Analysis of a single hot particle by a combination of non-destructive analytical methods

Transcription

1 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , 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

2 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 2 Introduction JRC Non-destructive analysis of a radioactive particle Dissolution properties after digestion

3 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , 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

4 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 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.

5 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 5 Radioactive particle

6 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , 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)

7 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 7 Single radioactive particle Non-destructive characterization Dissolution behaviour in human digestive solutions

8 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , 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

9 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 9 Gamma spectrum: small Cs-137 peak + Bremsstrahlung Cs-137

10 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 10 SEM Tescan Vega TS5130 LS SEM EDX: Ca, Fe U inclusions

11 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , 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.

12 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 12 HASYLAB, Hamburg monochromator: Si (111) focusing device: polycapillary lens 10 µm step size silicon drift detector

13 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , 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.

14 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 14 Ca matrix of particle Fe on the surface Uranium inclusions

15 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , 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

16 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 16 sample absorption edge energy mean oxidation state location of measurement point UO (09) 4 U 3 O (08) 5.33 sediment point (24) 5.40 (15) central part sediment point (29) 6.01 (18) surface layer sediment point (34) 6.04 (21) surface layer sediment point (26) 5.63 (16) central part

17 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 17 SIMS Cameca 6f O 2 - primary beam Depleted Uranium Weight % U ± U ± U ± U ± U-236

18 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 18 Dissolution

19 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 19 Physiological Model for the Study of the Dissolution Characteristics of Environmental Particles Stomach Solution Compound Mmol/l Calcium Carbonate 2 Magnesium Carbonate 2.1 Potassium Chloride 9 Sodium Chloride 48 Sodium Lactate 2.2 Citric acid 0.21 Urea 5 Small Intestine Solution Compound Mmol/l Calcium Carbonate 2 Magnesium Carbonate 2.1x10-3 Potassium Chloride 9 Sodium Crloride 48 Sodium Lactate 2.2 Citric acid 0.21 Urea 13.3 Pepsin (1 g/l) Pancreatin (2 g/l) Bovine Ox Gall powder (2 g/l)

20 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 20 Leaching solutions Gamma spectrometry LSC for Sr-90 ICP-MS for Uranium and Tc-99 Radioactive Particle Stomach Compartment + fresh stomach solution Stomach (solution 1) (1 hour, 37 C) Stomach Compartment Stomach (solution 2) (1 hour, 37 C) + fresh intestine solution Intestine Compartment Intestine (solution 1) (4 hour, 37 C)

21 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 21 Cs Bq in total in stomach compartment Cs-137 [Bq] Cs-137 % Stomach ± ± 9.9 Stomach ± ± 0.6 Intestine < < 1 Residual < < 1

22 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 22 Sr Bq in total in stomach compartment LSC after separation with Sr-Spec 10 mg Sr carrier ICP-MS for recovery Sr-90 [Bq] Sr-90 % Stomach ± ± 6.6 Stomach ± ± 0.3 Intestine 72 ± ± 0.02 Residual 5.6 ± ±0.002

23 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 23 Uranium 43.6 ng in total 21 % in residual fraction composition in agreement with SIMS Uranium [ng] Uranium % Stomach ± ± 1.4 Stomach ± ± 0.4 Intestine 1.24 ± ± 0.1 Residual 9.1 ± ± 0.5 Tc-99 not detected < 1 pg Weight % U ± U ± U ± U ± 1.74

24 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , 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

25 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 25 Gerald Falkenberg Mats Eriksson, Maria Betti Marek Bielewski, Ramon Carlos and many others...

26 Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, , Monaco 26 Thank you!