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DIPARTIMENTO DI ENERGIA - CeSNEF
Dipartimento di ENERGIA
Centro Studi Nucleari Enrico Fermi
Radiochimica e Chimica delle Radiazioni nel Ciclo del Combustibile Nucleare
Mario Mariani
Francesca Giacobbo
Enrico Padovani
DIPARTIMENTO DI ENERGIA - CeSNEF
Laboratory of Radiochemistry & Radiation Chemistry
and
Laboratory of Contaminants Migration & Safeguards
DIPARTIMENTO DI ENERGIA - CeSNEF
Lab Equipments
• UV-VIS, IR spectrophotometers• potentiometric and electrochemical equipments• HPLC• ICP-MS• experimental columns for transport experiments• lisimeter filled with sand and clay
• hot cells and gloves boxes
• HPGe X-γ ray detectors• NaI(Tl) detectors• alfa spectrometers• positron annihilation lifetime spectrometers• centrifugal contactor battery• fast neutron and gamma ray detectors
Radiochemistry & Radiation Chemistry LabContaminants Migration & Safeguards Lab
DIPARTIMENTO DI ENERGIA - CeSNEF
Radiochemistry & Radiation Chemistry and Contaminant Transport & Safeguards Labs
Permanent staff:• Mario Mariani (Researcher)
• Francesca Giacobbo (Researcher)
• Enrico Padovani (Researcher)
• Mirko Da Ros (technician)
• Marco Giola (technician)
2 Post Doctoral Researchers
3 PhD students
4 Undergraduate students
DIPARTIMENTO DI ENERGIA - CeSNEF
• Partitioning of Fission Products, Lanthanides and Minor Actinides(i.e. Am, Cm…) from irradiated spent nuclear fuel
• Confinement of Nuclear Waste into inert solid matrices (i.e. zeolites, apatites, glasses…)
• Decommissioning & Waste Management of industrial and nuclear plants
• Radiation Damage of materials and ageing
• Radiation Processing for the improvement of the chemicalphysical properties of materials
• Chemical Dosimetry for technological and medical appplications
Radiochemistry & Radiation Chemistry Lab
Basic and Applied Research Activities
DIPARTIMENTO DI ENERGIA - CeSNEF
Radiochemistry & Radiation Chemistry Lab
Strategies for nuclear waste management
DIPARTIMENTO DI ENERGIA - CeSNEF
Fuel Cycle
• partitioning
Solvent extraction
• confinement
Synthesis and characterization of matrices
Advanced strategiesfor radioactive wastemanagement:
Radiochemistry & Radiation Chemistry LabRadiochemistry & Radiation Chemistry
DIPARTIMENTO DI ENERGIA - CeSNEF
Reprocessing of spent nuclear fuel
• Partitioning of minor actinides (Am, Cm) from lanthanides by means of solvent extraction
EC Projects:
• Newpart (FP4)
• Partnew (FP5)
• Europart (FP6)
• ACSEPT (FP7)
Funding:
• European Commission –EURATOM Programme
Radiochemistry & Radiation Chemistry Lab
DIPARTIMENTO DI ENERGIA - CeSNEF
AQUEOUS PHASE ORGANIC PHASE
OHOH HO
RR R R
OH
Lnacq
Anacq
AQUEOUS PHASE ORGANIC PHASE
OHOH HO
RR R R
OH
Lnacq
Anacq
Lnorg
Anorg
• Solvent Extraction on simulated spiked solutions
Reprocessing of spent nuclear fuel: Partitioning of MAs
Radiochemistry & Radiation Chemistry Lab
DIPARTIMENTO DI ENERGIA - CeSNEF
Reprocessing of spent nuclear fuel: Partitioning of MAs
• Examples of organic extractants
Radiochemistry & Radiation Chemistry Lab
Supramolecular ligands BTBPs
N N
N
N
NN
N
N
N N
N
N
NN
N
N
Collaborations within the extractants synthesis:
• Università di Parma
• University of Reading (UK)
Collaborations within the extraction tests:• Università di Parma• University of Reading (UK) • CSIC - Barcellona
Example: PAR4
DIPARTIMENTO DI ENERGIA - CeSNEF
Diluent+
Ligand-An
HNO3 aq
+
Ln
HNO3 aq+
An/Ln
Diluent+
Ligand
γγγγ
γγγγγγγγ
γγγγ
O
2
O
2
O
2
LLLL
LLLLLLLL LLLLLLLL
LLLL
LLLL
LLLL
LLLLLLLLLLLL
Engineering of solvent extration: Centrifugal Contactors (I)
• working scheme of a centrifugal contactor
Laboratory of Radiochemistry & Radiation Chemistry
DIPARTIMENTO DI ENERGIA - CeSNEF
Engineering of solvent extration: Centrifugal Contactors (II)
• example of 16-stage centrifugal contactor battery
Radiochemistry & Radiation Chemistry Lab
DIPARTIMENTO DI ENERGIA - CeSNEF
1 EXTRACTION BATTERY 8
Ln
An
Ln+An
ORGANIC PHASE
AQUEOUS PHASE
Profile of H+, Am(III), and Eu(III) concentration in organic phase
1,00E-06
1,00E-05
1,00E-04
1,00E-03
0 2 4 6 8 10
stage number
con
cen
trat
ion
(m
ol.L
-1)
H+
Am
Eu
> 130000> 95Am3+/Eu3+
decontamina-tion factor
99.99%99.67%Am3+
recovery
16-STAGE8-STAGE
An example of calculated process scheme
LigandPAR4
• the processflow-sheet can be designed and its performancescalculated
Radiochemistry & Radiation Chemistry Lab
DIPARTIMENTO DI ENERGIA - CeSNEF
Confinement
• Confinement of chloride/fluoride waste coming from pyrometallurgical partitioning processes in inorganic matrices
Projects:
• ACSEPT (FP7)
Collaborations:
• ENEA - Casaccia;
• CEA - Marcoule
Funding:
• European Commission –EURATOM Programme
Radiochemistry & Radiation Chemistry Lab
Fluoroapatite
Sodalite
DIPARTIMENTO DI ENERGIA - CeSNEF
Radiation Chemistry: Radiation Damage studies within Partitioning
Radiochemistry & Radiation Chemistry Lab
• Irradiation Effects: reduction of extracting capabilities and selectivity
T. Retegan, C. Ekberg, S. et all “The behaviour of organic solvents containing C5-BTBPand CyMe4-BTBP at low irradiation doses”Radiochim. Acta 95, 637–642 (2007)
Case study: C5-BTBP dissolved in cyclohexanone
SF= DAn / DLn
DIPARTIMENTO DI ENERGIA - CeSNEF
• Influence of the aromatic density on the stability
• Role of Oxygen in the radiation damage
• Radicals produced and their characterization
Radiochemistry & Radiation Chemistry Lab
Radiation Damage on Polymers
• Effects induced by ionizing radiation on polymers
O
O
*
O *
O
O
O
O
O
*
*
PENPET
DIPARTIMENTO DI ENERGIA - CeSNEF
PEN films
PET films
PEN sheets
PET sheets
Laboratory of Radiochemistry & Radiation Chemistry
Radiation Damage on Polymers
• Molecular Weight Variation
DIPARTIMENTO DI ENERGIA - CeSNEF
O
O
O
O
O
O
O
O
O
O
O
O
O
HO
O
O
O
O
CO2
H
Radiation Damage on Polymers
• Degradation Mechanism
Collaborations:
• Università di Pavia
• Università di Bologna
PEA
Radiochemistry & Radiation Chemistry Lab
DIPARTIMENTO DI ENERGIA - CeSNEF
Chemical Dosimetry for radiotherapy and industrial applications
Collaborations: Università di Milano, Università di Pavia
• Inorganic chemical dosimeters: study of dosimetric systems in gel state (Frixy-Gel) for high and low radiation doses.
• Polimeric dosimeters: development of a dosimeter based on polymerization promotedby ionizing radiation.
Radiochemistry & Radiation Chemistry Lab
DIPARTIMENTO DI ENERGIA - CeSNEF
• Radiochemical separation
• Analysis of difficult-to-measureradionuclides (i.e. H-3, Fe-55, Ni-59, Ni-63, Sr-90, α-emitters) in nuclearwastes
• Chemical physical and radiometricalcharacterization
• Methods for removal, treatment and confinement
Decommissioning & Waste Management
TENORM (Technologically EnhancedNaturally Occurring RadioactiveMaterials) from industrial plants
Nuclear Waste characterization
Radiochemistry & Radiation Chemistry Lab
DIPARTIMENTO DI ENERGIA - CeSNEF
Contaminant transport in porous media
Measurements and modelling of processes that govern contaminant transport through porous media
Applicationsnuclear waste disposal, groundwater pollution and
remediation
Investigated Processes: Advection, dispersion, adsorption, desorptionExperiments: Batch and Column experimentsPorous media: Sands and Activated carbonsContaminants: Salts, Metal ions and Micro organic pollutants
Predictive Models: Development of deterministic and stochastic models of contaminant transport in porous and fractured media
Contaminants Migration and Safeguards Lab
Collaborations: Università di Milano, Parma, Pavia, Politecnico di Torino
DIPARTIMENTO DI ENERGIA - CeSNEF
Contaminant transport in porous media
Contaminants Migration and Safeguards Lab
Collaborations: Università di Milano, Parma, Pavia, Politecnico di Torino
StrumentazioneStrumentazione
• colonne sperimentali
• spettrofotometro UV-Vis
DIPARTIMENTO DI ENERGIA - CeSNEF
Contaminant transport in porous media
Contaminants Migration and Safeguards Lab
Collaborations: Università di Milano, Parma, Pavia, Politecnico di Torino
• sistema HPLC
• strumentazione per misure potenziometriche,conduttimetriche e di radiazione gamma
StrumentazioneStrumentazione
DIPARTIMENTO DI ENERGIA - CeSNEF
Contaminant transport in porous media
Contaminants Migration and Safeguards Lab
Collaborations: Università di Milano, Parma, Pavia, Politecnico di Torino
lisimetro contenente sabbie e argille
StrumentazioneStrumentazione
DIPARTIMENTO DI ENERGIA - CeSNEF
Nuclear safeguards
?
Fissile sample
Detectors
Interrogating source
Detector
Simulation of correlated count measurements for the detection of nuclear materials inside sealed tanks
by means of passive and active (neutron, photon) interrogation
Monte Carlo code developing: MCNP-PoliMi, customized MCNPX
Applications: U.S.A. homeland security
Collaborations: University of Michigan, ORNL, JRC-Ispra
Contaminants Migration and Safeguards Lab
DIPARTIMENTO DI ENERGIA - CeSNEF
Nuclear safeguards
Collaborations: University of Michigan, ORNL, JRC-Ispra
Contaminants Migration and Safeguards Lab
sistema di misura di fotoni e neutroni veloci
StrumentazioneStrumentazione