future nuclear fuel cycles : prospects and challenges · radiochemistry and processes department....
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IEMPT-10, Mito, Japan, October 8, 2008 1/22Radiochemistry and Processes Department
FUTURE NUCLEAR FUEL CYCLES :PROSPECTS AND CHALLENGES
D. WARIN, B. BOULLISCEA, Nuclear Energy Division
1 – Main achievement in the frame of 1991 Act 2 – P and T in the 2006 Act3 – Fuel cycle possible options 4 – On going R and D programs
The Tenth OECD Nuclear Energy Agency Information Exchange Meetingon Actinide and Fission Product Partitioning and Transmutation
IEMPT-10, Mito, Japan, October 8, 2008 2/22Radiochemistry and Processes Department
The 1991 French Act: frame of the Program
3 Research thematics:
● partitioning and transmutation of LLRNs
● deep repository
● confinement and interim storage
Deadline : final report in 2006
December 30, 1991
IEMPT-10, Mito, Japan, October 8, 2008 3/22Radiochemistry and Processes Department
Minor Actinide Partitioning strategy
Two
step
stra
tegy
Spent Fuel
U, Pu Np
Ln
PUREX
SANEX
FissionProducts DIAMEX CO-EXTRACTION
of MAs and Ln
SEPARATIONof Mas from LnAm, Cm
IEMPT-10, Mito, Japan, October 8, 2008 4/22Radiochemistry and Processes Department
DIAMEX demonstrative hot run, Nov. 2005
Am ~ 0.015 %Cm < 0.002 %
extraction
(CP)(CP)
-
HEDTA
HNO3H2C2O4HEDTA
HNO3
FPRaffinate
extractionAn+ Ln
(CP)
ScrubbingFP
(CP)
Am, Cm, Ln> 99.9%
Back-extraction An-Ln (MS)
NaOHHEDTA
Solvent Treatment(ECRAN)
0.65 MDMDOHEMA/TPH
PUREX raffinate15 kg genuine fuel
Ln ~ 2.5 g/L
Am ~ 150 mg/LCm ~ 15 mg/L
V ~ 1 L/h4 m highPulsed columns HNO3
H2C2O4HEDTA
HNO3
extraction
(CP)
extractionAn+ Ln
(CP)
DIAMEXProductionAm, Cm, Ln
IEMPT-10, Mito, Japan, October 8, 2008 5/22Radiochemistry and Processes Department
An
Solvent DMDOHEMA 0.5 M
+ HDEHP 0.3 MTPH
Lnscrubbing
HNO3
extraction-scrubbing
HEDTACitric ac.
Ln stripping
LnHNO3
DIAMEXProductionAm, Cm, Ln~ 45 mL/h
NaOHHEDTA
HNO3
An stripping
Am, Cm < 0.01%
Am, Cm > 99.9%F.D.Ln ~ 80 Am < 0.06 %
Cm < 0.03 %
Raffinate
SANEX demonstrative hot run, December 2005
IEMPT-10, Mito, Japan, October 8, 2008 6/22Radiochemistry and Processes Department
The 2006 French Act
PRINCIPLES : ● Recycle (reprocess)
to decrease waste amount and toxicity
● Retrievable Geological Repository,the reference option for ultimate waste management
A « ROADMAP » :● 2012 : industrial potentialities of the diverse P&T
options, and prototype by 2020● 2015 : repository defined, and operation by 2025
June 28, 2006
IEMPT-10, Mito, Japan, October 8, 2008 7/22Radiochemistry and Processes Department
(Article 3) PARTITIONING and TRANSMUTATION OF LLRNs
« The research in this field will be connected toresearch concerning the new generation of nuclearreactors, as well as accelerator driven systemsdevoted to waste transmutation, in order to have, by2012, an evaluation of the industrial potentialities ofthese concepts, and in order to start operating aprototype before December 31st, 2020… »
The 2006 French Act
IEMPT-10, Mito, Japan, October 8, 2008 8/22Radiochemistry and Processes Department
Minor Actinide Partitioning : what processes ?
Solvent extraction, first !● Already developed at commercial plant scale
(Industrial potentiality)● high separation yields !● low amount of secondary waste !
The main alternative: Pyro_processes
IEMPT-10, Mito, Japan, October 8, 2008 9/22Radiochemistry and Processes Department
Define the several options of interest, which could be successively deployed (all-actinide, Americium only, heterogeneous, homogeneous,…)
Assess benefits /costs ratiofor the several recycling options, considering diverse criteria and “densification” of the final storage
Design / Optimize separation processes, transmutation fuels and their fabrication processes
and gather technical elements for industrial operation evaluation
Future fuel cycle options : the 2012 milestone
IEMPT-10, Mito, Japan, October 8, 2008 10/22Radiochemistry and Processes Department
R T
U
U PuU and Pu recycled,
COEX
MA homogeneous recycling
R T
U
FP
U Pu AM
R T
U
MAU Pu
FPFP&MA
MA heterogeneous recycling
R TU
UU and Pu recycled,
PUREX
Pu
FP&MA R T
U
U Pu
FP
TADS
« double strata »
MA
Future fuel cycle options, Reactor and Treatment
IEMPT-10, Mito, Japan, October 8, 2008 11/22Radiochemistry and Processes Department
Fuel cycle, the « COEXTM » concept
- U and Pu recycling, extraction-fabrication- without anywhere, anytime « pure » plutonium- suitable for Gen3 and MOX-LWRs- a first step before more advanced options ?
REACTOR TREATMENT
URANIUM
FPs & MAs
Pu and UU
IEMPT-10, Mito, Japan, October 8, 2008 12/22Radiochemistry and Processes Department
Fuel cycle, the MA heterogeneous recycling option
FPs
- U, Pu, Np by COEXTM (or PUREX)- Am (and Cm) separation : DIAMEX, SANEX,…- Am (and Cm) recycled on dedicated « targets-blankets »
REACTOR TREATMENT
URANIUM
MAs
Pu,U,(Np) U
IEMPT-10, Mito, Japan, October 8, 2008 13/22Radiochemistry and Processes Department
DIAMEX-SANEX with extractant separation
DTPA or HEDTA Glycolic acid
pH 3
PUREX raffinate
EXTRACTION / SCRUB. (DIAMEX process)
F.P.(except Ln+Y)
Ln + Y
Ln STRIPPING
Am + Cm
An STRIPPING
HNO3
DMDOHEMAHTP
Acidic extractantHTP
HNO3HEDTA. oxalic acid
HNO3
DMDOHEMA HTP
DMDOHEMA Solvent
treatment
pH > 5
Extractantseparation
Fuel cycle, the MA heterogeneous recycling option
(hot test scheduled in 2009)
IEMPT-10, Mito, Japan, October 8, 2008 14/22Radiochemistry and Processes Department
- U, Pu, Np by COEXTM + Am (and Cm) by DIAMEX-SANEX
- or all-actinide grouped management (GANEX), the mostadvanced option, but drawbacks for fuel cycle operation
FPsREACTOR TREATMENT
URANIUM
Pu, U, MAs U
Fuel cycle, the MA homogeneous recycling option
IEMPT-10, Mito, Japan, October 8, 2008 15/22Radiochemistry and Processes Department
F.P.
DISSOLUTION
Spent fuel
1st step U Extraction
Ln Stripping
Ln
WASTE
UPuNpAmCm ConversionDISSOLUTION
U
Pu+MA
2nd step An Stripping
Ln
RECYCLE
Fuel cycle, the GANEX concept
IEMPT-10, Mito, Japan, October 8, 2008 16/22Radiochemistry and Processes Department
1st step : U selective extraction
2nd step : Pu-Np-Am-Cm co-recovery (diamide-based process)
(scheduled in November 2008)
Fuel cycle, the GANEX hot runs in Atalante
(performed successfully in June 2008)
Solvent clean-up
Mono Amide
Extraction Scrubbing U stripping
FeedNp, Pu, Am, Cm + FPs
HNO3 Diluted HNO3
U
U > 99.9%
IEMPT-10, Mito, Japan, October 8, 2008 17/22Radiochemistry and Processes Department
Atalante/L15
U 70 % - Pu 30 %
U, Pu, Np, AmU 78 % - Pu 20 % - Np 1% - Am 1 %
Continuous operation
ATALANTE – L15
U, Pu,Np
Fuel cycle, from MA solutions to fuels
Actinide oxalic co-conversion (precipitation, filtration, calcination)
COPIX (UPu)O2 irradiation test in Phénix, 2008-2009
IEMPT-10, Mito, Japan, October 8, 2008 18/22Radiochemistry and Processes Department
Fluoride Salt
Metal Solvent
AnF3
An
AlF3An
Al
Actinide distribution coefficients >100 An/Ln separation factors > 1000
CEA Pyro reference route: reductive extraction
Salt before extraction
Salt after extraction• Attractive potentialities:•Compactness•No radiolytical effects•Suitable for advanced fuels, hot fuels•…
• but still heavy work, still questions:•Operating pyro-processes at industrial scale ?•Technological waste amount ?
Al
IEMPT-10, Mito, Japan, October 8, 2008 19/22Radiochemistry and Processes Department
Separation process : CEA on going R and D
COEXTM: « Demo runs » (separation, conversion, COPIX)
DIAMEX, SANEX :● Single cycle flowsheets● « Am only » recovery concepts
GANEX :● 1st and 2nd cycles● New flowsheets considered…
Atalante new hot runs : from 2008 to 2012
PYRO: Stripping in molten salts (after extraction)
IEMPT-10, Mito, Japan, October 8, 2008 20/22Radiochemistry and Processes Department
Separation process : consolidation towards industrialization
NCH3
C8H17
NCH3
C8H17
O O
C2H4
OC6H13
Extractantsynthesis
Modeling(flowsheet, sensitivity, operation)
DMDOHEMA + HDEHP
RaffinatPUREX
Ln stripping
Ln
Extr-scrub.
PF
An(III) + Ln(III)
DTPA pH 3-4
An stripping Ln(III)
An
Core of the process demonstrated at small scale
Long term effects(solvent treatment)
Equipments(Implementation,extrapolation) In situ
analysis(cations,
pH...)
InterfaceCo-conversion
FP solution adaptedto vitrification
(Concent. Calcination)
IEMPT-10, Mito, Japan, October 8, 2008 21/22Radiochemistry and Processes Department
New workshops at La Hague Areva plant ?
SFR MOX FUEL FABRICATION
MINOR ACTINIDE PILOT
(remote fabrication)(the core of SFR proto ASTRID, tons) (experimental pins,
MONJU demo, kg)
IEMPT-10, Mito, Japan, October 8, 2008 22/22Radiochemistry and Processes Department
En résumé… towards 2012 milestoneRecycling options, for sustainable systems
Many options still open (what, and how)
A progressive step by step approach,(from U and Pu first, to MA recovery?)
A need for flexible processes?
On-going research in the Atalante facility(many process options already explored)
A consolidation program for industrial potentiality
Prototype(s) fuels (driver fuel, and MA-bearing experimental fuel): new facilities under design, and open to international collaboration
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