future nuclear fuel cycles : prospects and challenges · radiochemistry and processes department....

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


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


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


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


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


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


(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


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


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


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


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


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


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)


- 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


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


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%


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


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


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)


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)


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)


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

future nuclear fuel cycles : prospects and challenges · radiochemistry and processes department....

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