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Analysis of a single hot particle by a combination of non-destructive - - PowerPoint PPT Presentation

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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,

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Analysis of a single hot particle by a combination

  • f 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

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  • Introduction – JRC
  • Non-destructive analysis of a

radioactive particle

  • Dissolution properties after digestion
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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

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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

  • f highly radioactive elements.
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Radioactive particle

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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.
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Single radioactive particle Non-destructive characterization Dissolution behaviour in human digestive solutions

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Analytical methods

g-spectrometry – nuclides, activity SEM –

  • surf. morphology, element composition

m-XRF – elemental distribution m-XANES –

  • xidation states

SIMS – surface isotopic distributions & ratios

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Gamma spectrum: small Cs-137 peak + Bremsstrahlung

Cs-137

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SEM Tescan Vega TS5130 LS SEM EDX: Ca, Fe U – inclusions

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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.

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HASYLAB, Hamburg monochromator: Si (111) focusing device: polycapillary lens 10 µm step size silicon drift detector

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Confocal geometry of measurements

Synchrotron radiation... ...is focused... ...and passes through the sample. Excited atoms emits fluorescence radiation... Properly aligned optics transmits the radiation only from a short section of excited volume. ...in all directions, but... ...only the photons emitted into the polycapillary solid angle can reach the detector. On its way the atoms are excited.

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Ca matrix of particle Fe on the surface Uranium inclusions

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Confocal μ-XANES

X-ray absorption near edge structure Confocal geometry Fluorescence mode U LIII absorption edge 4 Uranium inclusions measured U oxidation states

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sample absorption edge energy mean oxidation state location of measurement point UO2 17168.65 (09) 4 U3O8 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

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SIMS Cameca 6f O2

  • primary beam

Depleted Uranium U-236

Weight % U-234 0.0046 ± 0.0005 U-235 0.312 ± 0.002 U-236 0.057 ± 0.001 U-238 99.627 ± 0.002

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Dissolution

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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 Pepsin (1 g/l) 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 Pancreatin (2 g/l) Bovine Ox Gall powder (2 g/l)

Stomach Solution Small Intestine Solution Physiological Model for the Study of the Dissolution Characteristics of Environmental Particles

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Stomach (solution 1) Stomach Compartment Radioactive Particle Stomach (solution 2) Stomach Compartment Intestine Compartment Intestine (solution 1)

(1 hour, 37°C) (1 hour, 37°C) + fresh stomach solution + fresh intestine solution (4 hour, 37°C)

Leaching solutions Gamma spectrometry LSC for Sr-90 ICP-MS for Uranium and Tc-99

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Cs-137 [Bq] Cs-137 % Stomach 1 0.364 ± 0.038 95.2 ± 9.9 Stomach 2 0.019 ± 0.002 4.8 ± 0.6 Intestine < 0.004 < 1 Residual < 0.004 < 1

Cs-137 0.383 Bq in total in stomach compartment

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Sr-90 [Bq] Sr-90 % Stomach 1 23300 ± 1200 95.4 ± 6.6 Stomach 2 1036 ± 52 4.2 ± 0.3 Intestine 72 ± 4 0.29 ± 0.02 Residual 5.6 ± 0.4 0.023 ±0.002

Sr-90 24400 Bq in total in stomach compartment LSC after separation with Sr-Spec 10 mg Sr carrier ICP-MS for recovery

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Uranium [ng] Uranium % Stomach 1 26.3 ± 0.5 60.0 ± 1.4 Stomach 2 7.1 ± 0.1 16.3 ± 0.4 Intestine 1.24 ± 0.04 2.8 ± 0.1 Residual 9.1 ± 0.2 20.9 ± 0.5 Weight % U-234 0.0046 ± 0.0002 U-235 0.419 ± 0.008 U-236 0.041 ± 0.001 U-238 99.54 ± 1.74

Uranium 43.6 ng in total 21 % in residual fraction composition in agreement with SIMS Tc-99 not detected < 1 pg

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Summary Non destructive analysis of particle Ca, Fe major components U inclusions, more oxidised on surface Depleted Uranium Sr-90 major activity, soluble

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Gerald Falkenberg Mats Eriksson, Maria Betti Marek Bielewski, Ramon Carlos and many others...

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Thank you!