization Water diffusion coefficient (D e ) (mortar, concrete,..) => containment in wet medium of waste packages Upper compartment tritiated water D e Downstream compartment Q( t). L C 0 α. L = De. t 6 α. L π n= 1 ( 1) n n e n π t De α. L C 0 / Q(t) (3, Bq/m 3 ) Transfert Activity (Bq/m 3 ) Balance mass transfer L 1,6E-05 1,4E-05 1,E-05 1,0E-05 8,0E-06 Q(t)L/Co (m²) Modèle Expérience Régime transitoire Régime permanent 6,0E-06 4,0E-06,0E temps (j) 0,0E+00 15

16 Destructive characterization Measurements realized on sample or all the package (Scale 1) Leaching rate =>salting out of radionuclides Radioactivity kinetic leaching measurement of waste enrobement in a concrete water 0,08 Sb15E14 Sb15E4 Co60E0 Sb15E0 Co60E14 Co60E4 E14 E0 LIME WATER E4 WATER Cs134E14 Cs134E0 Cs134E4 Cs137E14 Cs137E0 Cs137E4 Lixiviated Fraction 0,04 0, Time (Days) L F = lixiviated activity / total activity of sample 16

17 Waste producers to storage through «super-controls» Producers Compactage des futs Injection des caissons e barrière l ouvrage de stockage 1 ère barrière le colis 3e barrière l environnement géologique Non destructive characterization Destructive characterization and technical tests CCMES* Super control results Chemical and radiochemical analysis 17