Status of SNF Pyro Reprocessing RIAR, Dimitrovgrad, Russia Mikhail Kormilitsyn Research Institute of...
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Transcript of Status of SNF Pyro Reprocessing RIAR, Dimitrovgrad, Russia Mikhail Kormilitsyn Research Institute of...
Status of SNF Pyro Reprocessing
RIAR, Dimitrovgrad, Russia
Mikhail Kormilitsyn
Research Institute of Atomic Reactors (RIAR)
Radiochemical Complex
SSC Research Institute of Atomic Reactors. RUSSIA
RIAR General Goal
Research Reactors PIE Radionuclide Productions
Fuel Supply of BOR-60/MBIR
Closing of FC
Advanced Fuel development
and testing
Demo of Closed Fuel Cycle
MA recycling
R&D for MSR Fuel Cycle
Fundamental Studies
RAW Treatment
2
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”
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 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 typeBurn-up
% h.a.Cooling time,
Yrs Weight, kg Date Reactor
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
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 or electrolytic MOX from the melt
• Processing of the cathode deposit and production of vi-pack
10
Production and testingof vi-pack MOX fuel
Fuel typeNumber of
FAsBurn-up, max.%
Load, kW/m
Temperature, 0С Reactor
(U, Pu)O2
Civil grade/ or
weapon quality330 30,3 51,5 720 BOR-60
UO2 + PuO2
Civil grade/ or
weapon quality132 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
DDP MOXPuO2 flow sheet
Cathode(pyrographite)
Stirrer
Stirrer
UO2
2+
O2
Pu4
+
PuO22
+
+
Pu4
+ UO22+
UO2 PuO2
UO22+
UO2 +
NpO2
Cl2 Ar (Cl2) Cl2+O2+Ar Cl2+O2+ArStirrerCathode
Na3PO4
+
Fuel chlorination
700 оС
pyrographite bath,
NaCl - KCl
Preliminary electrolysis
680 оС
Precipitation crystallization
680 оС
Electrolysis-additional 700
оС
Melt purification700 оС
UO22+
PuO2
Cl-
(MA,REE) RW4
UO2
MA,REE
NpO2+
Cathode(pyrographite)Stirrer
UO2
2+
+
Pu4
+ UO22+
UO2 PuO2
Cl2 Cl2+O2+ArStirrerCathode
Na3PO4
Fuel chlorination
650 оС
pyrographite bath,
NaCl -2CsCl
Electrolysis-additional 630
оС
Melt purification6500 оС
Cl-
(MA,REE) RW4
MA,REE
UO22+
UO2 +
NpO2
Ar (Cl2)
+
Preliminary electrolysis
630 оС
NpO2+
DDP MOXMOX flow sheet
UO22+
MOX
Cl2+O2+Ar
+
Main MOX electrolysis
630 оС
PuO2+
PuO2+
MOX
12
MOX-MOX Reprocessing
2004 YearMOX - 3 400 g Pu content - 33,5 % wt.
2000 YearMOX - 3 200 gPu content - 10 % wt.
13
Pyro HLW treatment
Salt residueSalt
purificationPyroreprocessing
Na3PO4
Phosphates
Fission products
Radioactive Cs
NaClCsClNdPO4C
ePO4
Waste Phosphates Salt residue
Special features
contain fission productsAlkaline metal chlorides, high activity, significant
heat release
Basic elements11 wt.% Nd4,4 wt.% Ce
81,96 wt.% CsCl18,04 wt.% NaCl
Quantity* <0,15 kg/kg of fast reactor SNF
<0,03 kg/kg of fast reactor SNF
14* - TOSHIBA estimation for DDP
Characteristic
HLW type
Phosphate precipitate
Spent salt electrolyte
Phosphate precipitate + spent
salt electrolyte
Glass matrix typePb(PO3)2
NaPO3
NaPO3, AlF3
Al2O3
NaPO3, AlF3
Al2O3
Introduction methodvitrification,
Т=9500С
vitrification without chloride
conversion, Т=9500С
vitrification without chloride conversion,
Т=9500С
Introduced waste amount, % 28 20 36
137Cs leaching rate as of the 7th day, g/cm2 * day
7*10-6 7*10-6 4*10-6
Thermal resistance, 0С 400 400 400
Radiation resistance 107 Gr (for and ) 1018 -decay/g
Vitrification of HLW from pyro process
15
Characteristics Type of high-level wastes
Phosphate deposit Spent salt electrolyte
Type of ceramics monazite Cosnarite (NZP)
Method of introduction into ceramics 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
Thermal stability, 0С 850 1000
Radiation resistance 5*108 Gy( for and ) 1019 - decay/g
Ceramization of HLW arising from pyro process
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
Experience in DOVITA Program
Irradiated (U,Np)O2 fuel, 19% burn-up
Pyrochemical technology of adding Np into oxide fuel (5-
20%) 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
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 DOVITA-2
1992 Dry technologies Oxide fuel with MA Vi-pack Integrated disposition
same site with the reactor
TA Transmutation of Actinides
2007+Dry technologiesOn-site reprocessingVarious type of fuel with
MAIntegration of MA
recycling into FR Closed Fuel Cycle
TA - Transmutation of Actinides 20
DOVITA-2
Fuel type/ Stages
Oxide vi-pack
Oxide pellet
Nitride vi-pack
Metal Molten salt
Concept Studies
+ + + +/- +
R&D + -/+ +/- - +
Fuel Production
+ - - - -
Irradiation Testing
+ - - - -
PIE + - - - ----
Reprocessing -/+ - - - +/-
DOVITA-121
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
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
(NaCl-2CsCl, T=550oC)
PuO2 Pellets
(3LiCl-2KCl, T=450oC)
PuO2 Pellets Characteristics
25
80%UO2 + 20%PuO2 MOX Pyro Pellets
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.
MOX Pellets Characteristics
26
0
10
20
30
40
50
60
70
80
90
3000 3500 4000 4500 5000 5500 6000
Расстояние, мкм
Массовая д
ол
я U
, P
u,%
U Pu
μm
Cont
ent,
wt%
Composition of pellet Medium of powder production
Insoluble residue,
% wt.
Residue composition, wt%
80wt%UO2
+20wt%PuO2
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
EPMA
Solubility test in 8M HNO3 at 95-96оC , duration – 10 hrs.
Pickled pelletUnpickled pellet
Microstructure of MOX pellets
Pyro MOX pellets (80%UO2 + 20%PuO2)
27
Fundamental Studies
Curium containing salt for spectroscopy studies
NaCl-2CsCl-CmCl3(0.115mol/kg)
29
-0.05
0.25
0.55
320 370 420 470 520
wave-length, nm
tra
ns
mis
sio
n d
en
sit
y
Spectrum of curium-containing melt under atmosphere of Ar- HCl-H2O
NaCl-2CsCl-CmCl3(0.115mol/kg)
750oC
log(P2HCl/PH2O)=-7.14
Cm3+
Am3+
CmO+
30
Cavity from optical quartz
Oxygen sensor
Oxygen pump
CE
RE
Gas-supply tube
Synchronized potentiometric titration by oxygen pump and spectroscopy
31
MA and FP Partitioning
-1.6
-1.4
-1.2
-1
-0.8
-0.6
-0.4
-0.2
0
0 200 400 600 800 1000 1200 1400
Time, sec
I, A
Ga cathod
Run #
T,oC Weight, g Content in melt, % E, V
(Li,K,Cs)Cl Ga Am Ce
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
32
RIAR Site
Post Irradiation complex
RadioWaste complex
Chemical-Technological complexRadiochemical
Complex
R&D on Reprocessing
and Refabrication
of Advanced Fuels
Post Irradiation Examination
MBIR
Вибро
MOX or other fuel
ПироRefabricated Fuel
Отходы на хранение
electricityHeat powerradionuclides
Pyro
Vi-pack
RAW
RIAR Radiochemical Complex
CFC Pyro technology for International RIAR-based Center of
Excellence
MOX Production
Facility
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