Upload
others
View
5
Download
0
Embed Size (px)
Citation preview
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.
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.
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 LIII 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
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
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
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
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
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
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
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
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
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!