la radiochimica e la chimica delle radiazioni nel ciclo del

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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
Laboratory of Radiochemistry & Radiation Chemistry
and
Laboratory of Contaminants Migration & Safeguards
Radiochemistry & Radiation Chemistry Lab
Contaminants Migration & Safeguards Lab
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
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
Basic and Applied Research Activities
• 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 chemical
physical properties of materials
• Chemical Dosimetry for technological and medical appplications
Strategies for nuclear waste management
Fuel Cycle
Advanced strategies
for radioactive waste
management:
• partitioning
Solvent extraction
• confinement
Synthesis and
characterization of
matrices
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
Reprocessing of spent nuclear fuel: Partitioning of MAs
•
Solvent Extraction on simulated spiked solutions
AQUEOUS PHASE
ORGANIC PHASE
Lnacq
R
Anacq
OH
AQUEOUS PHASE
R
R
OH
OH
R
HO
ORGANIC PHASE
Lnacq
Lnorg
Anacq
Anorg
R
OH
R
R
OH
OH
R
HO
Reprocessing of spent nuclear fuel: Partitioning of MAs
• Examples of organic extractants
Supramolecular ligands
BTBPs
N
N
N
N
N
N
N
N
N
N
N
N
N
N
N
N
Example: PAR4
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
Laboratory of Radiochemistry & Radiation
Chemistry
Engineering of solvent extration: Centrifugal Contactors (I)
• working scheme of a centrifugal contactor
Diluent
+
Ligand-An
HNO3 aq
+
Ln
O
O
2
Diluent
+
Ligand
L L
L
L
L
γ
2
γ
O
2
γ
γ
L L
L
L L L
HNO3 aq
+
An/Ln
Engineering of solvent extration: Centrifugal Contactors (II)
• example of 16-stage centrifugal contactor battery
An example of calculated process scheme
An
Ln
+
• the process
flow-sheet can
be designed and
its performances
calculated
Ln
AQUEOUS PHASE
1
EXTRACTION BATTERY
ORGANIC PHASE
An
8
Ligand
PAR4
Am3+
recovery
Am3+/Eu3+
decontamination factor
8-STAGE
16-STAGE
99.67%
99.99%
> 95
> 130000
concentration (mol.L-1)
Profile of H+, Am(III), and Eu(III) concentration in organic
phase
1,00E-03
1,00E-04
H+
Am
Eu
1,00E-05
1,00E-06
0
2
4
6
stage number
8
10
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 –
Fluoroapatite
EURATOM
Programme
Sodalite
Radiation Chemistry: Radiation Damage studies within Partitioning
•
Irradiation Effects: reduction of extracting capabilities and selectivity
Case study: C5-BTBP dissolved in cyclohexanone
SF= DAn / DLn
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)
Radiation Damage on Polymers
• Effects induced by ionizing radiation on polymers
O
O
O
O
*
*
O
O
O
*
PET
O
PEN
• Influence of the aromatic density on the stability
• Role of Oxygen in the radiation damage
• Radicals produced and their characterization
*
Laboratory of Radiochemistry & Radiation
Chemistry
• Molecular Weight Variation
PEN films
PET films
PEN sheets
PET sheets
• Degradation Mechanism
O
O
O
PEA
O
O
O
O
O
O
O
O
O
H
CO2
O
O
O
Collaborations:
• Università di Pavia
O
HO
O
• Università di Bologna
Chemical Dosimetry for radiotherapy and industrial applications
• 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 promoted
by ionizing radiation.
Collaborations: Università di Milano, Università di Pavia
Decommissioning & Waste Management
Nuclear Waste characterization
• Radiochemical separation
• Analysis of difficult-to-measure
radionuclides (i.e. H-3, Fe-55, Ni-59,
Ni-63, Sr-90, α-emitters) in nuclear
wastes
TENORM (Technologically Enhanced
Naturally
Occurring
Radioactive
Materials) from industrial plants
• Chemical physical and radiometrical
characterization
• Methods for removal, treatment and
confinement
Contaminants Migration and Safeguards Lab
Contaminant transport in porous media
Measurements and modelling of processes that
govern contaminant transport through porous
media
Applications
nuclear waste disposal, groundwater pollution and
remediation
Investigated Processes:
Advection, dispersion, adsorption, desorption
Experiments: Batch and Column experiments
Porous media: Sands and Activated carbons
Contaminants: Salts, Metal ions and Micro organic pollutants
Predictive Models: Development of deterministic and stochastic
models of contaminant transport in porous and fractured media
Collaborations: Università di Milano, Parma, Pavia, Politecnico di Torino
Strumentazione
• colonne sperimentali
• spettrofotometro UV-Vis
Strumentazione
• sistema HPLC
• strumentazione per misure potenziometriche,
conduttimetriche e di radiazione gamma
Strumentazione
lisimetro contenente sabbie e argille
Nuclear safeguards
Simulation of correlated count measurements
for the detection of nuclear materials inside sealed tanks
by means of passive and active (neutron, photon)
interrogation
Applications: U.S.A. homeland security
Detectors
Interrogating
source
?
Detector
Fissile sample
Monte Carlo code developing: MCNP-PoliMi, customized MCNPX
Collaborations: University of Michigan, ORNL, JRC-Ispra
Strumentazione
Nuclear safeguards
sistema di misura di fotoni e neutroni veloci
Collaborations: University of Michigan, ORNL, JRC-Ispra

la radiochimica e la chimica delle radiazioni nel ciclo del

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