Progress in Nuclear Energy, Vol. 29 (Supplement), pp.

335-341, 1995
1995 Elsevier Science Ltd
Pergamon Printed in Great Britain
0149-1970/95 $29.00

0149-1970(95)00061-5

TRANSMUTATION OF FISSION PRODUCTS WITH THE USE OF AN

ACCELERATOR

T. Kase, H. Harada and T. Takahashi

Power Reactorand NuclearFuel DevelopmentCorporation,Tokai,

Ibaraki-ken319-11, Japan

ABSTRACT

The three transmutation methods with the use of an accelerator, the proton method, the spallation neutron
method and the gCF method, are employed for the transmutation of long-lived nuclides in high level
radioactive wastes. The transmutation energies and the effective half-lives of 99Tc and 137Cs for these
transmutation methods are calculated by the Monte Carlo simulation codes for particle transport. The
transmutation energies of the proton method are larger than those of the spallation neutron method and the
gCF method under the condition of the same effective half life. The proton method is difficult to meet
energy balance criterion. On the other hand, the spallation neutron method and the ~tCF method have
possibility to meet the energy balance criterion.

KEYWORDS

Transmutation; radioactive waste; fission products; accelerator; muon catalyzed fusion; neutron capture;
spallation.

INTRODUCTION

Several transmutation approaches for the long-lived nuclides in high level radioactive wastes (HLW), which
are generated in spent nuclear fuel reprocessing plants, have been studied to establish the transmutation
method (Harada et al., 1993, Kase et al., 1991, Kase et al., 1993, Kase et aI., 1994, Krenciglowa et al.,
1981, Takahashi et al., 1980, Takahashi, 1989, Wootan et al., 1992). The transmutation approach means to
transmute the long-lived nuclides to stable or short-lived nuclides by nuclear reaction mainly using an
accelerator or a fission reactor. The nuclide 99Tc is a very long-lived fission product (Tl~=2x 105 year) and

335
336 T. Kase et al.

its radioactivity is one of the main components in HLW after the cooling time of 1000 years. On the other
hand, the nuclide 137Cs (T1/2=30.0 year) is one of the main components of radioactivities in HLW before
the cooling time of 1000 years.

This paper shows comparison of the three transmutation methods by accelerator in terms of the
transmutation energies and the effective half-lives of both 99Tc and 137Cs. These transmutation methods are
followings:
(a) transmutation through spallation reaction by high energy proton (proton method) (Kase et al., 1993,
Kase et al., 1994),
(b) transmutation through spallation-induced neutron reaction, mostly (n,),) reaction, by use of secondary
neutrons from high energy proton-induced spallation reaction (spallation neutron method) (Kase et al.,
1993, Kase et al., 1994), and
(c) transmutation through (n,2n) or (n,y) reaction by use of neutrons generated by muon catalyzed fusion
(~CF method) (Kase et al., 1991, Kase et al., 1994).

EVALUATION METHOD

The major factors to evaluate transmutation method are the transmutation rate (effective half-life) and the
transmutation energy. The average transmutation rate in a target region, ~,tr, is expressed by

)~t~(r)=I (r(E)0(E,r)dE

- Iv )~(r)dr
)~tr-
Iv dr (1)

where
r = position of waste nuclide in target system,
E = particle energy,
V = target volume,
orE) = cross section of relevant nuclear reaction,
0(E,r) = particle flux.

A relation between the transmutation rate and the number of target nuclide can lead to the concept of an
effective half-life to describe the target nuclide reduction. The effective half-life, Teff is defined as
following,
 Transmutation of fission products 337

Weft ~ -
0.693
- m

X,nat + X,tr , (2)

where
~nat = decay constant of target nuclide.

The transmutation energy, Err is defined as a primary beam energy used for transmutation per nuclide.
This factor is written by,

Epart
E n - P(V), (3)

where
Epart = particle energy,
P(V) = probability of reaction in a transmutation region with the volume of V (reactions/incident particle).

These factors are calculated by Monte Carlo simulation codes. The calculation condition and used calculation
codes for the evaluation of these transmutation methods are summarized in Table 1.

Table 1. Calculation condition

Transmutation method Nuclide Particle Energy Current Code

[MeV] [mA]
Proton method 99Tc p 800 562.5 NMTC
Proton method 137Cs p 500 900 NMTC
Spallation neutron method 99Tc p 1500 300 NMTC+MCNP
Spallation neutron method 137Cs p 1500 300 NMTC+MCNP
p.CF method 99Tc d 4000 25 MCNP
txCF method 137Cs d 4000 25 MCNP

The NMTC/JAERI code (Nakahara et al., 1982) and the MCNP code (Briesmeister, 1986) were used in this
study. Transport of proton and neutron with energy above 15 MeV was calculated by the NMTC/JAERI
code. The MCNP code was used in calculations of neutron transports and reactions in low energy region,
<15 MeV.

The btCF method uses (n,2n) or (n,y) reaction for transmutation. In the case of 137Cs, the (n,2n) reaction is
used for transmutation. The cross section of (n,2n) reaction (1.2 b) is larger than that of (n,y) reaction (0.25
b). In the case of 99Tc, the thermal neutron, which is moderated by D20, is used for transmutation, since
338 T. Kase et al.

(n,7) reaction cross section of 99Tc is very large (20 b). The (n,2n) reaction can not use for transmutation.
The 98Tc, which is produced by (n,2n) reaction, has a long half-life (4.2× 106 year).

RESULTS AND DISCUSSION

The effective half-lives as a function of target volume are shown in Fig. 1. These figures indicate that the
effective half-life increases with increasing target volume. This is because the increase of the target volume
is greater than that of the number of transmutation reactions. Effective half-life depends on beam current. If
high current accelerator is developed, the effective half-life can become shorter.

----~- - Proton
- - ,=- - Spalration neutron ___~'.. ~rgt~oo
• p. CF - - * - -Spallation neutron
tO 10 '''"1 ' ' '''"'1 '# • ' .... I

8
...... , ........
:// , / . . . . i...,

6
1/ / I'
,//
a~

t3
4 //// j' .~ 4

Tu 2 ~ i i ~
W 2

0
...... i , , , , , , , , i . . . . ,,,,i ,-~7,,,m~l" , . , ..... i ........ i
0.01 0.1 0.01 0.1
T a r g e t v o l u m e [m :}] Target volume [m 3]

(a) 99Tc (b) 137Cs

Fig. 1. Effective half-life as a function of target volume.

The transmutation energies as a function of target volume are shown in Fig. 2. As shown in Fig. 2, the
transmutation energies of the proton method are large, since protons may give energy to the electrons of the
target material other than to the nuclear reactions. It is difficult to use effectively the secondary reactions for
the transmutation, since the target volume is restricted to obtain short effective half-life. If longer effective
half-life is adopted, transmutation energy is lower.

On the other hand, nuclear reaction with neutron has the advantage in the point of view of the transmutation
energy. The transmutation energies of the spallation neutron method and the IxCF method are lower than
those of the proton method.
 Transmutation of fission products 339

• ~.t CF
.--..o- - Proton - - Protorl
e.- - Spallation neutron
m ,-. =Spallation neutron

1400 1400 . ' ..... = . . . . . . . . I . . . . . . . . I

. . . . . . "1 • ' ..... '1

N"
1200 1200 ~

looo

8o0
g
600
•~

E
600

40O
"\. ~5
400

I-
2OO F- 200
0 0 i,.,,I . . . . . . . . I . . . . . . . . I

0.01 0.1 0.01 0.1

Target volume [m~] T a r g e t v o l u m e [m 3]

(a) 99Tc (b) 137Cs

Fig. 2. Transmutation energy as a function of target volume.

The comparison between the transmutations of 99Tc and those of 137Cs is tabulated in Table 2. According to
these calculations, the transmutation energies of 99Tc are about 10 times lower than those of 137Cs in the
spallation neutron method and the ~tCF method, since reaction cross section of 99Tc is much larger than
those of 137Cs. Thermal neutron capture cross section and (n,2n) cross section of 137Cs are 0.25 b and 1.2
b, respectively. On the other hand, thermal neutron capture cross section of 99Tc is 20 b. The spallation
neutron method and the t.tCF method for 99Tc have advantage of those of 137Cs from the point of view of
transmutation energy. The transmutation of other long-lived fission products with large thermal neutron
cross section, for example 1291, 135Cs, are also expected to have the same advantage.

The energy released per fission event is 200 MeV and the fission yields of 99Tc or 137Cs are 6%,
respectively. The energy of 3300 MeV is obtained by fission of uranium or plutonium, when one 99Tc or
137Cs is generated in a fission reactor. It is assumed that the efficiency for thermal to electrical
conversion is 33% and efficiency for particle beam acceleration is 50%. The upper limit of particle beam
energy, which can be used for the transmutation of 99Tc or 137Cs, is calculated to be 550 MeV by the
following equation,

(200/0.06)×0.3 3x0.5=550 [MeV].

The transmutation energy should be smaller than at most 550 MeV to realize energy balance, even if the
transmutation of only a kind of nuclide (99Tc or 137Cs) is considered. In Table 2, the calculated
transmutation energies reveal that it is possible for the spallation neutron method and the ~tCF method of
99Tc to meet the energy balance criterion for the effective half-life of 1-5 years.
340 T. Kase et al.

Table 2. Comparison of transmutation of 99Tc and 137Cs

Transmutation method Nuclide Transmutation Effective half-life

energy [Year]
[MeV]
99Tc 1400 1.0
99Tc 330 2.0
~ o m n method 99Tc 320 5.0
137Cs 600 1.0
137Cs 570 2.0
137Cs 500 5.0
99Tc 43 1.0
99Tc 35 2.0
Spallation neutron 99Tc 29 5.0
method 137Cs - 1.0
137Cs 510 2.0
137Cs 60 5.0
99Tc 54 1.0
99Tc 40 2.0
gCF method 99Tc 25 5.0
137Cs 400 1.0
137Cs 195 2.0
137Cs 120 5.0

The upper limit of particle beam energy decreases when the transmutation of several kinds of fission
products is considered. For example, it is assumed that 90Sr, 99Tc, 129I and 137Cs are the objective nuclides
of the transmutation. The fission yields of 9°Sr and 129I are 5.9% and 0.9%, respectively. The total yield of
these four nuclides is 18.8%. The upper limit of particle beam for four nuclides is calculated to be about 175
MeV. In this case, the spallation neutron method and the gCF method for 99Tc can also meet the energy
balance criterion as shown in Table 2. If longer effective half-life is adopted, the transmutation energy can
be reduced and the spallation neutron method and the gCF method for 137Cs can meet the energy balance
criterion.

In order to establish the above transmutation methods, the following R&D are also necessary:
(a) development of structure material in an intense neutron irradiation,
(b) study of heat removal from the target systems, and
(c) development of high power accelerator.
 Transmutationof fissionproducts 341

CONCLUSION

The three transmutation methods using accelerator were evaluated by computer simulation. Three
dimensions Monte Carlo codes were used to calculated the effective half-life (transmutation rate) and the
transmutation energy for the practical target geometries. Three transmutation methods were compared with
each other in terms of transmutation energies and effective half-lives for 99Tc and 137Cs.

The short effective haft-lives of 99Tc of 1-5 years could be obtained with the spaUation neutron method and
the ~tCF method, considering the low transmutation energy of 55-25 MeV. In the case of 137Cs, the
transmutation energies of both methods were 60-120 MeV for the effective half-life of 5 years. These both
methods have the possibility to meet the energy balance criterion. On the other hand, the transmutation
energies of the proton method were so large because of energy loss of ionization.

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