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Role of Minor Actinides For Protected Plutonium Production PDF
Role of Minor Actinides For Protected Plutonium Production PDF
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.
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%
Uranium
Fuel Storage
LWR
U,Pu
U,Pu
Fuel
Fabrication
MA, FP
Reprocessing
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
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
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)
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
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
Example I:
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
80
235
UOX(5%
Pu Fraction (%)
1.2
Pu Fraction (%)
5% U-235
PWR
50
GWd/tHM
65.5%
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
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
UOX(20%
Burnup (GWd/tHM)
14
100
Example II:
Np-Doped UOX
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
UOX(5%
Fraction (%)
k infinity
UOX(5%235U)+1%Np
239
235
UOX(5%
Example III:
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
1.4
X
k infinity
5% U-235
PWR
50
GWd/tHM
Am
241
235
1.3
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
Gd-157
1E+5
0.025
B-10
1E+4
Er-167
1E+3
1E+2
1E+1
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 (% )
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
1E+7
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)
#
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%
83.6%
Cm
1.2%
La
4.9%
Np
0.2%
Pu
2.5%
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
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
P/D: 2.2
0.03
P/D: 2.0
1.15
1.1
1.05
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
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
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%
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
(Fuel Protection)
MA
Natural
Uranium
238U
Advanced
Nuclear
Energy System
238Pu
Long-Life
Core
239Pu
(Fuel Production)
Protected Pu
Production
239Pu
238Pu
New
Markets
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
EOC
Discharged Np 150kg
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