O 2

Report
SSC Research Institute of Atomic Reactors. RUSSIA
Status of
SNF Pyro Reprocessing
RIAR, Dimitrovgrad, Russia
Mikhail Kormilitsyn
Research Institute of Atomic Reactors (RIAR)
Radiochemical Complex
RIAR General Goal
PIE
Research Reactors
Fuel Supply of
BOR-60/MBIR
Closing of FC
MA
recycling
Advanced Fuel
development
and testing
RAW
Treatment
Demo of Closed
Fuel Cycle
Radionuclide
Productions
Fundamental
Studies
R&D for MSR
Fuel Cycle
2
New Generation Technological Package
“Pyro-Chemistry for CFC”
Universal technological platform for
decisions in the field of Closed Fuel Cycle of
Nuclear Power:
• No limitation for:
 fuel types (oxides, nitrides, metal, carbides, cermet, MSR, IMF)
 burn up,
 cooling time
• No limitation for requirements of
decontamination factor (DF up to 106)
3
New Generation Technological Package
“Pyro-Chemistry for CFC”
• The Base System – Molten chlorides
 The Base processes




Dissolution of initial SNF ( chlorination or anodic dissolution)
Electrolysis on solid and/or liquid cathodes
Precipitation
Purification of the melt
• Option – Technology of fluoride volatility
• Option – Partitioning in fluoride melt
• Option – chemistry and technology of molten
fluoride fuel of MSR
4
R&D on SNF Pyro Reprocessing in a World
• Oxide SNF reprocessing into Oxide – RIAR (Russia), JNC/JAEA (Japan)
• Oxide SNF reprocessing into Metallic – CRIEPI (Japan), KAERI (Korea)
• Nitride SNF reprocessing – JAERI/JAEA (Japan), RIAR (Russia)
• Metallic SNF reprocessing – INL, ANL (US), CRIEPI (Japan), RIAR
(Russia)
• SNF metallization – KAERI (Korea), RIAR (Russia)
• HLW partitioning in molten salts – CRIEPI (Japan), RIAR (Russia),
KAERI (Korea), CEA (France), ITU (EU)
• Fluoride volatility processes – CRIEPI, Hitachi/TEPCO (Japan),
Kurchatov Inst., RIAR (Russia), INR (Czech. Rep.)
• MSR Fuel Cycle – RIAR, Kurchatov Inst., CNRS (France), Institute for
Applied Physics, Shanghai (China)
• Other application
5
RIAR Experience
6
RIAR activities in the field of CFC
Since 1964 RIAR has been pursuing large-scale
investigations in the following research lines:
 Pyrochemical production technology of vi-pack U and MOX fuel
 Pyrochemical reprocessing of SNF from nuclear reactors of various types .
 Fluoride volatility reprocessing of SNF
7
Milestones of Experience in Closed Fuel Cycle
• Pyro R&D- from early 1960-s
• Demo of fluoride volatility reprocessing – 1970s
• Pilot facility for pyro/vi-pack MOX fuel production for fast
reactor – from late 1970-s
• BOR-60 full scale fuel supplying only on the base of
own RIAR pyro/vi-pack fuel production facilities –
from 1980
• Pyro reprocessing experience – from 1991
• Study on transmutation cycle, nitride fuels and others – from
1992
• Start of industrial implementation of pyro/vi-pack MOX
technology – 2012
• Start of so called “high density” FR SNF (nitride, metal) - 2010
• Creation of “Poly-functional Radiochemical Complex” (PRC) 2010-2017
8
RIAR experience in reprocessing
of spent fuel of the BOR-60 and BN-350 reactors
Fuel type
Burn-up
% h.a.
Cooling time,
Yrs
UO2
7,7
5
2,5
1972..1973
BN-350
MOX
4,7
10
4,1
1991
BN-350
MOX
21..24
1-2
6,5
1995
BOR-60
UO2
10
15
5
2000
BOR-60
MOX
10
10
12
2000…2001
BOR-60
MOX
16
4-6
5
2004
BOR-60
U-Pu /Na
6,4
19
0,13
2010
BOR-60
(U,Pu)N /Pb
0,53
8
0,28
2010
BOR-60
U-Zr / Na
9,7
9,5
0,12
2010
BOR-60
U-Pu-Zr /Na
9,7
9,5
0,10
2010
BOR-60
MOX
15
5
4
2011
BOR-60
Weight, kg
Date
Reactor
9
Dimitrovgrad Dry Process (DDP) –
MOX Fuel Pyro processing
Basic research of the molten salt systems allowed for the
development of technological processes for production of
granulated U and Pu dioxides and MOX.
A distinctive feature of the Pyro technology is a possibility to
perform all the deposit production operations in one apparatus - a
chlorinator-electrolyzer
Pyrochemical reprocessing consists of the following main
stages
•
Dissolution of initial products or spent
nuclear fuel in molten salts
•
Recovery of crystaline Pu dioxide
electrolytic MOX from the melt
•
Processing of the cathode deposit and
production of vi-pack
or
10
Production and testing
of vi-pack MOX fuel
Fuel type
Number of
FAs
Burn-up,
max.%
Load,
kW/m
Temperature,
0С
Reactor
(U, Pu)O2
Civil grade/ or
weapon quality
330
30,3
51,5
720
BOR-60
UO2 +
PuO2
Civil grade/ or
weapon quality
132
14,8
45
705
BOR-60
(U, Pu)O2
Weapon grade
26
11,1
46
680
BN-600
(U, Pu)O2
Civil grade
4
development of the production technique
BN-600
11
Cl2
Stirrer
Na3PO4
Cathode
(pyrographite)
Ar (Cl2)
Cl2+O2+Ar
Cathode
Cl2+O2+Ar
Stirrer
Stirrer
pyrographite bath,
NaCl - KCl
+
UO22+
O2
UO2 +
NpO2
Pu4+
UO2
+
UO22+
MA,RE
E
UO2
Pu4+
UO22+ NpO2+
PuO2
Fuel chlorination
700 оС
PuO22+
PuO2
Preliminary
electrolysis
680 оС
(MA,REE)
RW4
UO22+
Precipitation
crystallization
680 оС
Cl-
Electrolysisadditional 700 оС
Melt purification
700 оС
DDP MOXPuO2 flow sheet
Stirrer
Cl2
Cathode
(pyrographite)
Cl2+O2+Ar
Ar (Cl2)
Na3PO4
Cathode
Cl2+O2+Ar
Stirrer
pyrographite bath,
NaCl -2CsCl
+
+
UO22+
UO2
Pu4+
PuO2
Fuel chlorination
650 оС
UO2 +
NpO2
UO22+ NpO2+
Preliminary
electrolysis
630 оС
MOX
UO22+ PuO2+
Main MOX
electrolysis
630 оС
+
MOX
UO22+
PuO2+
Electrolysisadditional 630 оС
DDP MOXMOX flow sheet
MA,RE
E
Cl-
(MA,REE)
RW4
Melt purification
6500 оС
12
MOX-MOX Reprocessing
2004 Year
MOX - 3 400 g
Pu content - 33,5 % wt.
2000 Year
MOX - 3 200 g
Pu content - 10 % wt.
13
Pyro HLW treatment
Na3PO4
Pyroreprocessing
Salt
purification
Radioactive Cs
Fission products
Phosphates
Waste
NdPO4C
ePO4
Salt residue
NaCl
CsCl
Phosphates
Salt residue
Special features
contain fission products
Alkaline metal chlorides,
high activity, significant
heat release
Basic elements
11 wt.% Nd
4,4 wt.% Ce
81,96 wt.% CsCl
18,04 wt.% NaCl
Quantity*
<0,15 kg/kg of fast
reactor SNF
* - TOSHIBA estimation for DDP
<0,03 kg/kg of fast
reactor SNF
14
Vitrification of HLW from pyro process
HLW type
Characteristic
Glass matrix type
Introduction method
Introduced waste amount, %
137Cs
leaching rate as of the 7th day,
g/cm2 * day
Thermal resistance, 0С
Radiation resistance
Phosphate
precipitate
Spent salt
electrolyte
Phosphate precipitate +
spent salt electrolyte
Pb(PO3)2
NaPO3
NaPO3, AlF3
Al2O3
NaPO3, AlF3
Al2O3
vitrification,
Т=9500С
vitrification without
chloride conversion,
Т=9500С
vitrification without chloride
conversion, Т=9500С
28
20
36
7*10-6
7*10-6
4*10-6
400
400
400
107 Gr (for  and )
1018 -decay/g
15
Ceramization of HLW arising from pyro process
Type of high-level wastes
Characteristics
Phosphate deposit
Spent salt electrolyte
monazite
Cosnarite (NZP)
pressing, calcination ,
Т=8500С
Conversion to NZP from the melt
or aqueous solution, pressing,
calcination , Т=10000С
Quantity of waste introduced into
ceramics, %
100
30..40
Leaching rate of 137Cs on 7-th day,
g/cm2 * day
1*10-6
3*10-6
850
1000
Type of ceramics
Method of introduction into ceramics
Thermal stability, 0С
Radiation resistance
5*108 Gy( for  and )
1019 - decay/g
16
RIAR R&D PROGRAM DOVITA
Since 1992
• Dry technologies
• Oxide fuel with MA
• Vi-pack
• Integrated disposition on the same
site with the reactor
• TA Transmutation of Actinides
17
18
Experience in DOVITA Program
 Pyrochemical technology of adding Np into oxide fuel (520%) has been developed
 Performance of vi-pack fuel with (U,Np)O2 fuel has been
validated experimentally to ~20% burnup in BOR-60
 No evidence of significant difference in performance of fuel
rods with (U,Np)O2 fuel compared with UO2 or MOX fuel rods
has been noticed
 Pyrochemical process of codeposition of Am with MOX fuel
(2-4%) has been developed
 Methods of Am/REE separation in melts has been tested
Irradiated
(U,Np)O2 fuel,
19% burn-up
 Special vi-pack targets containing Am oxide with UO2 or
inert matrix have been developed
 Transmutation of Np, Am, Cm is being studied in BOR-60
19
New times consideration:
DOVITA
1992
 Dry technologies
 Oxide fuel with MA
 Vi-pack
 Integrated disposition
same site with the
reactor
 TA Transmutation of
Actinides
DOVITA-2
2007+
Dry technologies
On-site reprocessing
Various type of fuel with
MA
Integration of MA
recycling into FR Closed
Fuel Cycle
TA - Transmutation of
Actinides
20
DOVITA-2
Fuel type/ Oxide
Stages
vi-pack
Concept Studies
+
Oxide
pellet
+
Nitride
vi-pack
+
Metal
+/-
Molten
salt
+
R&D
+
-/+
+/-
-
+
Fuel Production
+
-
-
-
-
Irradiation
Testing
PIE
+
-
-
-
-
+
-
-
-
----
Reprocessing
-/+
-
-
-
+/-
DOVITA-1
21
Current R&D
22
In the Frame of Federal Target Program
For the First Time in a World –
pyrochemical reprocessing
of FBR spent U-Pu
nitride fuel and metal fuel
~ 0,6 kg SF
2 Cd ingots
for
fabrication
of fuel
Oxide
concentrate FP
for wastes
preparation
23
Experimental Tests of
Spent Nitride Fuel Reprocessing Methods
The empty pies
of cladding after
anodic
dissolution of
nitride SNF in
chloride melt
The sample of
fluoride-phosphate
glass with real
immobilized FPs
after reprocessing
24
100% PuO2 Pyro Pellets
PuO2 Pellets Characteristics
Melted salt
3LiCl-2KCl
NaCl-2CsCl
Pellets density, g/sm3
8.5-10.2
9.8-10.3
Visual view
no cracks
no cracs
PuO2 Pellets
(3LiCl-2KCl, T=450oC)
PuO2 Pellets
(NaCl-2CsCl, T=550oC)
25
80%UO2 + 20%PuO2 MOX Pyro Pellets
MOX Pellets Characteristics
Batch № 1
Technical
Requirements*
Pellet density, g/sm2
10.2-10.4
10.2-10.7
Deviation of pellet density,
g/sm2
+0.1
+0.1
O/Me
1.98
1.97+0.01
Impurities content, %
масс.
<0.3
<0.4
Average size of crystalline
granules, microns
30-40
<
50
Visual view
no cracks
no cracks
Porosity
uniform
uniform
*Reshetnikov Ph.G. and et al. Working out,
production and operation of fuel rods
of power reactors-M:.Energoizdat, 1995-320p.
26
Pyro MOX pellets (80%UO2 + 20%PuO2)
Microstructure of MOX pellets
Content, wt%
Массовая доля U, Pu,%
EPMA
90
80
70
60
50
40
30
20
10
0
3000
3500
4000
U
4500
Pu
5000
5500
6000
Расстояние, мкм
μm
Unpickled pellet
Pickled pellet
Solubility test in 8M HNO3 at 95-96оC , duration – 10 hrs.
Composition of pellet
80wt%UO2
+20wt%PuO2
Medium of powder
production
Insoluble
residue,
% wt.
Residue composition, wt%
3LiCl-2KCl
0.14
(Pu0.81, U0.19)O2
3LiCl-2KCl
0.14
(Pu0.49, U0.51)O2
NaCl-2CsCl
0.40
(U0.65, Pu0.31,Am0.04)O2
27
Fuel pin #TM0-01 with pyro MOX pellets
Dismountable BOR-60 FAs
28
Fundamental Studies
Curium containing salt for spectroscopy studies
NaCl-2CsCl-CmCl3(0.115mol/kg)
29
transmission density
Spectrum of curium-containing melt
under atmosphere of Ar- HCl-H2O
CmO+
0.55
Cm3+
0.25
Am3+
-0.05
320
370
420
470
520
wave-length, nm
NaCl-2CsCl-CmCl3(0.115mol/kg)
750oC
log(P2HCl/PH2O)=-7.14
30
Synchronized potentiometric titration by oxygen pump and spectroscopy
Oxygen pump
CE
RE
Gas-supply tube
Oxygen sensor
Cavity from optical
quartz
31
MA and FP Partitioning
T,oC
Run
#
Weight, g
Content in melt, %
(Li,K,Cs)Cl
Ga
Am
Ce
E, V
1
350
200
95
0.6
3
-1.2
2
350
200
95
0.6
3
-1.4
3
350
200
95
0.6
3
-1.6
Ga cathod
0
-0.2
-0.4
I, A
-0.6
-0.8
-1
-1.2
-1.4
-1.6
0
200
400
600
800
1000
1200
1400
Time, sec
32
Experimental Facilities till 2020
34
CFC Pyro technology
for International RIAR-based Center of Excellence
RIAR Site
Post Irradiation Examination
electricity
Heat power
radionuclides
R&D on
Reprocessing
MBIR
MOX or other
fuel
and
Refabrication
of Advanced
Fuels
Post Irradiation complex
RadioWaste
complex
Вибро
Vi-pack
Отходы на хранение
RAW
Radiochemical
Complex
Refabricated
Fuel
RIAR Radiochemical Complex
Пиро
Pyro
MOX
ChemicalProduction
Technological
Facility
complex
35
Federal Tasks-oriented Program
“New Generation Nuclear Power Technologies”
• Large Poly-functional Radiochemical Complex (PRC) - 2017
 Molten salt Reprocessing Facility (1st hot cell line)
 capacity – up to 1-2 tons of FR SNF per Year (fuel type: oxide, nitride,
metallic, IMF)
 Advanced water-technology Facility, (2nd hot cell line)
 capacity – up to 1-2 tons kg of SNF per Year
• New Lab for Experimental and Innovative Fuel Production –
2010-1017 (incl. Fuel and Targets with MA)
• New facility for HLW treatment
• Demonstration of Closing Fuel Cycle
• Testing and Demonstration of Closing FR Fuel Cycle for MA
• Develop the full scale Design of Industrial plants for FR SNF
Reprocessing
36
List of Advanced R&D for PRC
•
•
•
•
•
•
Testing of prototypes of technological equipment
Development and testing of automatic and robotics systems
Comparative FS for different technologies
Advanced thermo-chemical decladding technologies
Voloxidation
Pyrochemical molten salt technologies




•
MOX fuel
Mixed Nitrides
Metallic
IMF, MSR
Remote control fabrication technologies
 Vi-pack
 Pelletizing
 Metallic
•
RAW treatment
•
•
Vitrification
Ceramization
37
37
38
THANK YOU FOR
ATTENTION!
RIAR Radiochemical Complex
38

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