Annals of Nuclear Energy 38 (2011) 1347–1350

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Annals of Nuclear Energy

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99
Transmutation of the radiotoxic isotope Tc under irradiation in the BR2 high
flux reactor
Naïma Amrani ⇑, Ahmed Boucenna
DAC Laboratory, Physics Department, Faculty of Sciences, Ferhat ABBAS University, Sétif 19000, Algeria

a r t i c l e i n f o a b s t r a c t

Article history: In this study we present data on the transmutation of the long lived fission product Technetium to the
Received 21 July 2010 stable Ruthenium under irradiation in the high flux reactor BR2. The Technetium transmutation rate
Received in revised form 22 January 2011 and the evolution of Ruthenium mass under irradiation were numerically simulated using ChainSolver
Accepted 31 January 2011
2.34 code.
Available online 19 February 2011
Ó 2011 Elsevier Ltd. All rights reserved.

Keywords:
Technetium
Transmutation
ChainSolver 2.34

1. Introduction reaction used for transmutation of radiotoxic isotope 99Tc in nucle-

Technetium-99 (99Tc) is one of the most important long lived
fission products present in the spent nuclear fuel. The beta radio
toxicity of 99Tc is far below the alpha radio toxicity of minor actin-
ides, but its high mobility and very long life (half life of
2  105 years) increase significantly the very long-term risk during
storage (Gunsing et al., 2000). Technetium-99 is produced as a re-
sult of nuclear transformations in nuclear reactors with a large
cumulative yield of 6.11% from the thermal neutron fission of
235
U (Matsumoto et al., 2003). Neutron irradiation of 99Tc yields
valuable Ru which is promising for practical applications. This plat-
inoid could be obtained in amounts satisfying the modern de-
mands by the transmutation of 99Tc. But the development of
Technetium transmutation into Ruthenium is in its early days.
The Technetium transmutation rate in reactor is lower than the de-
sired one that is required for commercial process (Tarasov et al.,
2007).
The Objective of this study is the estimation of Technetium
transmutation rate and Ruthenium mass obtained from Techne-
tium targets irradiated in high flux reactor BR2 considering its
large capture cross section in thermal and epithermal region.
2. Transmutation process
The scheme of Technetium transmutation and Ruthenium for-
mation under neutron irradiation is presented in Fig. 1. The basic
⇑ Corresponding author.
E-mail address: naima2073@yahoo.fr (N. Amrani).
ar reactor is the neutron absorption (Gudowski, 2000).
T 1=2 ¼15:8 s
99
Tc ðn; cÞ100 Tc ! 100
Ru
After capturing the neutron, 99Tc becomes 100Tc, usually in excited
state which decays very fast typically in a few ns into the 100Tc
ground state, by emitting the so called prompt photons. The 100Tc
with half life of 15.8 s decays by b transition into 100Ru, about
7% of the cases into the excited state of this isotope. This 100Ru ex-
cited states decays very fast, in less than 1 ns into the 100Ru ground
state, emitting the so-called delayed photons (Gonzalez, 1998).
From Fig. 2 it can be seen that 99Tc has a weak thermal cross
section but a very large and strong resonance absorption in the epi-
thermal energy range.
3. Description of BR2 high flux reactor
The BR2 reactor is a 100 MWth high-flux ‘materials testing reac-
tor’ witch first became operational in 1963 and has been refur-
bished in 1995–1997 after more than 30 years utilization to
provide a life time extension of more than 20 years (Ponsard
et al., 2003). This reactor is operated by the Belgian Nuclear Re-
search Center in the framework of programs concerning the devel-
opment of structural materials and nuclear fuels for fission–fusion
reactor. The availability of high thermal neutron fluxes up to
1015 n cm2 s1 allows an important opportunity for routine pro-
duction of radioisotopes for medical and industrial applications.
Currently, a standard irradiation cycle consists of 3–4 weeks oper-
ation at an operating power between 50 and 70 MWth. The present
operating regime consists of five irradiation cycles per year. The

0306-4549/$ - see front matter Ó 2011 Elsevier Ltd. All rights reserved.
doi:10.1016/j.anucene.2011.01.035
1348 N. Amrani, A. Boucenna / Annals of Nuclear Energy 38 (2011) 1347–1350

99
Fig. 1. Reaction path of Tc under neutron irradiation.

2–20 eV and its resonance integral is much higher than the thermal
cross section (Harada et al.,1995).
The Technetium transmutation rates in the central irradiation
Cross section (barns)

position H1 is evaluated with ChainSolver 2.34 code used for

99
Fig. 2. The Tc (n,c) Tc cross section as a function of neutron energy from the
ENDF/B-6 nuclear data file.
transmutation calculations (Romanov, 2003). The ChainSolver
code is intended for fast carrying out transmutation simulation
of samples during irradiation in nuclear reactors. The code calcu-
lates a nuclide density time evolution with burn up, decay and
build-up. The depression of a thermal neutrons flux, resonance
self-shielding of isotopes during an irradiation, and the irradia-
tion schedule (the schedule of the reactor work and rearrange-
ment of an irradiated target in various positions) are taken
into account. These calculations are extremely tedious because
of at each stage of an irradiation the fast, epithermal and ther-
Incident neutrons energy (MeV)
100

BR2 reactor uses 93% 235U enriched uranium as fuel and is moder-
ated by light water and beryllium. The core is composed of beryl-
lium hexagons with central irradiation channels of 200, 84, 50 or
33 mm diameter. The cooling water is pressurized at 12 bars and
has a temperature of 40–45 °C. The aluminum pressure vessel
(Fig. 3) is located in a pool filled with demineralized water (Pon-
sard et al., 2009).

4. Evaluation and calculation method

In this study, the transmutation rate of Technetium transmuta-

tion in BR2 high flux reactor is calculated. The BR2 core design
adopted for this study is given in Fig. 4. This core configuration is
characterized by 32 fuel elements, seven control rods and a regu-
lating rod. These are arranged around the central beryllium plug
H1 in order to provide thermal neutron fluxes up to
1015 n cm2 s1 in its seven irradiation channels. Other irradiation
positions are located in peripheral reflector channels.
The neutron flux in the standards BR2 fuel element in the cen-
tral position of the H1 beryllium plug characterized by a peak neu-
tron flux (En > 100 keV) up to 6  1014 n cm2 s1. Neutron flux
data used in these calculations are summarized in Table 1. Thermal
neutron cross-sections and resonance integrals were obtained
from the literature (Mughabghab, 2006).
The contribution of the epithermal flux to the Technetium
transmutation process is important, because the main cross section
peaks of the reaction 99Tc (n,c) 100Tc are in the energy interval Fig. 3. BR2 high flux reactor.
 N. Amrani, A. Boucenna / Annals of Nuclear Energy 38 (2011) 1347–1350 1349

Fig. 4. BR2 core configuration.

Table 1
BR2 neutron flux data (n cm2 s1).
Ruthenium Mass Evolution (g)

Neutron energy BR2 (H1)

Thermal 4.2  1014
Epithermal 4.0  1013
Fast > 100 keV 6.0  1014

Table 2
Kozar et al. neutron flux data (n cm2 s1).

Neutron energy Kozar et al.

Thermal 1.7  1015
Epithermal 1.07  1014

Irradiation Time (Days)

Fig. 5. Ruthenium mass evolution in BR2 during irradiation time.
mal fluxes, cross sections of reactions, time of an irradiation and
structure of initial product should taken in consideration (Krivo-
hatskii and Romanov, 1969).
Such calculations allow to define the chosen mode of an irradi-
ation and to calculate the expected outputs for both products and
inevitable impurities. The main approximation used at calculation
of transmutations is the assumption that the influence of changes
in the irradiated material structure on characteristics of a reactor
as a neutron source is insignificant.
1350 N. Amrani, A. Boucenna / Annals of Nuclear Energy 38 (2011) 1347–1350
Transmutation Rate (%)
100 MW
70 MW
Irradiation Time (Days)
Fig. 6. Technetium transmutation rate in BR2 for 70 MW and 100 MW.
5. Results and discussion
The Technetium mass loading in the central position H1 is
about 10 g. For 110 irradiation days (operating power 70 MWth),
the transmutation rates is estimated to 13.17%. The evolution
of Ruthenium mass under irradiation in the BR2 high flux reactor
is shown in Fig. 5. The obtained Ruthenium mass is estimated to
1.32 g.
We notice that the transmutation rate is less than the obtained
one in the same kind of reactor (Amrani et al., 2008). The reason is
that the BR2 reactor is not operating at its full power (100 MW),
because in this case the transmutation rate is high than the ob-
tained one. In the results of Kozar et al. on the transmutation of
99
Tc in the SM-3 high flux research reactor, 30 ± 2% of Technetium
is converted to stable Ruthenium after 72.7 effective full power
days (100 MW thermal power) (Kozar et al., 2002).
In this study, for the same values of the flux densities of thermal
and resonance neutron used in Kozar et al., given in Table 2, and for
110 effective full power days, the transmutation rate in the BR2
high flux reactor is estimated to 47.25%. The use of BR2 reactor
in its full power (100 MW) may increase considerably the Techne-
tium transmutation rate, as shown in Fig. 6.
The principal contributor in this considerable augmentation in
the transmutation rate is the increase in the epithermal flux value
due to its primordial role in Technetium transmutation process.
6. Conclusion
In this study the Technetium transmutation rate and the Ruthe-
nium mass obtained from irradiated Technetium targets in high
flux reactor BR2 were evaluated. This calculation was performed
using ChainSolver 2.34 code. For 110 irradiation days (operating
power 70 MWth), the transmutation yields is 13.17% in the cen-
tral position H1. To increase the Technetium transmutation rate
we suggest that the BR2 high flux reactor became operating at its
full power (100 MW) during the transmutation process. Under this
condition the transmutation rate may increases to 47.25%.
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