ps resins for the characterization of nuclear wastes: application...
TRANSCRIPT
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PS resins for the characterization of nuclear wastes: application to 126Sn and
63Ni
Eduard Pelay, Ariadna Ferradal, Ignasi Villarroya, Héctor Bagán, Alex Tarancón, José F. García
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Introduction
High number of nuclear facilities to be decommissioned
Necessity of new methods
126Sn: fission product importance in long term storage 63Ni: activation product high importance in decommissioning
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Introduction
• LS common technique for measurement of β emitters
• Problems of selectivity
chemical separations
• γ emitters easy to determine
• β and α some challenges
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
IntroductionPSm
alternative to LS for the measurement of high and medium energy radionuclides
O
O
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OO
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O
O O
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O O
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O O
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OO
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OO
OOO O
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OO
O
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O O
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O
OO
O O
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O O
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OO
O
O O
O OOO
O
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OO
O
O
O
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O
O
O
O
O
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O
O
O
O
O
O
O
O
O
Polymeric support
PS resins
unifies separation and measurement in a single step
immobilize selective extractants
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Objective
The objective of this study is to develop new PS resin follow new preparation procedures for the analysis of nuclear wastes
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Results and discussionExtractant
TBP in n-dodecane
Dissolves PSm
C-PS
126Sn
Tropolone
Stability problems
O
OH
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Results and discussionImpregnation
TBP
Agitate 24 hFiltrate Rinse with H2O
n-dodecane
PSm
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Results and discussionProportion
0-100% TBP
Best PS resin proportion80% TBP0
20
40
60
80
100
100% 80% 60% 40% 20% 10% C- PSm
Sn re
tent
ion
(%) 0
20
40
60
80
100
20 40 60 80
Sn e
lute
d (%
)Total volume passed (mL)
100%
80%
60%
40%
20%
10%
C-PSm
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Results and discussionBatch medium determination
Optimum mediumHCl 2 M
0.00
10.00
20.00
30.00
40.00
50.00
60.00
70.00
80.00
90.00
100.00
0 1 2 3 4 5 6 7 8 9
Ret
entio
n(%
)
[HCl] (M)
Sn
Cs
Sb
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Results and discussionCalibration
Isotope Mean Energy (keV)
Detectionefficiency
(%)63Ni 17.43 15.514C 49.16 54.899Tc 94.60 81.736Cl 316.00 98.5
Isotope Mean Energy (keV)
Detectionefficiency
(%)126Sn 118.7 83.7
121mSn 120.7
y = -34.578x + 4.7249R² = 0.9986
0
1
2
3
4
5
0 0.02 0.04 0.06 0.08
ln(E
ff)
1/Emean (keV-1)
Ni-63
C-14
Tc-99
Cl-36
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Results and discussionQuantification
Replicate Count rate(cpm)
Activity(dpm/g)
Quantification Error(%)
R1 420.00 5004 1.3R2 420.09 4943 2.5R3 412.46 4851 4.3
Mean 4933 ± 77
Quantitative retention
Isotopes Estimated Activity(dpm/g)
126Sn 79121mSn 4988241Am 56
Total activity 5067
Laboratoire Nationale Henry Becquerel
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Results and discussionPreparation strategy
Immobilization
63Ni
Imprinted
Covalent bound
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Results and discussionImmobilization
DMG (2-1H-imidazol-2-il)piridina
With/without 1-octanol
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Results and discussionResins properties
Best column:DMG
Resin Detection efficiency(%)Solution Evaporated
DMG + 1-octanol 11.0±1.1 29.4±1.5DMG 14.6±1.3 17.9±0.4iPyr + 1-octanol 8.1±1.0 12.4±1.1iPyr 7.9±0.6 27.6±1.5
0
20
40
60
80
100
DMG + 1-octanol DMG iPyr + 1-octanol iPyr
Rete
ntio
n (%
)
NiFeCo
Medium:Ammonium citrate pH 8
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Results and discussionColumn analysis
Resin Total Efficiency (%)
DMG + 1-octanol 0.15 ± 0.04 DMG 0.54 ± 0.07
Total Efficiency = Detection Efficiency x Retention yield
Lost of the extractant
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Results and discussionImprinted
VbIDA
polymerization rinse
Synthesis in presence of template
Selectivity based on steric impediment
No break through volumeUse of generic extractants
N COOH
COOH
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Results and discussionRetention
Medium:Ammonium
citrate pH 7-11
ResinDetection
efficiency(%) SQP(E)
Solution Evaporated Solution EvaporatedMIP 3.1±0.4 11.8±0.9 506.1 475.4
Optical quenching
0
20
40
60
80
100
7 9 10 11
Rete
ntio
n (%
)
pH
MIP Ni
Fe
Co
Preliminary results
High selectivity
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
N
N
N
Br
Results and discussionCovalent bound
Di-(2-picoyl)amine
HN
N
N
No break through volumeMore reproducible
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Conclusions
A new PS resin for 126Sn determination has been developed
Different approaches for the preparation of a 63Ni PS resin were evaluated
MIP procedure shows a high selectivity
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PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
PS resins for the characterization of nuclear wastes: application to 126Sn and
63Ni
Eduard Pelay, Ariadna Ferradal, Ignasi Villarroya, Héctor Bagán, Alex Tarancón, José F. García
Acknowledgments
• Ministerio de Economia y Competitividad (MINECO) for financial support under CTM2014-02020
• Agència de Gestió d’Ajuts Uiversitaris i de Recerca (AGAUR) for financial support under 2014-SGR-1277.
• Dr. Philippe Cassette from LNHB (France) for supplying the 126Sn solution.