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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, 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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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
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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
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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.
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Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 5
Radioactive particle
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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.
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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
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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
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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
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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
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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.
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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
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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.
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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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
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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 LIII absorption edge
4 Uranium inclusions measured
U oxidation states
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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
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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Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 17
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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Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 18
Dissolution
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Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 19
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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Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 20
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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Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 21
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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Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 22
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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Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 23
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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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
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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...
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Int. Symp. on Isotopes in Hydrology, Marine Ecosystems, and Climate Change Studies, 27 03 - 01 04 2011, Monaco 26
Thank you!