French fuel cycle strategy and partitioning and ... · DEN 9-IEMPT NIMES September 26 , 2006 6 Which goals? Goal 1 research : solutions that would allow partitioning and transmutation

1DEN 9-IEMPT NIMES September 26 , 2006

French fuel cycle strategy

and partitioning and transmutation programme

Philippe PRADELNuclear Energy Division

Charles COURTOISNuclear Energy Division / Waste Management Research Program


UP2-800 : 1994 : Commissioned for PWR fuelsCapacity : 800 t/y(Its an upgrade of UP2-400)Dedicated to French customers (EDF)

UP3 :1990 : Commissioned for PWR fuelsCapacity : 800 t/yDedicated to foreign customers

Reaching maturity : the 90’

Reprocessing :The La Hague integrated site


Relative contribution to totalradiotoxicity after 1 000 years

Fission products

Minor actinides

Plutonium

Cladding & structural materials : medium level & long lived waste

Recyclable materials (95 %)Fission products :25 kg

Minor actinides :~ 0,5 kg

Vitrified HL radwaste (5%) Plutonium :

5 kg (1 %)

Uranium :

470 kg (94 %)

Spent fuel processingSpent fuel processing

Current scheme for the PUREX process


Waste management

Heat load of the TRU Potential radiotoxicity

(241Pu ---> 241Am ---> 237Np)

• Urgent matter for public acceptance of nuclear energy• Recycling minimizes both the repository space and

environmental impact

1st contributor : Pu ; 2nd contributor : Minor Actinides (MA)


Bitumen

Grout concreteTechnological waste

Glass

ConcreteHulls & end fittings

CompactionHulls, end fittings &technological waste

Volume of waste in m3/tHM

0

3

2

1

4

1995 20001989(Design)

0.1 % 0.1 %1 % 100 %Pu losses

Fuel treatment optimization : Specific waste volume for the UP3 plant

Conditionedspent fuel


Which goals?Goal 1 research : solutions that would allow partitioningand transmutation of long lived radionuclides present in HL LL waste and reduce the overall radwaste quantity and toxicity.

Goal 2 research : feasibility of reversible or irreversible repository in deep geological formations.

Goal 3 research : conditioning processes and feasibility of long term storage, above-grade or below-grade.

Deadline set in law : 2006

The Law of December 30, 1991


Partitioning : key nuclides

minor actinides : Am - Cm - Npmajor contributors to long term radiotoxicinventory;

fission products : I - Cs - Tc– long lived isotopes significantly present in spent fuel,– with a potential for mobility within rock formations;

processes : hydro-metallurgy (consistent with PUREX) and pyro-chemistry (more innovative);

partitioning of nuclides present in the already vitrified HL waste would be rather difficult.


Research steps

Fundamental research : a wide co-operative framework- exploration : new extracting systems ;- fundamentals : in-depth study of mechanisms

at work ;

Applied research :- process design ;- lab experiments on actual spent fuel

material ;- « demonstration » experiments :

integration, representativeness, long-lastingperformance ;

A true challenge : a sophisticated partitioning chemistry under highly radioactive conditions.

A few hundreds

of new molecules

Scale : 1/10000

Scale : 1/100 à 1/1000


Actinides partitioning : research path used

Spent fuel

U, Pu Np

Cm

AmLn

PUREXPUREX

SANEXSANEX

Fissionproducts DIAMEXDIAMEX CO-EXTRACTION

of An et LnCO-EXTRACTION

of An et Ln

PARTITIONINGbetween An & LnPARTITIONING

between An & Ln

1

H2

He3

Li4

Be5

B6

C7

N8

O9

F10

Ne11

Na12

Mg13

Al14

Si15

P16

S17

Cl18

A19

K20

Ca21

Sc22

Ti23

V24

Cr25

Mn26

Fe27

Co28

Ni29

Cu30

Zn31

Ga32

Ge33

As34

Se35

Br36

Kr37

Rb38

Sr39

Y40

Zr41

Nb42

Mo43

Tc44

Ru45

Rh46

Pd47

Ag48

Cd49

In50

Sn51

Sb52

Te53

I54

Xe55

Cs56

Ba Ln72

Hf73

Ta74

W75

Re76

Os77

Ir78

Pt79

Au80

Hg81

Tl82

Pb83

Bi84

Po85

At86

Rn87

Fr88

Ra An104

Rf105

Db106

Sg107

Bh108

Hs109

Mt110

Uun

LANTHANIDES

57

La58

Ce59

Pr60

Nd61

Pm62

Sm63

Eu64

Gd65

Tb66

Dy67

Ho68

Er69

Tm70

Yb71

Lu

ACTINIDES

89

Ac90

Th91

Pa92

U93

Np94

Pu95

Am96

Cm97

Bk98

Cf99

Es100

Fm101

Md102

No103

Lr

NOYAUX LOURDS PRODUITS D’ACTIVATION

PRODUITS DE FISSION PRODUITS DE FISSION ET D’ACTIVATION


The ATALANTE facility…

From basic studies to demonstrative experiments …… up to kgs of spent fuel


Am, Cm, Np, Tc, I et Cs partitioning :lab scale results

Americium & curium : recovery ratio up to 99,9%for Am & 99,9% for Cm ;

long-lasting performance tested (« accelerated » simulation within an irradiation loop) ;

confirmation test with the use of « industrial » technology have been successful in 2005 ;

Neptunium : recovery ratio up to 99% ;

Technetium : recovery ratio from 45 à 90%;

Iodine : - recovery ratio > 97% with PUREX; - additional recovery up to ~ 99% possible ;

Caesium : recovery ratio > 99,8%, with the use of the calixarene extractant.

N

O

C2H4

N

O

C8H17

CH3CH3

C8H17O

C6H13

DMDOHEMA

OP

O

O O

HHDEHP

N

O

O

ON

OH

OH

OHOHHEDTA


Conclusion …. for partitioning R&D

A large scope for research :from fundamentals to applications;

- the actinides: the key target;

- partitioning of nuclides present in the already vitrified HL waste is no more considered.

- a scope wide open : (numerous options explored and co-operations);

- feasibility of pyro-chemical processes not yet demonstrated;

- molecules and partitioning processessuccessfully tested at the lab scale;

- and successfully tested in 2005 within the Atalante hot cells (to replicate an industrial-like set-up);

- a research booster for partitioning and actinides chemistry;

- further steps will be required prior to any industrial implementation.

Atalante in Marcoule

CBP


Transmutation : capture & fission

Making use of neutron flux (within a reactor) to turn LL radionuclides into stable or shorter-lived isotopes through neutron capture or fission reactions.

For actinides, fission reaction, not neutron capture, must be considered.

For fission products, neutron capture reactions are observed resulting in stable or short-lived nuclides.


Transmutation output according to neutron spectrums used

- Two recycling modes have been considered : homogeneous mix within the nuclear fuel or heterogeneous in targets at higher concentrations;

- There is obviously a net advantage in using a fast neutron flux to get higher fission rate, however increasing the fission rate requires multiple recycling ;

Fast neutron flux and spectrum are more efficient to transmute actinides through fission reaction.

R&D on basic nuclear data :Nuclear data obtained on actinides cross-sections is used to rank the

transmutation potential of various systems.


Transmutation tools : existing reactors?(1/2)

• PWR : the scientific feasibility to transmute americium is established; however more enriched uranium is needed in the fuel and more curium is produced as a result, which is not recyclable in PWR;

PHENIX

FNR should be able to help eliminate minor actinides produced in the existing PWR fleet of reactors and to manage those produced within FNR.

• FNR : minor actinides transmutation is established with no detriment on the normal operating conditions of the reactor.

REP


Transmutation tools : future reactors ? (2/2)

• FNR-gas (GEN IV) :- up to 5 % of minor actinides

concentration in fuel could be acceptable (only limited by the fuel behaviour under irradiation);

• Hybrid systems (ADS) : 5th et 6th

European FP, CEA/CNRS collaboration :- significant R&D work is on-going,- ADS concept is highly complex,

however there appears to be so far no show-stoppers towards demonstrating the feasibility of an experimental facility,

- nevertheless, stumbling stones have been highlighted.

ADS

Génération IVInternational

Forum Members


Forum Members

U.S.A.U.S.A. Génération IVInternational

Forum Members


Forum Members

U.S.A.U.S.A.U.S.A.U.S.A.U.S.A.U.S.A.

ArgentinaArgentinaArgentinaArgentinaArgentinaArgentinaArgentinaArgentina

BrazilBrazilBrazilBrazil

CanadaCanada

BrazilBrazilBrazilBrazil

CanadaCanadaCanadaCanadaFranceFranceFranceFrance

JapanJapanJapanJapan

CanadaCanadaFranceFranceFranceFrance

JapanJapanJapanJapan

South AfricaSouth AfricaSouth AfricaSouth AfricaSouth AfricaSouth Africa

UnitedUnitedKingdomKingdom

South AfricaSouth Africa

UnitedUnitedKingdomKingdomUnitedUnitedKingdomKingdom

South KoreaSouth Korea

SwitzerlSwitzerlandand

SwitzerlSwitzerlandand

E.U.E.U.E.U.E.U.


Nuclear fuel for transmutation : current R&D programmesReactors in use or considered :

- irradiation reactors : HFR,SILOE;- fast neutron research reactors :

• PHENIX,• JOYO, MONJU (Japan),• BOR 60 (Russia).

Design and fabrication of experimental fuel, and associated safety case ;

- irradiation (minimum 5 years),- non destructive and destructive examinations,- 35 irradiation experiments have been conducted or

are on-going.

PHENIX

Results validation :- actinides concentration and burn-ups;- fission rate for one cycle :

i.e. 70% of the americium contained in one target has undergone fission.


Conclusion … for transmutation

the feasibility of transmuting actinides such as Am and Np is recognised in fast neutron reactors according to experiments run in SFR;

ADS systems are quite complex, and their technical and economical viability for actinides transmutation is yet to be proven;

transmutation of technetium 99 is feasible, but not efficient;

transmutation of caesium 135 is no longer pursued;

transmutation of iodine 129 is not currently feasible.

Reducing the ultimate waste radiotoxicinventory is possible with implementinga continuous improvement step-wise process;

Goal 1 cannot apply to current ultimatewaste (vitrified).

An international expert peer-review report is available

1

0,1

10

100

1000

10000

10 100 1000 10000 100000 1000000Temps (années)

Rad

ioto

xici

té rela

tive

PFAM +PF

Combustible usé( Pu+ AM + PF)

Minerai uranium naturel1

0,1

10

100

1000

10000

10 100 1000 10000 100000 1000000Temps (années)

Rad

ioto

xici

té rela

tive

Combustible usé(U + Pu +Actinides Mineurs + Produits de Fission)

Actinides Mineurs+ Produits de Fission

Produits de Fission


Future nuclear systems for a nuclear renaissance

• It clearly means fast reactors for sustainability,

• Sodium fast reactor is more mature

• Gas fast reactor is an alternate track

• Minor Actinides recycling may be a progressive approach


ReferencesPresident Chirac statement (Jan 06) : « A number of countries are working on future generation reactors, to become operational in 2030-2040, which will produce less waste and will make a better use of fissile materials. I have decided to launch, starting today, the design work by CEA of a prototype of the 4th generation reactor, which will be commissioned in 2020.We will naturally welcome industrial or

international partners who would like to get involved. »

The Radwaste Management Act (June 06) :“Transmutation : studies to be carried out within the R&D framework of future nuclear energy and ADS systems - aiming at 2012 for the technical feasibility evaluation (industrial level), and 2020 for the commissioning of a prototype”.


Nuclear Fuel Cycle Goals

R T

Ude

FP

U Pu MA

R T

Ude

MAU Pu

FPR T

Ude

FP MA

U Pu

Homogeneousrecycling (GenIV)

Heterogeneousrecycling

U & Pu recycling

Natural resources conservation

Waste minimisation

Proliferation resistance

All paths should be kept available, they could be used in a sequence.

50 more electricityproduced with the same

quantity of naturaluranium


The next generations of reprocessing facilities

UOx – LWR fuel1000 t/yearPUREX process MOX & UOx LWR fuels

Higher throughputIntegrated fuel processing and recycling : COEXAdvanced separation technologies

LWR & FR fuels> 2000 t/yearNew technologies

1990

∼ 2020

> 2040

Gen II

Gen III

Gen IV


Looking for a long term management strategy?Results already in use :

- improved industrial facilities and processes;- since 1991, significant waste volume reduction

(by a factor of 6);- feasibility of disposal

A continuous improvement process to be continued:- for opening the scope of possible solutions;- and defining future electricity generating systems.

A new bill.Ufrom mine

Actinides

Comb.usé

Ultimatewaste

FP

GEN IV NR

Traitement et

Re-fabrication

U

Actinides

Spent.fuel

GEN IV NR

-

- Minimising ultimate waste

- Optimal use of energy-bearing natural resources

- Proliferation resistance

Documents

French fuel cycle strategy and partitioning and ... · DEN 9-IEMPT NIMES September 26 , 2006 6 Which goals? Goal 1 research : solutions that would allow partitioning and transmutation