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Nuclear Energy and Technology 3 (2017) 220–223

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The results of the transmutation of fission fragments in the spectrum of

neutrons of thermal and fast reactors
N.V. Ivanov∗, Yu.A. Kazansky, G.V. Karpovich
Obninsk Institute for Nuclear Power Engineering, NRNU “MEPhI”, 1 Studgorodok, Obninsk, Kaluga reg. 249040, Russia
Available online 14 August 2017

Abstract
Radioactivity of spent nuclear fuel (SNF) discharged from nuclear reactor core is determined during the first 100 years by fission
fragments (FF), after that the main contribution in the SNF activity is made by actinides. Existing scenarios of SNF handling are based on
the transmutation of minor actinides (MA) into fission fragments accomplished in fast reactors. Scenarios of transmutation of fission fragments
in thermal and fast neutron spectra and time-dependent radiation characteristics are examined in the present study. Nuclide composition of
fission fragments is taken from the results of simulation of burnup of 439GT fuel assembly (TVSA type) for VVER-1000 nuclear reactor
during 3 years performed using MCU-5 software complex. The obtained data were used for determining starting nuclide composition for
different cooling-down times prior to the beginning of transmutation (irradiation in neutron fluxes) to be input in the ORIGEN2 code.
The following three options of irradiation of fission fragments are presented: transmutation without cooling down, cooling down fission
fragments during 4 years prior to irradiation, cooling down fission fragments during 30 prior to irradiation. Duration of irradiation was
selected to be equal to 3 and 15 years. Efficiency of transmutation was determined using time-dependent “transmutation factor” equal to the
ratio of radioactivity of nuclides in the process of transmutation and after its completion to their radioactivity without transmutation.
The calculated values of transmutation factors proved to be noticeable only during irradiation in reactor core: these values reached 5–10
and were dependent only on the duration of fission fragment cooling down prior to the beginning of transmutation. After removal of fission
fragments from neutron flux transmutation factor decreased to unity within several years. After one hundred more years after irradiation in
neutron spectrum of thermal reactor transmutation factor reduces to 0.8–0.5 depending on the duration of the transmutation process. Slight
growth of transmutation factor to the values of 1.2–1.8 was observed after irradiation in fast reactor spectrum within the time interval of
200–1000 years and after 1000 years following this its reduction to the value of 0.9–0.7 was noted.
The main conclusion is that purposeful incineration of fission fragments is senseless because only insignificant gain in radioactivity (a
little less than by the factor two) is achieved after 1000 years.
The indifference of fission fragments with regard to transmutation can be partially explained by the fraction of stable nuclides which
increases with extension of the period of fission fragments cooling down. Upon completion of the cycle of fuel use it contains approximately
15% of stable nuclides among fission fragments, and after 30 years of cooling down the fraction of stable isotopes reaches 85%.
Copyright © 2017, National Research Nuclear University MEPhI (Moscow Engineering Physics Institute). Production and hosting by
Elsevier B.V. This is an open access article under the CC BY-NC-ND license. (http://creativecommons.org/licenses/by-nc-nd/4.0/)

Keywords: Fission fragments; Transmutation; Transmutation factor; Radioactivity.

Introduction

It is known that after discharging spent nuclear fuel (SNF)

∗ Corresponding author.
E-mail addresses: ivanovnik100@gmail.com (N.V. Ivanov),
kazansky@iate.obninsk.ru (Yu.A. Kazansky), gleb3452006@rambler.ru (G.V.
Karpovich).
Peer-review under responsibility of National Research Nuclear University
MEPhI (Moscow Engineering Physics Institute).
from the reactor its radioactivity is mostly determined by fis-
sion fragments and that after several hundred years of cool-
ing down it is determined by actinides (the so called minor
actinides—neptunium, americium, curium). Danger associated
Russian text published: Izvestiya vuzov. Yadernaya Energetika (ISSN
0204-3327), 2017, n.2, pp. 118–125.

http://dx.doi.org/10.1016/j.nucet.2017.07.004
2452-3038/Copyright © 2017, National Research Nuclear University MEPhI (Moscow Engineering Physics Institute). Production and hosting by Elsevier
B.V. This is an open access article under the CC BY-NC-ND license. (http://creativecommons.org/licenses/by-nc-nd/4.0/)
 N.V. Ivanov et al. / Nuclear Energy and Technology 3 (2017) 220–223
with SNF is presupposed by the possibility of release of ra-
dioactive products from SNF in the environment and by the
level of their radioactivity. Therefore, solution of the problem
of SNF and radioactive wastes (RW) is found in the reduc-
tion of probability of their escape in the environment and
reduction of associated radioactivity.
Three decades ago the issue of reduction of radioactivity of
heavy nuclei and fission fragments by transmutation was very
popular. The idea of transmutation consists in the irradiation
of radioactive materials in reactors (dedicated and/or power
reactors). As the result of irradiation heavy nuclei is trans-
muted into fission fragments, which, after capturing neutrons,
can be converted into stable or short-lived nuclides. Trans-
mutation of fission fragments found its reflection in numer-
ous publications, reviews, seminars and conferences. Small
fraction of these references is reflected in [1–8].
The following main results (in the opinion of the authors
of the present paper) were obtained:
- RW transmutation can be accomplished because of the ex-
cess of “surplus” neutrons in self-sustained fission reaction
[2,4–6];
- Only about a dozen of fission fragment species meet the
requirements imposed in the existing conditions on the
transmutation (rate of neutron absorption during irradia-
tion must significantly exceed the rate of radioactive de-
cay) [2,3,5,7];
- In order to be able to formulate conclusions on the fea-
sibility of transmutation of fission fragments it is neces-
sary to account for the probability of escape of radioactive
products in the environment and radioactivity of daughter
nuclei [3,8].
Experimental study of transmutation of two long-lived
technetium nuclides and iodine [9,10] deserves special notice
among later publications.
Fig. 1. Transmutation factor for fission fragments after their discharging from the reactor core: 1—without cooling down prior to irradiation; 2—with cooling
down during 4 years; 3—with cooling down during 30 years (irradiation in thermal spectrum during 3 years).
221
Results of calculations of transmutation factors are re-
ported in the present paper not for separate nuclides, but for
all fission fragments (including as well stable nuclides, be-
cause separation of radioactive and stable fission fragments is
not likely). It is helpful to use here the transmutation factor
ξ r suggested in [8] which is defined as the ratio of radioac-
tivity of nuclides (in the process of transmutation and after
its completion) to radioactivity of the same nuclides with-
out transmutation. This ratio is time-dependent and can be
in excess of unity (transmutation is harmful) and less than
unity (transmutation is beneficial). Dependence of transmuta-
tion factor as function of time has “bipolar” nature respective
to unity. Therefore, the problem emerges whether it is possible
as the result of transmutation “today” to admit some increase
of radioactivity in order to have its reduction “tomorrow”.
Input data
Composition of fission fragments incorporating 830 nu-
clides obtained as the result of simulation of the burnup for
439GT fuel assembly (TVSA type) for VVER-1000 nuclear
reactor [11] during 3 years using MCU-PTR software com-
plex [12] was selected for transmutation. Subsequently, irra-
diation of the above set of fragments in neutron flux was
simulated using ORIGEN2 code [13].
ORIGEN2 code is supported with its own neutron data
library of one-group cross-sections for typical spectra of ther-
mal and fast reactors. Calculation was performed using ho-
mogenous model with spatially uniform neutron flux not tak-
ing into account the effects of blocking of cross-sections.
Therefore, calculations of transmutation factors ξ r are of ap-
proximate nature.
Calculation was performed for two neutron spectra: fast re-
actor spectrum ( = 3.65 × 1015 s–1 cm–2 ) and thermal reactor
spectrum ( = 3.65 × 1014 s–1 cm–2 ).
222 N.V. Ivanov et al. / Nuclear Energy and Technology 3 (2017) 220–223

Fig. 2. Transmutation factor for fission fragments after their discharging from the reactor core: 1—without cooling down prior to irradiation; 2—with cooling
down during 4 years; 3—with cooling down during 30 years (irradiation in fast spectrum during 3 years).

Fig. 3. Transmutation factor for fission fragments after their discharging from the reactor core: 1—without cooling down prior to irradiation; 2—with cooling
down during 4 years; 3—with cooling down during 30 years (irradiation in thermal spectrum during 15 years).

Results of calculation of transmutation factors
Simulation of irradiation of fission fragments was per-
formed for three values of duration of cooling down period
after discharging FF from the reactor core as follows: without
FF cooling down prior to irradiation; with FF cooled down
during 4 years prior to irradiation; with FF cooling down prior
to irradiation during 30 years. For each of the above options
the time of subsequent continuous irradiation by neutron flux
with constant density was equal to 3 years or to 15 years.
Time dependences of transmutation factors ξ r for thermal
and fast neutron spectra are shown in Figs. 1–4. For the sake
of convenience logarithmic time scales are shifted in such a
way as to have the beginning of irradiation at the same time
moment equal for all irradiation exposures to 0.04 years.
Conclusions and discussion
The calculated transmutation factors proved to be notice-
able only during residence of fission fragments in the reactor
core: their values reach 5–10 and depend only on the duration
of cooling down of fission fragments prior to the beginning
of transmutation. The longer is the cooling down period the
higher value is attained by the transmutation factor. This is
most likely in correlation with the fraction of stable fission
fragments which amounts for the case of cooling down dur-
 N.V. Ivanov et al. / Nuclear Energy and Technology 3 (2017) 220–223
Fig. 4. Transmutation factor for fission fragments after their discharging from the reactor core: 1—without cooling down prior to irradiation; 2—with cooling
down during 4 years; 3—with cooling down during 30 years (irradiation in fast spectrum during 30 years).
ing 30 years to about 85%, and to only about 15% for zero
cooling down time. After extraction of fission fragments from
the neutron flux transmutation factor reduces to unity within
several years. After additional hundred years of irradiation in
thermal reactor neutron spectrum the value of transmutation
factor reduces to 0.5–0.8. The following trend is clearly vis-
ible here: the longer is the irradiation time the larger is the
gain obtained as the result of transmutation.
After irradiation in fast reactor spectrum during the time
interval of 100–800 years slight increase of transmutation fac-
tor to the values of 1.2–1.8 is observed and after 1000 years
its reduction to the values of 0.9–0.7 follows. The source of
increase of the transmutation factor appears to be 151 Sm mak-
ing noticeable contribution in radioactivity after 200 years.
Close to 500 years content of this radionuclide in FFs ir-
radiated in fast spectrum is by 4.4 times higher than that
for FFs kept in long-term storage facility without irradiation,
and contribution in the overall FF activity amounts to 44.9%,
while among the non-irradiated FFs 151 Sm contributes only
14.6%. This effect is not observed in the case of FF irra-
diation in thermal spectrum due to high value of radiation
capture cross-section of 151 Sm (∼1.2 × 104 barn) within ther-
mal energy range, which leads to smaller accumulation of
151
Sm in FFs irradiated in thermal spectrum.
Detailed examination of the obtained results allows making
assumption that purposeful incineration of fission fragments
is senseless because of insignificant improvement in radioac-
tivity by not more than two times gained after 1000 years.
Besides that, probability of loss of control in the process of
fabrication and irradiation of fission fragments is higher as
compared with keeping the same radioactivity in storage fa-
cilities.
Estimations of transmutation factors were made for fission
fragments after cooling down during 30 years under the con-
223
dition of their separation from stable fission fragments. In this
case, as it had to be expected, transmutation factor reduced
after 1000 years to the values equal to 0.2 (radioactivity re-
duced by five times as the result of transmutation).
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