French fuel cycle strategy
and partitioning andtransmutation programmePhilippe PRADEL
Nuclear Energy DivisionCharles COURTOIS
Nuclear Energy Division / Waste Management Research Program

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1Reaching maturity : the 90’

Reprocessing :The La Hague integrated site
UP2-800 :1994 : Commissioned for PWR fuels
Capacity : 800 t/y(Its an upgrade of UP2-400)
Dedicated to French customers (EDF)

UP3 :1990 : Commissioned for PWR fuels
Capacity : 800 t/y
Dedicated to foreign customers

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2Spent fuel processing

Cladding & structural materials : medium level& long lived waste

Plutonium

Recyclable materials (95 %) Vitrified HL radwaste (5%)
Uranium :470 kg(94 %)

Plutonium :5 kg(1 %)Fission products :25 kg
Minor actinides :~ 0,5 kg

Current scheme for the PUREX process

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Minor actinides
Fission products
Relative contribution to total
radiotoxicity after 1 000 years

3Waste management• Urgent matter for public acceptance of nuclear energy• Recycling minimizes both the repository space andenvironmental impact
1st contributor : Pu;

2nd contributor : Minor Actinides (MA)Heat load of the TRU

Potential radiotoxicity(241Pu ---> 241Am ---> 237Np)
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Fuel treatment optimization : Specific waste volume for the UP3 plant

Volume of waste in m3/tHM
Bitumen

4

Grout concrete
Technological waste

Conditioned
spent fuel

3

Glass
2

Concrete
Hulls & end fittings

1Compaction
Hulls, end fittings &technological waste

01989

1995

2000

0.1 %

0.1 %(Design)

Pu losses
DEN

1%

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100 %5

The Law of December 30, 1991

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

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

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

BDeadline set in law : 2006
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Partitioning : key nuclides
Ö minor actinides : Am - Cm - Np
major contributors to long term radiotoxicinventory;
Ö fission products : I - Cs - Tc
– long lived isotopes significantly present in spent fuel,– with a potential for mobility within rock formations;
Ö processes : hydro-metallurgy (consistent with PUREX) andpyro-chemistry (more innovative);Ö partitioning of nuclides present in the already vitrified HL waste
would be rather difficult.

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Research steps
Ö Fundamental research : a wide co-operative framework- exploration : new extracting systems ;- fundamentals : in-depth study of mechanisms
at work ;A few hundredsof new moleculesÖ Applied research :- process design ;- lab experiments on actual spent fuelScale : 1/10000material ;- « demonstration » experiments :
integration, representativeness, long-lasting
Scale : 1/100 à 1/1000
performance ;Ö A true challenge : a sophisticated partitioning
chemistry under highly radioactive conditions.
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Actinides partitioning : research path used
12HHe

34Li
115Be
13Na Mg
20K
37Rb55CaSc
39Sr

YCs

Ba
88

Ra

An
57

LANTHANIDESACTINIDESU,Pu

PUREX
PUREX

Fissionproducts

DIAMEX
DIAMEX

Np

La

VCr
42Ta

Mn
43

74

Tc
75

Fe44Se
52

Hg

Hs

59

60

6162

Pa

As
51

Au

BhTh

Ge50

Cd

Sg

Ac

Ga
In
81

Sb
83

TlPb

DEN

SANEX
SANEX

Bi

Po

64

65

66

67

GdTb

Dy

Ho

92

96

97

98

99

93

94

95

Np

Pu Am Cm Bk

Cf

68

Er
100

69

At

70

71

Tm Yb

Lu

101

103

102

Es Fm Md No

NOYAUX LOURDSPRODUITS D’ACTIVATIONPRODUITS DE FISSION

PRODUITS DE FISSION ET D’ACTIVATIONPARTITIONINGPARTITIONING
between An
An && Ln
Ln
Cm between

September 26 , 2006

I

Mt Uun
63

9Kr54

85

CO-EXTRACTION
CO-EXTRACTION
ofof AnAn etet Ln
Ln

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Br

Te84

A
3653

AmLn

Cl

110

Nd Pm Sm Eu
U

Sn
82

Ne
18

35

4980

Db

S
34

Zn

Ag

Pt

P
33

F
1748

79

Ir

Si
32

10O
16Cu

Pd

109

31

N
15

947

78

Os

91

Ni
46

30

Rh

108

90

Co
45

2977

Re

89

28

Ru

107

Pr

27

76

106

CeW

26105

Rf5825

Nb Mo
73

Hf
104

2441

Zr72

Ln

23

Ti
40

56

Fr

Spent fuel228C14Al
213887

7B

12196LrXe86Rn

The ATALANTE facility…

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

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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 ;H 3CNNÖ long-lasting performance tested (« accelerated »C 8H 17
simulation within an irradiation loop) ;Ö confirmation test with the use of « industrial »technology have been successful in 2005 ;OO

C 2H 4CH 3
C 8H 17OC 6H 13DMDOHEMA

Neptunium : recovery ratio up to 99% ;OTechnetium : recovery ratio from 45 à 90%;

OP

HDEHP

OIodine :OH- recovery ratio > 97% with PUREX;- additional recovery up to ~ 99% possible ;OHO
HOCaesium : recovery ratio > 99,8%, with the use of theDEN

O

HEDTA

calixarene extractant.

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NNHOOOH

11

Conclusion …. for partitioning R&DÖA large scope for research :from fundamentals to applications;-the actinides: the key target;-

partitioning of nuclides present in the alreadyvitrified 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 processes
successfully tested at the lab scale;-and successfully tested in 2005 within theAtalante hot cells (to replicate an industrial-likeset-up);-a research booster for partitioning and actinides
chemistry;-

further steps will be required prior to any
industrial implementation.

Atalante in Marcoule

CBP
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Transmutation : capture & fission
Ö Making use of neutron flux (within a reactor) to turn LL radionuclides into stable orshorter-lived isotopes through neutron capture or fission reactions.

For actinides, fission reaction, notneutron capture, must be considered.

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

13

Transmutation output
according to neutron spectrums used

R&D on basic nuclear data :ÖNuclear data obtained on actinides cross-sections is used to rank thetransmutation potential of various systems.

- Two recycling modes have been considered : homogeneous mix within thenuclear 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 ;ÖFast neutron flux and spectrum are more efficient to transmute actinides
through fission reaction.

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September 26 , 200614Transmutation tools : existing reactors?(1/2)• PWR : the scientific feasibility to transmute
americium is established; however moreenriched uranium is needed in the fuel andmore curium is produced as a result, which is
not recyclable in PWR;
REP

• FNR : minor actinides transmutation is established with no
detriment on the normal operating conditions of the reactor.
ÖFNR should be able to help
eliminate minor actinides
produced in the existing PWR fleetof reactors and to manage those
produced within FNR.
PHENIXDEN

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Transmutation tools : future reactors ? (2/2)•FNR-gas (GEN IV) :- up to 5 % of minor actinides
concentration in fuel could beacceptable (only limited by the fuelbehaviour 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 anexperimental facility,- nevertheless, stumbling stones havebeen highlighted.

FranceUnitedKingdomE.U.
Génération IV

CanadaU.S.A.
BrazilInternational
ForumMembers

Argentina
South Africa

SwitzerlandJapan

South Korea

ADS

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Nuclear fuel for transmutation : current R&D programmes
Ö Reactors in use or considered :- irradiation reactors : HFR,SILOE;- fast neutron research reactors :• PHENIX,• JOYO, MONJU (Japan),• BOR 60 (Russia).
PHENIXÖ Design and fabrication of experimental fuel, andassociated safety case ;- irradiation (minimum 5 years),- non destructive and destructive examinations,- 35 irradiation experiments have been conducted or
are on-going.

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.

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Conclusion … for transmutation
10000

Ö the feasibility of transmuting
actinides such as Am and Np is
recognised in fast neutron reactors
according to experiments run in SFR;Ö ADS systems are quite complex,
and their technical and economical
viability for actinides transmutation is
yet to be proven;Ö transmutation of technetium 99 isfeasible, but not efficient;transmutation of caesium 135 is nolonger pursued;transmutation of iodine 129 is not
currently feasible.

DEN

Radiotoxicité
relative

1000

100
Combustible usé(U + Puusé
Combustible+Actinides( Pu+AM + PF)Mineurs+ Produits de Fission)

10
Minerai uranium
naturel
Produits de Fission
PF

10,1
10100

AM +PF
Actinides Mineurs+ Produits de Fission
1000
10000
Temps (années)

1000001000000

Ö Reducing the ultimate waste radiotoxic
inventory is possible with implementing
a continuous improvement step-wise process;Ö Goal 1 cannot apply to current ultimate
waste (vitrified).
Ö An international expert peer-review report isavailable

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Future nuclear systems for anuclear 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

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References
President Chirac statement (Jan 06) :« A number of countries are working on future
generation reactors, to become operational in2030-2040, which will produce less waste andwill make a better use of fissile materials.
I have decided to launch, starting today, thedesign work by CEA of a prototype of the 4thgeneration reactor, which will be commissioned
in 2020.
We will naturally welcome industrial orinternational partners who would like to get
involved. »The Radwaste Management Act (June 06) :“Transmutation : studies to be carried out within the R&D frameworkof future nuclear energy and ADS systems - aiming at 2012 for thetechnical feasibility evaluation (industrial level), and 2020 for thecommissioning of a prototype”.
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Nuclear Fuel Cycle Goals
Æ Natural resources conservation
Æ Waste minimisation
Æ Proliferation resistance

50 more electricity
produced with the same
quantity of naturaluranium

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

UdeRT

Ude
FP MART

Ude
FP

R

T

FP

MAU PuU & PurecyclingDEN

U Pu MA

U Pu
Heterogeneous
recycling
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Homogeneous
recycling (GenIV)
21

The next generations of reprocessing facilities
Gen IVLWR & FR fuels> 2000 t/year
New technologies> 2040Gen IIUOx – LWR fuel1000 t/year
PUREX process∼ 2020Gen III
MOX & UOx LWR fuels
Higher throughput
Integrated fuel processing and recycling : COEX
Advanced separation technologies

1990

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Looking for a long term management strategy?
ÖResults already in use :- improved industrial facilities and processes;- since 1991, significant waste volume reduction(by a factor of 6);- feasibility of disposal
ÖA continuous improvement process to be continued:- for opening the scope of possible solutions;- and defining future electricity generating systems.
ÖA new bill.
Ufrom mineSpent.
Comb.
uséfuelGEN IV

Traitement etUltimate
waste- Minimising ultimate waste

Re-fabricationFP- Optimal use of energy-bearing
natural resources

NR- Proliferation resistanceActinides

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23