Post on 18-Jun-2020
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
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
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
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
O
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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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OO
O O
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O O
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OO
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O O
O OOO
O
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OO
O
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Polymeric support
PS resins
unifies separation and measurement in a single step
immobilize selective extractants
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
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
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
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
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
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
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
PS resins for the characterization of nuclear wastes: application to 126Sn and 63Ni
Results and discussionPreparation strategy
Immobilization
63Ni
Imprinted
Covalent bound
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
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
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
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
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
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
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
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.