LES MESURES NUCLÉAIRES NON DESTRUCTIVES POUR LE CONTRÔLE DES DÉCHETS RADIOACTIFS, L ASSAINISSEMENT ET LE DÉMANTÈLEMENT DES INSTALLATIONS

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1 LES MESURES NUCLÉAIRES NON DESTRUCTIVES POUR LE CONTRÔLE DES DÉCHETS RADIOACTIFS, L ASSAINISSEMENT ET LE DÉMANTÈLEMENT DES INSTALLATIONS Bertrand PEROT, CEA DEN CADARACHE EFFMIN 4 MARSEILLE, FRANCE JUILLET 2016 EFFMIN4 MARSEILLE JUILLET PAGE

2 CONTENTS Photon imaging Gamma-ray spectroscopy Passive and active neutron measurements Coupling measurement results R&D on new techniques EFFMIN4 MARSEILLE JUILLET 2016 PAGE 2

3 TRANSMISSION RADIOGRAPHY AND DENSITOMETRY LINAC 60 Co source E ~ 1.25MeV Detection system PAGE 3 ln 0 ( E ) / L 0 Photon source EFFMIN4 MARSEILLE JUILLET 2016 PAGE 3

4 PHOTON TRANSMISSION TOMOGRAPHY Projections >1000 on 360 Reconstructed 2D cross sections EFFMIN4 MARSEILLE JUILLET 2016 PAGE 4

5 60 CO IMAGING: PRECISE DENSITY BUT LONG TRANSEC: historic 60 Co tomography system of LMN, CEA DEN CADARACHE 50 mm 120 mm 190 mm 260 mm 330 mm 400 mm 470 mm 540 mm Density mm 680 mm 750 mm 820 mm EFFMIN4 MARSEILLE JUILLET 2016 PAGE 5

6 HIGH ENERGY X-RAY IMAGING WITH A LINAC Bremsstrahlung X-ray beam LINAC Lead collimator Object (waste drum ) Scintillation plate Mirror CCD camera CINPHONIE: recent high energy imaging system of LMN, CEA DEN CAD CINPHONIE Vs. TRANSEC: Radiography: 240 faster (40 h 10 min) Tomography: 36 faster (15 h 25 min) 9 MeV LINAC (15 Gy/min at 1m) Moving platform (up to 2 tons) Scintillation plate (800 x 600 mm²) Gadox Gd 2 O 2 S ; 1.5 mm Nicolas Estre, Daniel Eck, Jean-Luc Pettier, Emmanuel Payan, Christophe Roure and Eric Simon, High-Energy X-Ray Imaging Applied to Non Destructive Characterization of Large Nuclear Waste Drums, ANIMMA 2013, June 2013, Marseille, France PAGE 6

7 HIGH ENERGY IMAGING OF LARGE CONCRETE DRUMS Concrete waste: density > 2 Less than 1 s per single radiography Radiography Tomography 1,2 tonne H=1,2m =0,84m EFFMIN4 MARSEILLE JUILLET 2016 PAGE 7

8 IN SITU HIGH ENERGY X-RAY IMAGING Bituminized waste drum characterization at BELGOPROCESS facility, Belgium Radioscopy of the corium - water interaction Nuclear accident studies, KROTOS facility, CEA Cadarache Water surface EFFMIN4 MARSEILLE JUILLET 2016 PAGE 8

9 COMPUTED GAMMA EMISSION TOMOGRAPHY?????????????????????????????????????? Transmission tomography 2D density map Gamma spectra Sinogram R. Thierry, J.L Pettier and L. Desbat, Simultaneous compensation for attenuation, scatter and detector response for 2D-emission tomography on nuclear waste with reduced data, 1 st World Congress on Industrial Process Tomography, Buxton, Greater Manchester, April 14-17, E1 : , 1999 Emission tomography 2D activity map PAGE 9

10 PHOTON IMAGING GAMMA SPECTROSCOPY PASSIVE AND ACTIVE NEUTRON MEASUREMENTS COMBINED MEASUREMENTS R&D EFFMIN4 MARSEILLE CEA JUILLET PAGE 10

11 GAMMA-RAY SPECTROSCOPY Radioactive object (e.g. a waste package) Detector and electronics A Gamma spectrum A ( E ) Activity Sn ( E ) ( E ) I( E ) T Net area S n Sn(E) Compton background EFFMIN4 MARSEILLE JUILLET 2016 PAGE 11

12 RADIOACTIVE WASTE CHARACTERIZATION Specific gamma spectroscopy stations the laboratory Part of combined measurements e.g. for ANDRA Super-Controls with X-ray imaging and neutron assay EFFMIN4 MARSEILLE JUILLET 2016 PAGE 12

13 IN SITU SPECTROSCOPY IN NUCLEAR REACTORS Historic activity > 300 campaigns (end of 70 s) EDF and foreign power plants EMECC device & software Intermediate activities (1 MBq/m² 100 GBq/m²) Pipes, steam generators, heat exchangers Characterization of a whole plant (all circuits) EMECC Deposited or volumetric activities (GBq / m² or m 3 ) Experimental qualification by EDF Support to OSCAR contamination transfer code Steam generator spectra (Ge vs. CZT) EFFMIN4 MARSEILLE JUILLET 2016 PAGE 13

14 IN SITU SPECTROSCOPY OF LARGE COMPONENTS Uranium hold-up measurement in a heat exchanger Segmented gamma spectrometry Vessel contamination and activation Underwater HP Ge gamma-ray spectroscopy SFR cold trap characterization HP Ge + CZT in inspection hall Characterization of activated components TORE SUPRA wastes HP Ge EFFMIN4 MARSEILLE JUILLET 2016 PAGE 14

15 IN SITU SPECTROSCOPY OF NUCLEAR MATERIALS Dismantling operations Fuel fabrication and reprocessing units Fissile mass estimation in a reprocessing unit HP Ge detector isotopic composition, activity or mass CZT probe introduced in glove boxes localization Characterization of Pu in glove boxes of a Pu fuel fabrication facility HP Ge detector CZT probe EFFMIN4 MARSEILLE JUILLET 2016 PAGE 15

16 IN SITU SPECTROSCOPY FOR BUILDINGS Inside After removing all components Outside Walls control High efficiency HP Ge with tungsten shield EFFMIN4 MARSEILLE JUILLET 2016 PAGE 16

17 PHOTON IMAGING GAMMA SPECTROSCOPY PASSIVE AND ACTIVE NEUTRON MEASUREMENTS COMBINED MEASUREMENTS R&D EFFMIN4 MARSEILLE CEA JUILLET PAGE 17

18 MIXED PASSIVE & ACTIVE NEUTRON CELL (R&D) PROMETHEE VI R&D cell LMN, CEA DEN Cadarache Christian Passard et al., PROMETHEE: An Alpha Low Level Waste Assay System Using Passive And Active Neutron Measurement Methods, NUCLEAR TECHNOLOGY VOL. 140 DEC A. Mariani et al., The help of simulation codes in designing waste assay systems using neutron measurement methods: Application to the alpha low level waste assay system PROMETHEE 6, Nuclear Instruments and Methods in Physics Research B 211 (2003) Fanny Jallu et al., Alpha-Particle Low-Level Waste Control: Improvement of the PROMETHEE 6 Assay System Performances, Nuclear Technology Vol. 153 Jan EFFMIN4 MARSEILLE JUILLET 2016 PAGE 18

19 PASSIVE NEUTRON MEASUREMENT Total counting Spontaneous fission + (,n) neutrons 242 and 244 Cm, 238, 240 and 242 Pu, 241 Am (+ 238 U if mass > kg) Coincidence counting Spontaneous fission neutrons only 242 and 244 Cm, 238, 240 and 242 Pu (+ 238 U) Counts Real coincidences R A Accidental coincidences A A Time R+A Gate a few 10 µs Delay 1 ms A Gate (same duration as R+A gate) EFFMIN4 MARSEILLE JUILLET 2016 PAGE 19

20 ACTIVE DIFFERENTIAL DIE AWAY TECHNIQUE Prompt zone de mesure des neutrons prompts de neutrons fission zone mixte Background Bruit de fond uranium 235 m = 30 mg uranium 235 m = 60 mg uranium 235 m = 122 mg uranium 235 m = 242 mg Signal (c/s) 1000 Delayed zone de mesure des neutrons retardés de fission neutrons zone de saturation des chaînes d'acquisition inexploitable Temps Time après after l'impulsion neutron pulse de neutrons (s) (µs) Prompt and delayed neutron signals 235 U and 239 Pu discrimination Prompts neutrons 235 U, 239 and 241 Pu Delayed neutrons 235 U, 239 and 241 Pu U and 232 Th EFFMIN4 MARSEILLE JUILLET 2016 PAGE 20

21 CALIBRATION WITH DIFFERENT MATRIX MATERIALS Passive detection Active neutron signal F. Jallu et al. / Nuclear Instruments and Methods in Physics Research B 271 (2012) A.-C. Raoux et al. / Nuclear Instruments and Methods in Physics Research B 266 (2008) R. Antoni et al. Matrix effect correction with internal flux monitor in radiation waste characterization with the Differential Die-away Technique, IEEE Transactions on Nuclear Science, Vol. 61, No. 4 (2014) EFFMIN4 MARSEILLE JUILLET 2016 PAGE 21

22 PASSIVE & ACTIVE NEUTRON CELL Pulsed DT neutron generator GENIE 36 SODERN, n/s Polyethylene Graphite Neutron generator Lead ring around the generator Turntable 99 3 He counters in 3 detection blocks (CH 2 + Cd) empty cell ~ 23% Lead shield Graphite SYMETRIC measurement cell LMN, CEA DEN Cadarache ANDRA -CEA Super-controls EFFMIN4 MARSEILLE JUILLET 2016 PAGE 22

23 IN SITU PASSIVE / ACTIVE NEUTRON SYSTEMS PACCMAN, COQUINA: active neutron interrogation systems plugged to hot cells to assess Pu and U in high level wastes 3 He+CH 2 +Cd detection blocks Graphite measurement cavity Neutron generator (hole) Detection blocks (U shape) Neutron generator in a graphite reflector PACCMAN COQUINA LMN, CEA DEN CADARACHE ATALANTE, CEA DEN MARCOULE EFFMIN4 MARSEILLE JUILLET 2016 PAGE 23

24 IN SITU NEUTRON MEASUREMENTS Characterization of large components in uranium enrichment facilities (UF 6 gas diffusion technology) Passive neutron measurement of the uranium hold-up in UF 6 compressors Passive (and active) neutron measurements of uranium holdup in an UF 6 crystallizer Measurement of the uranium enrichment in an UF 6 container by active neutron interrogation F. Jallu et al., Dismantling and decommissioning: The interest of passive neutron measurement to control and characterise radioactive wastes containing uranium, Nuclear Instruments and Methods in Physics Research B 271 (2012) EFFMIN4 MARSEILLE JUILLET 2016 PAGE 24

25 PHOTON IMAGING GAMMA SPECTROSCOPY PASSIVE AND ACTIVE NEUTRON MEASUREMENTS COMBINED MEASUREMENTS R&D EFFMIN4 MARSEILLE CEA JUILLET PAGE 25

26 RADIOACTIVE WASTE CARACTERISATION X-RAY RADIOGRAPHY + SPECTROSCOPY + PASSIVE NEUTRON COUNTING X-ray radiography PEGAZE 100 L historic waste drums, CEA DEN CADARACHE -ray Spectro. Passive Neutron Coinc. Counting F. Jallu et al. / Nuclear Instruments and Methods in Physics Research B 271 (2012) EFFMIN4 MARSEILLE JUILLET 2016 PAGE 26

27 COMBINED MEASUREMENT SYSTEM RADIOGRAPHY + SPECTROSCOPY + ACTIVE & PASSIVE NEUTRON CELL > 60,000 historic 225 L bituminized waste drums (Marcoule, France) Non Destructive Assay performance study Low resolution gamma radiography ( 60 Co) BGO detector + Fe collimator 60 Co source + lead plates Filling height Matrix density Gamma spectroscopy, radionuclides 241 Am activity Coaxial HP Ge (100% rel. eff.) Planar HP Ge + BGO Compton suppression Passive & active neutron cell Pu, U Graphite and polyethylene cell 99 3 He counters + Pb and Cd shields Pulsed n/s neutron generator Open geometry + lead shield Waste drum Iron collimators B. Pérot, J.-L. Artaud, C. Passard, A.-C. Raoux, Experimental Qualification With a Scale One Mock-Up of the Measurement and Sorting Unit for Bituminized Waste Drums, PAGE 27

28 COUPLING MEASUREMENT RESULTS Neutron measurements passive active Gamma imaging Density, filling height Gamma-ray spectroscopy U, Th 240 Pu 239 Pu Waste production data Matrix composition, homogeneity Isotopic composition of U and Pu Ratios between beta-gamma RNs and non detectable radionuclides Total alpha activity 241 Am Individual beta activities 137 Cs, 60 Co, 154 Eu... PAGE 28

29 PHOTON IMAGING GAMMA SPECTROSCOPY PASSIVE AND ACTIVE NEUTRON MEASUREMENTS COMBINED MEASUREMENTS A FEW R&D TOPICS EFFMIN4 MARSEILLE CEA JUILLET PAGE 29

30 DUAL ENERGY IMAGING (SATURNE LINAC PROJECT) Mass attenuation coefficient µ/ LINAC acquisitions at 15 MeV and 9 MeV µ 15MeV (E~ 6 MeV) / µ 6MeV (E~4 MeV) Atomic number Z (simulation of a 870 L drum) 3 Density (simulation of a 870 L drum) EFFMIN4 MARSEILLE JUILLET 2016 PAGE 30

31 HIGH ENERGY X-RAY TOMODENSITOMETRY Attenuation up to 5 decades (40 cm steel) Radiography and 2D plane tomography 3D helicoidally tomography 0.5 to 2 mm spatial resolution 1 h (2D) to several days (3D) acquisitions Collimated CdTe detectors Simulations of a 5 m 3 concrete waste package 9 MeV LINAC 15 MeV LINAC EFFMIN4 MARSEILLE JUILLET 2016 PAGE 31

32 ACTIVE PHOTON INTERROGATION: PHOTOFISSION U and Pu measurement in large concrete waste packages High energy X rays produced by an electron LINAC (photofission threshold ~ 6 MeV) Delayed neutron counting between the pulses Delayed gamma-ray spectroscopy after stopping irradiation Setup with 5 HP Ge detectors 100 g U in the center of the 870L drum 2h irradiation + 3h counting Useful delayed gamma signal (MCNP simulation) Waste package passive gamma background 15 MV Linac beam (870 L drum) U in the center Background & detection limit - 1 detector Backgr. & detection limit - 5 detector cluster ray (kev) B (counts) L D (counts) L D (g 235 U) B (counts) L D (counts) L D (g 235 U) , , , , , , , , , , , , , , , , , , , , , , , ,00 E. Simon, F. Jallu, B. Pérot, S. Plumeri, Feasibility study of fissile mass quantification by photofission delayed gamma rays in radioactive waste packages using MCNPX, submitted to Nuclear Instruments and Methods in Physics Research A PAGE 32

33 NEUTRON ACTIVATION ANALYSIS Toxic chemical or matrix material characterization in radioactive wastes PGNAA Prompt Gamma Neutron Activation Analysis Pulsed neutron generator + HP Ge gamma-ray detector Neutron flux A few 10 µs Up to few ms Time Fast neutrons during the pulses (n,n ) Thermal neutrons between pulses (n,) (+ deactivation gamma rays after irradiation) Mercury sample Mercury nitrate sample No sample Difference Hg capture gamma rays Hg sample Neutron generator 30% HPGe with 6 Li shield J.-L. Ma et al., Prompt Gamma Neutron Activation Analysis of toxic elements in radioactive waste packages, Applied Radiation and Isotopes 70 (2012) 1261 REGAIN cell, CEA DEN CAD, LMN EFFMIN4 MARSEILLE JUILLET 2016 PAGE 33

34 CEA- FZJ COLLABORATION ON PGNAA MEDINA PGNAA cell FZJ, Germany, GENIE 16 neutron generator and ~ 100% HP Ge EXP / MCNP comparisons MCNP performance optimization Fission delayed (see next slide) POSTER Tangi NICOL EFFMIN 4 tangi.nicol@cea.fr T.Nicol, C. Carasco, B. Perot, J.L. Ma, E. Payan et al., Quantitative comparison between PGNAA measurements and MCNPX simulations, Journal of Radioanalytical and Nuclear Chemistry, DOI /s PAGE 34

35 NEUTRON-INDUCED FISSION DELAYED -RAY YIELDS Gamma spectra of 235 U and 239 Pu samples measured in REGAIN between neutron pulses 95 Y 235 U 239 Pu 90 Rb- 90m Rb 132 Sb- 132m Sb 89 Rb REGAIN and its MCNP model 94 Sr 136 I- 136m I Gamma spectra after irradiation Low background -spectroscopy lead shelter 89 Rb 89 Rb 92 Sr T. Nicol, B. Pérot, C. Carasco, E. Brackx, A. Mariani, C. Passard, E. Mauerhofer, A. Havenith, 235 U and 239 Pu characterization in radioactive waste using neutron-induced fission delayed gamma rays, Nuclear Instruments and Methods in Physics Research A 832 (2016) PAGE 35

36 FISSION DELAYED -RAY DETECTION LIMITS MCNP calculations (MEDINA, 225 L drums) Active background (MEDINA, 225 L concrete mockup drum, measurement between pulses) Fission rate per volume unit (10 g 239 Pu) Detection limits in a 225 L concrete drum, with a n/s emission, 7200 s irradiation, 900 s post irradiation counting E (kev) Precursor T 1/2 (s) DL 239 Pu (g) DL 235 U (g) Rb- 90m Rb Y Sb- 132m Sb Rb I- 136m I Sr Sr Tc- 134 I T. Nicol, B. Pérot, C. Carasco, E. Brackx, A. Mariani, C. Passard, E. Mauerhofer, A. Havenith, 235 U and 239 Pu characterization in radioactive waste using neutron-induced fission delayed gamma rays, Nuclear Instruments and Methods in Physics Research A 832 (2016) PAGE 36

37 THE ASSOCIATED PARTICLE TECHNIQUE (APT) Alpha detector (position sensitive) Neutron TOF (alpha-gamma coincidence) T(D,n) 14 MeV neutron generator Inspected object Tagged neutrons Volume of interest Volume of interest Built-in segmented alpha detector d n Tritium target t Gamma-ray detector Gamma spectrum (selected volume) Unfolding (with a calibration database) B. Pérot, G. Sannié, Détection neutronique de matières illicites avec la technique de la particule associée, Editions Techniques de l Ingénieur, RE 177, février 2015 EFFMIN4 MARSEILLE JUILLET 2016 PAGE 37

38 ORGANIC MATERIALS IDENTIFICATION (SECURITY) Atomic fractions TNT simulant measurement Explosives Illicit drugs Benign materials A. Buffler, PAGE 38

39 RADIOACTIVE WASTE MATERIAL CHARACTERIZATION Feasibility study on non-radioactive materials (experiments) Enveloppe en béton Blocs Al Gamma spectra for different TOF windows Time-of-flight (TOF) spectrum Aluminum Concrete Random backround C. Carasco, B. Pérot, A. Mariani, W. El Kanawati, V. Valkovic, D. Sudac, J. Obhodas, Material characterization in cemented radioactive waste with the associated particle technique, Nuclear Instruments and Methods in Physics Research A 619 (2010) PAGE 39

40 PERFORMANCES FOR RADIOACTIVE WASTE PACKAGES MCNP simulations for 225 L bituminized waste drums (~ 1 TBq 137 Cs) Counts (source neutron) -1 Neutron generator background ( n/s) Counts Random background Counts (source photon) -1 Radioactive waste background 100 kev threshold Counts Random background Useful signal (not visible) Energy (MeV) Time Of Flight (ns) Energy (MeV) Time Of Flight (ns)

41 PERFORMANCES FOR RADIOACTIVE WASTE PACKAGES MCNP simulations for 225 L bituminized waste drums (~ 1 TBq 137 Cs) Counts (source neutron) -1 Neutron generator background ( n/s) Counts Counts (source photon) -1 Radioactive waste background 790 kev threshold Counts Random background Useful signal (visible) Energy (MeV) Time Of Flight (ns) Energy (MeV) Time Of Flight (ns)

42 SIMULATION OF OBJECTS IN THE 225 L BITUMINIZED DRUM Object of interest W. El Kanawati, B. Perot, C. Carasco, Monte Carlo Simulation of High-Level Radioactive Waste Characterization with the Associated Particle Technique, Nuclear Instruments and Methods in Physics Research A 705 (2013) EFFMIN4 MARSEILLE JUILLET 2016 PAGE 42

43 OBJECT IN THE CENTER OF THE BITUMINIZED DRUM (MCNP) 1 detector, 60 min 10 times more counts (10 detectors or 600 min) Object of interest W. El Kanawati, B. Perot, C. Carasco, Monte Carlo Simulation of High-Level Radioactive Waste Characterization with the Associated Particle Technique, Nuclear Instruments and Methods in Physics Research A 705 (2013) EFFMIN4 MARSEILLE JUILLET 2016 PAGE 43

44 SCINTILLATORS TO REPLACE 3 HE DETECTORS Passive neutron coincidence counting for radioactive waste drums - MCNP PoliMi simulation L waste drums - 10 cm thick plastic detectors (with lead shields) - ~ 0.5 g of 240 Pu eq s acquisition time 0.2 g/cm 3 organic matrix 0.5 g/cm 3 metallic matrix Triples (multiplicity 2 coincidences) B. Simony, C. Deyglun, B. Pérot, C. Carasco, N. Saurel, S. Colas, J. Collot, Cross-talk characterization in passive neutron coincidence counting of radioactive waste drums with plastic scintillators, IEEE Transactions on Nuclear Science, Vol. 63, No. 3, June 2016 PAGE 44

45 SIMULATED PERFORMANCES (TRIPLES) Few accidental coincidences up to 10 g of Pu Neutron vs. gamma events in the triples Plutonium localization effect Good signal to noise ratio (Pu/Total) POSTER Benoît SIMONY EFFMIN 4 benoit.simony@cea.fr EFFMIN4 MARSEILLE JUILLET 2016 PAGE 45

46 CONCLUSION Radioactive and nuclear material characterization Gamma-ray spectroscopy Passive neutron counting Neutron and photon interrogation Physical and elemental characterization Imaging techniques: gamma, X-ray Neutron activation analysis NDA for D&D and radioactive waste characterization Complementary to sampling & analytic methods Sensitivity, precision, accuracy Vs. complexity, acquisition time, cost The dream team = historic operators + NDA experts + D&D operators 26 JUILLET 2016 EFFMIN4 MARSEILLE JUILLET 2016 PAGE 46

47 EFFMIN4 MARSEILLE JUILLET 2016 THANK YOU! CEA International Expert PAGE 47 Commissariat à l énergie atomique et aux énergies alternatives Centre de Cadarache F Saint-Paul-lez-Durance FRANCE T. +33 (0) Laboratoire de Mesures Nucléaires Etablissement public à caractère industriel et commercial RCS Paris B Direction de l Energie Nucléaire Département de Technologie Nucléaire Service Mesures et Modélisation des Transferts et des Accidents Graves