Progress in Nuclear Energy, Vol. 40, No. 3-4. pp. 465-472.

2002
Q 2002 Published by Elsevier Science Ltd
Pergamon Printed in Great Britain
0149-1970/02/$ - see front matter
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PII: SO149-1970(02)00039-2

RECYCLE TRANSMUTATION OF MA AND LLFP

USING BWR FOR SUSTAINING GEOLOGIC DISPOSAL

ASASHI KITAMOTO, M. BUDI SETIAWAN

Research Laboratory for Nuclear Reactors

Tokyo Institute of Technology
2-12-l 0-okayama, Meguro-ku, Tokyo 1.5-8550 Japan
Tel. +81-3-5734-3073, Fax. +81-3-5734-29.59
e-mail: akitamot@nr titech.ac.jp

ABSTRACT

The actinides and fission products produced in nuclear fuels constitute an important part of
the HLW. Therefore, methods for reducing the radiotoxicity of the MA and LLFP in HLW are
presently under investigation. The purposes of this study are to evaluate the effectiveness of MA
transmutation by taking advantage of neutron spectrum hardening due to void fraction along
BWR axial direction; to understand the effectiveness of LLFP transmutation in BWR considering
the large capture cross section of FP in thermal region; and to evaluate the macroscopic
characteristics of longer residential period of LLFP target in the high burnup BWR core.
Conceptual B/T BWR supposed in this study was reactor which the performance comparable to
the current BWR. In MA transmutation case, the calculation was focused on varying the void
fraction of 0 to 40% along the axial direction, which were directly associated to the lower and
upper region of the BWR core. The performance of B/T BWR was evaluated in which four
components of MA (237Np,24’Am, 243Am, and 244Cm) with fixed fraction were blended with UO2
in B/T fuel. While, for LLFP transmutation, the B/T BWR was assumed to have two
homogeneous regions: { 1) the region for UO2 driver fuel (99% of fuel weight), and {2) the
region for LLFP (99Tc and lz91)target capsules (1% of fuel weight), in which metallic Tc rods and
iodine in the form of CeI3 was contained in cylindrical target capsules. The evaluation functions
are { I} fission-to-transmutation ratio, [F/T ratio]M*, and (2) transmutation fraction, TFL~~~.
Results show that the hardening neutron spectrum due to increase of void fraction in B/T BWR
would result a higher [F/T ratio] of MA transmutation performance. Np and Am would be
effectively loaded in the upper region of the core, while Cm could be loaded in any region of the
core. At the EOC of equal or more than 50 GWd/Mg(HM), technetium has a higher
transmutation jiwction compared to iodine. To obtain higher LLFP transmutation fraction, the
residential time in the LLFP targets in the core, should be kept for long time, for instance about
10 to 30 years. For that purpose, it was proposed that the number of B/T BWR system for LLFP
treatment corresponds to the residential time of the LLFP target, i.e. 10 to 30 units.
0 2002 Published by Elsevier Science Ltd.

1. INTRODUCTION

1.1 MA Transmutation in BWR

The actinides produced in nuclear fuel constitute an important part of the long-lived HLW. The
radiotoxicity of MA may not lead to select the direct storage of the spent fuels for very long time due
to LLMA. Therefore, the conceptual studies to reduce the radiotoxicity of those actinides are underway.

465
466 A. Kitamoto and M. B. Setiawan

Various types of reactors and accelerator driven transmutation (ADT) facilities are among the possible
choices for carrying out this extensive endeavor. However, a fully new technology, e.g. fusion reactor,
fast reactor or ADT can only now be assessed in a generic way since their development is still in their
preliminary stage. Adaptation of existing technologies will be more simply approached, such as
reprocessing of high burnup fuel from LWR-MOX, fabrication of actinide targets, minor modification
of current thermal reactors to suit the use of burning and transmutation (B/T) fuels, etc. A promising
scenario studied herein is by ~~smuting the long-lived isotopes of MA in BWR core by taking
advantage of neutron spectrum hardening due to void fraction along the axis.

1.2 LLFP Transmutation in BWR

Fission products (FP) are the most limiting factor in designing the repository facilities due to the
decay heat emission that increases proportionally to the burn up. After some 500 years the major part
of the FP have decayed, except for some Iong lived nuclides, such as Cs-13.5, Tc-99, I-129, Zr-93 etc,
which half-lives are in the order of lo5 to lo6 years. Some of them are relatively mobile in the
geosphere and contribute to the dose to man in the surroundings and even beyond the repository
facilities.
Transmutation of long-lived fission products (LLFP) is a very difficult task, since the capture
cross-section to transmute the radioactive nuclide into a short-lived fission products (SLFP) or stable
nuclides requires large reactor capabilities, Thermal reactors and accelerator driven transmutation
(ADT) facilities are the possible choices for carrying out this very expensive endeavor (BaetslC, 1996).
A completely new technology, e.g. accelerator driven transmutation, however, needs a longer
technological development since its low transmutation rate performance due to the characteristics of
intermittent pulsation of ADT. Thus at the present time evaluations have to be done on the existing
technologies which are more easily approached, such as minor modification of current LWRs to suit
the use of LLFP targets, reprocessing of high burnup fuel from LWR-MOX and fabrication of actinide
or LLFP targets.

1.3 Obiective of the study

The objective of this study is (1) to find the optimized MA loading in the axial direction, taking
into the account of the void change, and (2) to obtain the optimal discharged period of MA in the
burning and tr~smu~tion (B/T) BWR. (3) to understand the effectiveness of LLFP transmutation in
LWR considering the large capture cross section of FPs in thermal region; and (4) to understand the
macroscopic characteristics of longer residential period of LLFP target in the high bumup BWR core.
The summary of MA and LLFP transmutation studies is given in Table 1.

Table 1. Summary of MA and LLFP ~ansmutation studies

MA LLFP

nuclide 241Am,243Am,
237NpF ?c and “‘1
244Cm

in-core Loaded in B/T fuel Loaded in capsule

blended homogeneously targets: metallic Tc
with UOn and Gel,

evaluation fission-to-transmutation tfaffs~ufatio~

function ratio, F/T-ratio fraction, TF
 Recycle transmutationof MA and LLFP 467

2. EVALUATION FUNCTION

The function of (F/T) ratio (introduced by Kitamoto et. al., 1999) was used to evaluate
performance of the reactor for MA transmutation by taking the ratio of total fission rate to total
transmutation rate. If the reactor criticality is kept under the averaged neutron flux, the reactor can be
optimized by this evaluation function. The function, (F/T) ratio, is defined as CiCj {N,or,:&} / C,C,
VI (o,,/ + or,/+ cr& &’ } where N = nuclide number density, of = fission cross section, CJ,= capture
cross section, (3~~= n,2n cross section, i = MA nuclide and j = neutron energy group. The evaluation
function of transmutation fraction, TF, is defined by the ratio of the transmuted LLFP to the initial
LLFP loading, calculated at the various bum-up times. [TF] = {C(NLLI;P)~~~~ / C(NLLFP)init}x100%
where NLLFP= LLFP number density which is obtained from the calculation using the following
equation: N, = F,p NA/ib& where N = atomic number density of nuclide-i [atom/cm3], pF= fuel density
[g/cm3], F, = weight fraction of nuclide-i in fuel [-I, & = average molecular weight of fuel [g/gmol],
and NA = Avogadro’s number [6.024 x1023mol“].

3. MA AND LLFP SELECTION

In this study, MA selected was four components: Np-237, Am-241, Am-243 and Cm-244.
U&Pu, separated with MA (U&Pu unrecovered in a reprocessing plant) and UO2 blended with MA,
are considered as fuel, though they are reacted with neutron in B/T fuel, and UO2 and its transmuted
component to TRU in B/T fuel, is considered as fuel. In case of short-lived MA nuclide, there is no
influence on. the inventory reduction caused by the short-lived MA nuclide, because R&P process was
assumed not to having ability to separate the isotopic component. In case of the unrecovered
plutonium from ‘the reprocessing process were not included in the B/T fuel, since their influences in
the fission rate were quite dominant, so that the B/T reactor performance could not be clearly shown.
LLFPs to be treated in the BWR are selected using two-level selection, as following.
Selection-I comprises three criteria, which are (1) the natural decay of the radionuclides should
be more than 100 years, in the view that the deep-geological waste repository system would prevent
the release of the radionuclides for 100 years, (2) the fission yield of RI (radio isotope) should be more
than 1Om3, and (3) RI are selected according to their hazard index.
Based in selection-l criteria, six radioisotopes were selected. They are ordered according to the
magnitude of Hazard Index as following: I-129, Tc-99, Zr-93, Sn-126, Cs-135, Pd-107. Up to this
level, the following FPs is to be considered: iodine (I-129) technetium (Tc-99) and cesium (Cs-135).
Selection-2 comprises four criteria as following: (1) the decay acceleration, which is defined as
the ratio of total decay rate under neutronflux 4 to natural decay rate should be greater than 10, (2)
the nuclides should have a high transmutation fraction in one fuel life, (3) the partitioning of the
radionuclides from spent-fuel can be done by chemical separation; not isotopic separation, and (4) for
the technological and economical reason for no further separation process, their isotopic composition
have to be simple.
From these selections, two nuclides were chosen as candidates to be transmuted, which are:
iodine and technetium. Technetium and iodine are among the most important nuclides that dominate
the /3 activity of spent fuel after a hundred thousand years. Since their solubility in ground water is
high, Tc-99 and I-129 are easily mitigated to the environment once they are released from the
geological waste repository. To reduce the dose risks, Tc-99 and I-129 should be partitioned from the
spent fuel and treated separately.

4. CALCULATION METHOD

The performance of B/T (burning and/or transmutation) BWR was estimated by the conceptual
BWR with the specifications comparable to the current 1,000 MWe-BWR, including the size of the
468 A. Kitamoto and A4. B. Setiawan

core and fuel cell geometry. The core was assumed to be built with two homogeneous regions: (1) the
region for standard UOz fuel (90% of core volume) with standard enriched U-235, and (2) the region
for B/T fuel (10% of core volume) in which four components of MA (‘37Np, 241Am, 243Am, and 244Cm)
with fixed fraction were blended with UOZ in the oxide form. Calculations were done for several void
fraction conditions of 0, 10, 20, 30 and 40%. The void fractions of 0 to 40% were directly associated
to the lower and upper regions of the BWR core.
Conceptual BWR-type tr~smutation reactor only for LLFP ~ansmutation proposed in this
study was supposed as reactor which the performance comparable to the current 1000 MWe BWR.
The sizes of the core and the fuel cell geometry of conceptual transmutation reactor was kept to the
same as current ones. The core of transmutation reactor was assumed to have two homogeneous
regions: (1) the region for UOz driver fuel (99% of fuel weight) with 4.5% of enriched U-235, and (2)
the region for LLFP target capsules (1% of fuel weight), in which metallic Tc rods and iodine in the
form of Ce13was contained in cylindrical target capsules (Babelot, et al., 1995).
The numericai caiculations were done by using JAERl-SRAC95 code (Okumura K., 1996). The
mass balance of nuclides in the core was calculated by the cell depletion calculation for the
homogeneous core model. The time needed to attain the equilibrium state of the core can be estimated
by making a series of cell depletion calculations starting with a typical cell composition.
The reactivity swing for different MA or LLFP loading in the B/T fuel or target capsules was
examined in order to obtain a maximum loading of MA fraction which yields a safe and maintainable
reactivity swing over the fuel life time. The criterion for determining a maximum acceptable content
of MA or LLFP loading was settled from the aspect of reactor operability.

5. RESULTS AND DISCUSSION

The hardening neutron energy due to the void fraction in BWR would result in a higher
transmutation fraction of MA transmutation performance. Calculation results show that (F/T) ratio of
total MA increased for the higher void fraction (Fig.1). It is also observed for individual specified
nuclide, i.e. 237Np, **‘Am, 243Am, and 244Cm, that in case of 237Np, the higher void fraction of 40%
would effectively increase its (F/T) ratio. Am increased its {F/T) ratio with hardening spectrum which
correspond to 20% void fraction. In case (F/T) ratio of Cm, however, there was no observable
difference in all void fractions, as concluded in Table 2.
MA nuclei are not directly fissioned instead they change to fissionable nuclide by neutron capture
before fissioned. Figure 2a shows the main reactions of Np-237. As shown in this figure, Np-237
changes to fissionable Pu-239 by neutron capture and then fission. Figure 2b shows the main BIT
reaction of Am-24 1 and Am-243 in the core. As can be observed in Fig. 2b, Am-24 1 has three cases of
termination. Firstly, Am-24 1 changes to fissionable Am-242 by neutron capture; the main part proceed
with cr.-decay to fissionable Pu-239, and some parts go to Cm-243 by neutron capture and fission due
to very small capture cross section ofCm-242. Main B/T reaction of Am-243 is terminated by fission
of Cm-245.

5.2 LLFP Transmutation

Calculation results of first loading and remained of Tc-99 and I-129 in the target of both BWR
and PWR are shown in Fig. 3. At the BOC of both reactors the initial mass of Tc-99 and I-129 were
1200 kg respectively, which is equivalent to 1% of the 120 Mg fuel inventory in the core (Babelot, et
al., 1995).
5.2.1 Technetium. At the EOC which is equal to 50 GWd~g(HM), technetium mass decreased quite
rapidly compared to iodine. It is also shown that Tc-99 remained in BWR was lower than those in
PWR. In suggests that more technetium is transmuted in BWR core. The production of technetium in
the driver fuel of both reactors was comparably similar, in which production in BWR is slightly higher.
The amount of technetium remained in target capsules and technetium produced in driver fuel was
differed in the order of lo2 kg. These conditions were thought to be suitable to the purpose of
transmutation reactor for technetium transmutation, in which the productions of Tc-99 by fission in the
 Recycle transmutation of MA and LLFP 469

U02 driver fuel decreases the net ~nsmutation rate and reduces the necessities of large technetium
loadings.
5.2.2 Iodine. At the EOC, the remained of I-129 in target capsules of both BWR and PWR were
comparably the same. As in the case of technetium, the production of iodine in driver fuel of both
reactors was comparably similar. Production of iodine in the driver fuel is much lower than those of
technetium.
As a results the overall Tc-99 and I-129 remained in the target of BWR core was much lower
compared those in PWR. In the other words, more iodine is transmuted in the BWR core.
5.2.3 TF evaluation function. The evaluation of transmutationfraction, TF, was calculated at the EOC
of 50 GWd/Mg, as provided in Fig. 4. The [TF] value for BWR (with 40% void fraction) is higher than
that of PWR, which are 13% and 1O%, respectively.

30%

25%

20%
3
G
I 15%
t
B
10%

5%

#
0%
0 10000 20000 30000
Bum up (~Wd/Mg)

Fig. 1 FIT ratio of MA in B/T BWR (MA=5%, void 0%-40%)

Table 2. Effective loading region for B/T fuel

20 40
~5 Upper
0 0 @
0 @ @
0 @ @
0 0 0
Remarks:
@: the effective region for B/l treatment
(activated by the void fraction)
0: the normal region for B/T treatment
470 A. Kitamoto and M. B. Setiawan

94Pu Fig 2a. Main B/T reactions of Am-241, terminated

by fissions of Am-242, Pu-239 and Cm-243. And
those of Am-243 terminated by fission of Cm-245

“Np
Np-237

237 238 239

Mass Number

Fig 2b. Main B/T reactions of Np-237, terminated

by fission of Pu-239

I
238 239 240 241 242 243 244 245

Mass Number

1.4

-Tc-99 rem in BWR

------.Tc-99 rem in PWR

0.4

l-129 rem in BWR ~

0.2 1-129 rem in PWR
~_

0 ’
0 10000 20000 30000 40000 50000
Burn-up (MWd/MgHM)

Fig. 3 Mass of Tc-99 or I-129 in the BWR or PWR with respect to burn
up. The initial mass of Tc and I are equal to 45 GWd/MgHM discharged
fuel from each 24 units of 1000 MWe LWR.
 Recycle transmutation of MA and LLFP 471

6. CONCEPT OF TRANSMUTATION SYSTEM FOR LLFP IN LWR

From the calculation and evaluation results of technetium and iodine in light water reactors, a
concept of transmutation system for LLFP in LWR is proposed. In the LLFP transmutation treatment,
the residential time should be kept for long time. for instance about 10 to 30 years, for obtaining
higher transmutation fraction. Consequently, for maintaining the constant treatment for such a long
time, it is suggested that the number of reactor units should be proportional to the time of
transmutation treatment. For straightforwardness purpose, it is proposed that the number of
multi-recycle transmutation reactor system for LLFP treatment simply corresponds to the irradiation
time of the LLFP target, i.e. lo-30 units.
The upper limit of technetium and iodine loading in the core, with satisfy the critical condition
was 1 w% of normal fuel, i.e. 1.2 Mg/unit transmutation BWR. As mentioned before this amount is
equivalent to mass of Tc-99 produced by 57 unit of 45 GWd/MgHM LWR or to mass of I-129
produced by 237 unit of 45 GWd/MgHM LWR.
In case of 50 units of LWR. a brief concept for LLFP transmutation could be drawn as follows
(Table 2). For maintaining a higher transmutation fraction, the irradiation time of technetium and
iodine in the reactor is settled on 10 years and 30 years, respectively. The total inventory for one
irradiation time would be similar to 50 LWRxlO = 500 LWR equivalent and 50 LWRx30 = 1500
LWR equivalent. The number of transmutation BWR system needed for transmutation is about (500
LWR equiv./57 LWR) = 9 units of transmutation BWR for technetium and about (1500 LWR
equiv./237 LWR) = 6 units of transmutation BWR for iodine. As a whole, approximately 15 units of
transmutation BWR are required for transmuting technetium and iodine discharged from 50 units
LWR. In conclusion, it is not so easy to transmute technetium and iodine produced in 50 units LWR,
since it would require large num,ber of transmutation BWR.

30%

-Tc-99 BWR
;- - - Tc-99 PWR

20000 30000
Burn-up (MWd/MgHM)

Fig. 4 Transmutation Fraction (TF) of Tc-99 and I-129

in BWR and PWR (1 %w loading)
412 A. Kitamoto and M. B. Seriawan

Table 2. The number of transmutation BWR for 99Tc and ‘191, produced by 50 units 1GWe LWR,
based on once through and multi-recycle.

Irradiation Total mass produced Sum of NR, for Sum of Nk for

TF(-) Nuclide Time (y) by 50 unit LWR NR, 99Tc & “‘1 NRC 99Tc & ‘?

99Tc 10 10,525 8.8 21.9

0.4 15.1 37.7

129I 30 7,590 6.3 15.8

99Tc 12.5 13.156 11.0 21.9

0.5
129 18.9 37.7
37.5 9,487 7.9 15.8
Notes:
NFG = Number of BWR in once through
NRC = Number of BWR in multi-recycle
TF = Transmutation Fraction

7. CONCLUSIONS

(1) The hardening neutron energy due to the void fraction in B/T BWR would result in a higher
(F/T) ratio of MA transmutation performance. Np and Am would be effectively loaded into the
top region of the core, while Cm could be loaded in any region of the core. The top region of the
core is optimized for the position of loading in B/T fuel.
(2) In case of technetium, BWR is able to transmute more effectively than those of PWR. However,
in case of iodine, the significant difference of its remained in target capsule of both reactors was
not observed.
(3) BWR has a comparably higher transmutation fraction [TF] value for LLFP transmutation
compared to PWR.
(4) To obtain higher transmutation fraction, the residential time in the LLFP transmutation treatment,
should be kept for long time, for instance some 10 - 30 years. The number of transmutation
reactor for LLFP treatment simply corresponds to the residential time of the LLFP target
capsules, i.e. 10 - 30 units.

References
Babelot J.F (1995) Development of Fuels for Transmutation in the frame of EFFTRA European
Collaboration. International Conference on Evaluation of Emerging Nuclear Fuel Cycle Systems
(GLOBAL 199.5), pp 524-529. Versailles, 11-14 September
BaetslB L.H. (1996), A Comparative Systems-Analysis Approach on Fuel Cycles with Partitioning and
Transmutation. The Fourth International Information Exchange Meeting on Actinide and Fission
Product Partitioning and Transmutation. p. 45. Mito City, Japan, 11-13 September
Kitamoto A., Setiawan M.B., Taniguchi A. (1999), Proposal of New Evaluation Function to Indicate
the Performance of B/T Reactor. 1999 Annual Meeting of the Atomic Energy Society of Japan., Fl ,
p. 299
Okumura K., et al. (1996), SRAC9.5 General Purpose Neutronic Code System, Japan Atomic Energy
Research Institute JAERI Data/Code 96-015