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Role of Minor Actinides for Protected Plutonium Production (P3) (I)

Application of P3 in Uranium Fueled PWR


Yoga Peryoga and Masaki Saito
Research Laboratory for Nuclear Reactors, Tokyo Institute of Technology
2-12-1, O-okayama, Meguro-ku, Tokyo 152-8550, Japan
Phone: +81-3-5734-3060, Fax: +81-3-5734-2959
E-mail: 02d51204@nr.titech.ac.jp
Vladimir Artisyuk
Obninsk State Technical University for Nuclear Power Engineering (INPE)
2, Studgorodok, Obninsk, Kaluga Region, Russian Federation

Abstract

k-infinity

The present paper describes the utilization of the so far considered as unfriendly material-minor actinide
(MA) elements in a way of finding their merit rather than their geological disposal or elimination as it is.
Based on neutronic properties of minor actinides, a series of their application has been made possible. For
instance, their considerable capture cross section in the thermal neutronic environment would assist their
application in uranium fueled-light water reactor as burnable absorbers and serve as a source of even-mass
plutonium nuclides, e.g. 238Pu with 2.6x103 n/g/s and 567 W/kg of spontaneous fission neutron and decay
heat respectively, to dilute the weapon utilizable material 239Pu in the discharged plutonium. Hence it deals
with the issue on proliferation plutonium with simultaneous reduction of accumulated minor actinides
stockpiles.
An example of minor actinides application in a PWR environment is given in the present paper. Since
americium and curium do not require special proliferation resistance measures, their addition to highly
enriched uranium oxide fuel of 20% 235U (maximum enrichment to be exempted from nuclear explosive
proliferation concern) has been selected. An amount of 3% of their addition to uranium oxide fuel shows the
potential of achieving the burnup value of 100 GWd/tHM with discharged plutonium containing 20%238Pu
after irradiation, hence improves the plutonium proliferation resistance in comparison to 2% 238Pu fraction of
conventional discharged plutonium. An essential fact is that after irradiation of up to 100 GWd/tHM, the
discharged fuel still contains uranium enriched with 10% 235U, therefore giving the possibility to get excess
reactivity of this spent fuel by re-irradiation in the reactor vessel. A one year fuel cooling followed by
enlarging pitch-to-diameter ratio, P/D, up to 2.0 reveals the potential reactivity excess of the spent fuel for
the second irradiation to prolong the burnup for another 46 GWd/tHM as illustrated in Fig. 1 and maintain
the 238Pu fraction at about 20% level after the irradiation, thus sustain the proliferation resistance property of
the fuel.
1.25
1.2
1.15
1.1
1.05
1

1 st Irradiation
(P/D=1.38)

25

50

2 nd Irradiation
(P/D=2.0)

75
100
125
Burnup (GWd/tHM )
Fig. 1 Two strata irradiation of (Am-Cm)-doped UOX (20%235U) fuel

150

Acknowledgement
This work has been supported by the Ministry of Education, Culture, Sport, Science and Technology of
Japan.

Role of Minor Actinides for Protected


Plutonium Production (P3) - I
- Application of P3 in Uranium-Fueled PWR COE-INES Indonesia International Symposium
March 2 4, 2005

Y. Peryoga , M. Saito and V. Artisyuk


a

Research Lab. For Nuclear Reactors, Tokyo Institute of Technology, Japan


Obninsk State Technical University for Nuclear Power Engineering (INPE),
Russian Federation

Backgrounds

Am-241
26.26%

Cm-243
0.03%

Am-242m
0.07%

Cm-244
3.02%

Am-243
13.56%

56.93%

Cm-245
0.09%

235 3.3%

Accumulation of MA
stockpiles from
current spent fuel
Concern on
plutonium
proliferation as
explosive material
The fact that
plutonium is a nice
fuel material for
future use in
replacing the
declining quantity
of uranium

FP
34.9 kg
Fresh fuel
1,000 kg

MA
Np-237

0.93 kg

9.0 kg
PWR

Pu
235 0.8%

238

241

239

242

240

U
238

33
GWd/tHM

54.73%

U
238

1.46%

11.51%
26.22%

6.08%

Radionuclides Accumulated in PWR


(33GWd/tHM, 3 years cooling)

Uranium

Fuel Storage
LWR
U,Pu
U,Pu
Fuel
Fabrication

MA, FP
Reprocessing

Conventional Fuel Cycle

Disposal

Mechanism of Pu
Protection and
Issues on U & Pu
Proliferation

20%
235U

80%

80%
238U

600
Decay Heat (Watt/kg)

exemption from
proliferation concern

238Pu

400

Proposed
Kessler
Heising criteria
proposal (2004)
(1980)

IAEA
criteria
(1972)

200

Cm
242

163 d

Pu-238 Pu-239 Pu-240 Pu-241 Pu-242

Am
241
14.4 yr

2000

Pu
238
1000

Pu
239
2.1d

Np
237

0
Pu-238 Pu-239 Pu-240 Pu-241 Pu-242

Cm
243

83% 16h

3000

Np
238

Pu
240

Pu
241

Pu

Pu

Pu

SFN (n/g/s)

5%
238Pu

12%
238Pu

Cm
244
10h

242
Am
242m

Am
243

Pu
242

Pu
243

4.9h

26m

244
Am
244m

18.1 yr

Difference from Conventional Nuclear Transmutation Project


Conventional Project
FP
n

Objective
Reduction of HLW
(MA : Waste)

MA
FP

PPP
n

Protected Pu
MA

Pu238

Nuclear Non-Proliferation
(Fertile Material )
High Burn-up

238

Pu239

(Burnable Poison)
Effective Use of HLW
(MA : Treasure)

Advanced Concept of Fuel Cycle


Power
Uranium

Current

Fuel Storage

LWR
U,Pu
MA,U,Pu

Power
Accelerator

Fuel
Fabrication

Reprocessing

Power

MA,U,Pu

Advanced
reactor

Fusion
Uranium

FP

Fuel Storage
(Storage of Protected Pu)
50 -100yr

Disposal

Advanced Cycle Technologies (U-Pu-MA) C-Project


Denatured Pu Production (DPP)
B-Project

Protected Pu Production (PPP)

A-Project
FBR
Blanket
PPP

B-2

U-MA
A-2

A-3

U-Pu-MA

A-1

U-Np

U-Pu-Np

(U-236)

B-1

IMF
Th

ADS
D-Project

External Neutron

Fusion

(Sub-critical)

(14MeV)
E-Project

PPPU Int. Advisory Committee

Example I:

General Effect of MA Addition into


UOX Fuels

Effect of MA Addition on 238Pu Buildup


MA vector in
PWR spent fuel
(year cooling)

1.5

UOX(5%235U)

Oxide fraction

UOX(5%235U)+1%MA

1.4

UOX(5%235U)+2%MA
Np

FP

Np

1.3

X%

MA
Pu

Am

28.3%

Am

Cm

6.2%

Cm

k infinity

1.1

1.0

(100 X)%

0.9

(5% or 20%235U)

100
239

15
U)

14

Pu

60

13

40

12

20

240

Pu

241

11
Pu

0
0

10

20

30

242

Pu

40

238

Pu 10

50

10

20
30
Burnup (GWd/tHM)

100
UOX(5%

235

40

50

14
U)+1%MA

80
239

13
Pu

60
12
40
238

20

11

Pu
240

Pu

241

Pu

242

0
0

Burnup (GWd/tHM)
Note: Infinite lattice cell calculation with SCALE4.4 implementing
implementing PWR geometry & power rating

10

20

30

40

Burnup (GWd/tHM)

Pu

10
50

Pu Bare Critical Mass (kg)

80

235

Pu Bare Critical Mass (kg)

UOX(5%

Pu Fraction (%)

1.2

Pu Fraction (%)

5% U-235
PWR
50
GWd/tHM

65.5%

Effect of MA Addition on 238Pu Buildup (contd.)


100

14
UOX(20%

80
UOX(20%235U)
UOX(20%235U)+5%MA

1.4

239

Fraction (%)

1.5

k infinity

U)

UOX(20%235U)+10%MA

1.3

UOX(20%235U)+30%MA

1.2
1.1

13

Pu

60
12
40
240

20

Pu

241

238

Pu

Pu

242

Pu

11

Bare Critical Mass (kg)

1.6

235

1
0

0.9

0.8

30

60

90

120

10
150

Burnup (GWd/tHM)

0.7
0

100

200

300

400

500

235

U)+30%MA

Fraction (%)

80

13
238

60

Pu

12
40
239

20

11

Pu
240

Pu

241

Pu

242

0
0

100

200

300

400

Burnup (GWd/tHM)
Note: Infinite lattice cell calculation with SCALE4.4 implementing
implementing PWR geometry & power rating

Pu

10
500

Pu Bare Critical Mass(kg)

UOX(20%

Burnup (GWd/tHM)

A subcritical core with sub-criticality as low as


k=0.7 can still maintain the Energy Break-evenpoint of an ADS with Lead target incinerated by
1.6 GeV protons (50 neutrons are produced per
one incident proton)

14

100

Example II:

Np-Doped UOX

Effect of Np Addition on 238Pu Buildup


100

Pu Fraction (%)

80

1.5
1.4

UOX(5%235U)

1.3

15
U)

14

Pu

60

13

40

12

20

240

UOX(5%235U)+3%Np

Pu

241

11
Pu

242

1.2

10

20

1.1

30

Pu

238

Pu 10

40

50

Burnup (GWd/tHM)
100

235

14
U)+1%Np

80

0.9
0

10

20

30

Burnup (GWd/tHM)

40

50

13
239

60

Pu

12
40
238

Pu

11

20
240

Pu

241

Pu

242

0
0

10

20

30

40

Burnup (GWd/tHM)

Pu

10
50

Pu Bare Critical Mass (kg)

UOX(5%

Fraction (%)

k infinity

UOX(5%235U)+1%Np

239

235

Pu Bare Critical Mass (kg)

UOX(5%

Example III:

(Am-Cm)-doped UOX Fuel Intended


for High Burnup Core

Burnup-dependent Reactivity Swing of


(Am-Cm)-doped UOX Fuels*
Am-Cm vector in
PWR spent fuel
(year cooling)

1.6
UOX(5%235 U)
Oxide fraction (wt %)

UOX(20%235 U)

1.5
FP
MA

33.6%

Am
241

242m

0.3%

242m

Am
243

48.2%

Am
243

Cm

17.9%

Cm

Pu

UOX(20%

U)+1%(Am -Cm )

235

UOX(20% U)+2%(Am -Cm )


UOX(20%235 U)+3%(Am -Cm )

1.4
X

k infinity

5% U-235
PWR
50
GWd/tHM

Am
241

235

UOX(20%235 U)+5%(Am -Cm )

1.3

UOX(20%235 U)+8%(Am -Cm )

1.2
1.1

100 X

(20%235U)

0.9
0

20

40

60

80

100

120

140

Burnup (GWd/tHM)
3% (Am(Am-Cm) addition is taken as a reference due
to its relatively higher burnup value with
significant reduction in initial criticality
*Infinite lattice cell calculation with SCALE4.4 implementing PWR
PWR geometry & power rating

160

Reactivity Swing Adjustment


0.030
235

Gd-157

1E+5

0.025

B-10

1E+4

Er-167
1E+3
1E+2
1E+1

Capture cross-section of typical LWR


burnable absorbers

1E+0
1E-5

1E-4

1E-3

1E-2

1E-1

1E+0

0.010

BE = 0.35

Introduction of
additional burnable absorbers

BE = 0.30
BE: boron efficiency

1.3

100

1.25

80
1.2
70
60
50
1.1

40
10

10

106

1.2

103

1.15
1.1

100

1.05
1

97
0

0.5
1
Er-167 Addition (% )

G. Youinou, et al., Plutonium Management and Multirecycling in LWRs Using an Enriched Uranium Support,
International Conference on Future Nuclear Energy System (GLOBAL99), Wyoming, USA, Aug. 29 Sept. 5, 1999.

1.5

Maximum Burnup
(GWd/tHM)

90

1.15

0.1
1
Neutron energy (eV)

110

Maximum Burnup
(GWd/tHM)

Initial k infinity

0.015

0.000
0.01

1.25

1
Lanthanides addition (% )

Boron concentration in PWR#


Typical:
1500 1800 ppm
Maximum:
2500 ppm

BE = 1

1E+1

1.3

0.020

0.005

Energy (eV)

0.1

UOX(5% U)
235
UOX(20% U)
235
UOX(20% U)+3%(Am-Cm)

Initial k infinity

1E+6

Neutron Flux (arbitrary unit)

Capture cross section (b)

1E+7

(Am-Cm)-doped UOX Characteristics


1.6

UOX(20%235U)
UOX(20%235U)+3%(Am-Cm)
UOX(20%235U)+3%(Am-Cm)+1%Lth
UOX(20%235U)+3%(Am-Cm)+1%Lth+1%Er

1.5

25

BOC

EOC

PWR#

15

FTC (pcm/K)

5.2 ~ 1.8

10

Voidage
(pcm/%void)

11

190

negative

MTC
(pcm/K)

25

58

78 ~ + 8

UOX(20%
Pu/Pu (%)

1.4

238

1.3
1.2

1.1

UOX(5%

235

235

U)+(Am-Cm)+Lth+Er

UOX(20%

U)

235

U)
#

U. Kasemeyer, et al., Nuclear Technology, 122, p.52, 1998

1
0

20

40
60
80
Burnup (GWd/tHM)

100

120

20

40

60

80

100

Burnup (GWd/tHM)

Am
2.5%
14

Cm
0.5%

La
1%

Er
1%

1.1
Total Am-Cm

239

Pu

10

0.9

8
0.8
6
238

0.7
Pu
240

Pu

241

Pu

0
0

20

40
60
80
Burnup (GWd/tHM)

0.6
242

Pu

0.5
100

Am-Cm consumption
(normalized to initial load)

12
Pu inventory (kg/tHM)

k infinity

Safety
Coefficients

20

BOC
(0 GWd/t)

EOC
(100 GWd/t)

Am
0.7%

Uranium (20% U-235)


95%

Pu: 238 239 240 241 242


%
20 49 15.5 10.5 5
FP*
6.9%

Uranium (10% U-235)

83.6%

Cm
1.2%

La
4.9%

Np
0.2%

Pu
2.5%

Typical 33 GWd/tHM PWR


Pu: 238 239 240 241 242
% 1.5 54.7 26.2 11.5 6.1

Approach on Fuel Life Extension


50

100
GWd/tHM
Initial P/D: 1.38

P/D: ?
P: fuel pin pitch
D: fuel pin diameter

Initial k infinity

Re-arrangement
of fuel lattice

1.25

45
40
35
30

1.2
1.15
1.1
1.05

1 yr cooling
3 yrs cooling
5 yrs cooling
10 yrs cooling

1
0.95

Restoration of criticality
without fuel reprocessing

Potential Burnup (GWd/tHM)

1.3

Cooling time

0.9
1

1.2

1.4

1.6

UOX (20%235U)+(Am-Cm)+Lth+Er

1.8

2.2

2.4

25
20
15
10

2.6

1 yr cooling
3 yrs cooling
5 yrs cooling
10 yrs cooling

5
0
1

1.2

1.4

1.6

P/D Ratio

1.8
2
P/D Ratio

2.2

1.25

0.04

1.2
k infinity

Neutron Flux (arbitrary unit)

P/D: 2.2
0.03
P/D: 2.0

Enlarged P/D = 2.0

1.15
1.1
1.05

Initial P/D = 1.38

0.02

0.95

PWR (5%
0.01

235

40

50

Safety Coefficients

0 GWd/tHM

46 GWd/tHM

PWR#

P/D: 1.38

0.01

0.1

Neutron energy (eV)

10

FTC (pcm/K)

1.2

1.4

5.2 ~ 1.8

Voidage
(pcm/%void)

-190

212

negative

32

30

78 ~ + 8

1.37

NA

MTC (pcm/K)
Boron efficiency
(pcm/ppm)a

U. Kasemeyer, et al., Nuclear Technology, 122, p.52, 1998


The value is normalized to PWR (5% 235U)

20
30
Burnup (GWd/tH M)

P/D: 1.6

0.00

10

U)

2.4

2.6

Two-Strata Irradiation
of (Am-Cm)-doped UOX(20%235U) Fuel
k-infinity

1.3

st

1 Irradiation
(P/D=1.38)

1.2

nd

Irradiation
(P/D=2.0)

1.1
1
0

25

50

75
Burnup (GWd/tHM)

100

125

0.7%
2.5%

238Pu 239Pu 240Pu 241Pu 242Pu

20

0.5%

49

15.5

10.5

1.2%
0.2%

0.5%
238Pu 239Pu 240Pu 241Pu 242Pu

21.5

30

27

12

9.5

1.1%
0.3%

2.2%

2.5%

1%
1%

150

Am
Cm
Lth

95%

15.5%

11.8%

100 GWd/tHM

46 GWd/tHM

Er
Np

83.6%
235U

238U

20

80

80.4%

Pu
FP

235U

236U

10

238U

87

235U

236U

3.5

238U
90.5

Conclusions

PPP deals with finding the merits of MA, especially in the


enhancement of barrier for nuclear proliferation by
improving inherent properties of plutonium, rather than
their simply elimination or geologic disposal.
General overview reveals that MA doping into UOX fuels
increase the fraction of 238Pu which improves the
proliferation-resistant of plutonium
A partial addition of Am & Cm element from the spent
fuel shows their potential as burnable absorber for high
burnup fuel whilst improving the discharged plutoniums
inherent proliferation-resistant properties as contrasted
to the conventional discharged plutonium

Protected Plutonium Production ( P3)


MA
(Np, Am, Cm)

(Fuel Protection)
MA

Natural
Uranium
238U

Advanced
Nuclear
Energy System

238Pu

Long-Life
Core

239Pu

(Fuel Production)

Protected Pu
Production
239Pu

238Pu

New
Markets

(Long-term Storage for Future Energy Crisis)

A Brief Looks on Mass Balance


Np Recycle from Spent
Fuel of LWR : 100kg
Equilibrium (n-3)th cycle

237Np

Annual
production from Light
Water Reactor in the
World (Generating
Capacity328,950 MWe)
~5,000kg/y

BOC
Charged Np 250kg

Equilibrium n th cycle
BOC
Charged Np 250kg

P3 Innovative
Nuclear
Reactor

P3 Innovative
Nuclear
Reactor

EOC
Discharged Np 150kg

Np Production from Japanese


LWRs~ 880kg/y

EOC
Discharged Np 150kg

Np Recycle from Spent Fuel of P


Innovative Nuclear Reactor : 150kg

P3 Innovative Nuclear Reactor; Equivalent to1000MWePWR


Heavy Metal Inventory75000kg
Np Fraction1wt%
Fuel exchange3 batch

International Science and Technology Forum


On
Protected Pu Utilization
For
Peace and Sustainable Prosperity
International Advisory Committee
(IAEA, USA, EU, Russia, Japan)

Secretary Gr.

(WG-1)
Safeguard

(WG-2)
Safety

(WG-3)
Economy

(WG-4)
Reactor
Technology

(WG-5)
Fuel Cycle
Technology

(WG-6)
Waste
Management

(WG-7)
Nuclear
Data Base

To Discuss International Roadmap


Of
Protected Plutonium Production & Utilization (P3&U)
For
Peace and Sustainable Prosperity