Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 1 Analysis of a single hot particle by a combination of non-destructive analytical methods Erich Hrnecek, Laura Aldave de las Heras, Marek Bielewski EC Joint Research Centre (JRC) ITU - Institute for Transuranium Elements Karlsruhe, Germany http://itu.jrc.ec.europa.eu http://www.jrc.ec.europa.eu
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 2 • Introduction – JRC • Non-destructive analysis of a radioactive particle • Dissolution properties after digestion
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 3 Our Structure: 7 Institutes in 5 Member States IRMM - Geel, Belgium Institute for Reference Materials and Measurements ITU - Karlsruhe, Germany Institute for Transuranium Elements IE - Petten, The Netherlands Institute for Energy IPSC - Ispra, Italy Institute for the Protection and Security of the Citizen IES - Ispra, Italy Institute for Environment and Sustainability IHCP - Ispra, Italy Institute for Health and Consumer Protection IPTS - Seville, Spain Institute for Prospective Technological Studies
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 4 1963-2008 The mission of ITU is to provide the scientific foundation for the protection of the European citizen against risks associated with the handling and storage of highly radioactive elements .
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 5 Radioactive particle
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 6 Radionuclides released to the environment can be in different physico-chemical forms. This can influence their mobility and bioavailability. B. Salbu, J.Env.Rad. 96 (2007) 47-53 .
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 7 Single radioactive particle Non-destructive characterization Dissolution behaviour in human digestive solutions
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 8 Analytical methods g -spectrometry – nuclides, activity – SEM surf. morphology, element composition m -XRF – elemental distribution m -XANES – oxidation states – SIMS surface isotopic distributions & ratios
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 9 Gamma spectrum: small Cs-137 peak + Bremsstrahlung Cs-137
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 10 SEM Tescan Vega TS5130 LS SEM EDX: Ca, Fe U – inclusions
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 11 Confocal μ -XRF 3D analysis of elemental distribution. Collects information also from inside of the sample - from depth up to few hundreds of microns Multielemental technique. Nondestructive. Access to synchrotron facility.
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 12 HASYLAB, Hamburg monochromator: Si (111) focusing device: polycapillary lens 10 µm step size silicon drift detector
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 13 Confocal geometry of measurements Synchrotron radiation... ...is focused... ...and passes through the sample. On its way the atoms are excited. Excited atoms emits fluorescence radiation... ...in all directions, but... ...only the photons emitted into the polycapillary solid angle can reach the detector. Properly aligned optics transmits the radiation only from a short section of excited volume.
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 14 Ca matrix of particle Fe on the surface Uranium inclusions
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 15 Confocal μ -XANES X-ray absorption near edge structure Confocal geometry Fluorescence mode U L III absorption edge 4 Uranium inclusions measured U oxidation states
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 16 sample absorption edge energy mean oxidation state location of measurement point UO 2 17168.65 (09) 4 U 3 O 8 17170.77 (08) 5.33 sediment point 1 17170.87 (24) 5.40 (15) central part sediment point 2 17171.85 (29) 6.01 (18) surface layer sediment point 3 17171.90 (34) 6.04 (21) surface layer sediment point 4 17171.24 (26) 5.63 (16) central part
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 17 SIMS Weight % Cameca 6f 0.0046 ± 0.0005 U-234 0.312 ± 0.002 U-235 - primary beam O 2 0.057 ± 0.001 U-236 Depleted Uranium 99.627 ± 0.002 U-238 U-236
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 18 Dissolution
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 19 Physiological Model for the Study of the Dissolution Characteristics of Environmental Particles Stomach Solution Small Intestine Solution Compound Mmol/l Compound Mmol/l Calcium Carbonate 2 Calcium Carbonate 2 Magnesium Carbonate 2.1 Magnesium Carbonate 2.1x10 -3 Potassium Chloride 9 Potassium Chloride 9 Sodium Chloride 48 Sodium Crloride 48 Sodium Lactate 2.2 Sodium Lactate 2.2 0.21 Citric acid 0.21 Citric acid Urea 5 Urea 13.3 Pepsin (1 g/l) Pancreatin (2 g/l) Bovine Ox Gall powder (2 g/l)
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 20 Leaching solutions Radioactive Particle Gamma spectrometry LSC for Sr-90 Stomach Compartment ICP-MS for Uranium and Tc-99 + fresh stomach solution Stomach ( solution 1 ) Stomach ( solution 2 ) Stomach Compartment (1 hour, 37°C) (1 hour, 37°C) + fresh intestine solution Intestine Compartment Intestine ( solution 1 ) (4 hour, 37°C)
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 21 Cs-137 [Bq] Cs-137 % Cs-137 0.364 ± 0.038 95.2 ± 9.9 Stomach 1 0.383 Bq in total 0.019 ± 0.002 4.8 ± 0.6 Stomach 2 Intestine < 0.004 < 1 in stomach compartment Residual < 0.004 < 1
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 22 Sr-90 Sr-90 [Bq] Sr-90 % 23300 ± 1200 95.4 ± 6.6 Stomach 1 24400 Bq in total 1036 ± 52 4.2 ± 0.3 Stomach 2 in stomach compartment 72 ± 4 0.29 ± 0.02 Intestine LSC after separation 5.6 ± 0.4 0.023 ± 0.002 Residual with Sr-Spec 10 mg Sr carrier ICP-MS for recovery
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 23 Uranium Uranium [ng] Uranium % 26.3 ± 0.5 60.0 ± 1.4 Stomach 1 43.6 ng in total 7.1 ± 0.1 16.3 ± 0.4 Stomach 2 21 % in residual fraction 1.24 ± 0.04 2.8 ± 0.1 Intestine composition in agreement with SIMS 9.1 ± 0.2 20.9 ± 0.5 Residual Tc-99 not detected < 1 pg Weight % 0.0046 ± 0.0002 U-234 0.419 ± 0.008 U-235 0.041 ± 0.001 U-236 99.54 ± 1.74 U-238
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 24 Summary Non destructive analysis of particle Ca, Fe major components U inclusions, more oxidised on surface Depleted Uranium Sr-90 major activity, soluble
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 25 Gerald Falkenberg Mats Eriksson, Maria Betti Marek Bielewski, Ramon Carlos and many others...
Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 26 Thank you!
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