Applied Energy 75 (2003) 87–96

www.elsevier.com/locate/apenergy

Transmutation of radioactive waste

S. Chwaszczewskia,*, B. S•owińskia,b,*
a
Institute of Atomic Energy, Otwock-Świerk, Poland
b
Warsaw University of Technology, Poland

Abstract
The current status of radioactive-waste transmutation research is reviewed and suggestions
for further investigations are proposed.
# 2003 Elsevier Science Ltd. All rights reserved.
Keywords: Radioactive waste; Transmutation

1. Introduction

Analysis of the possible scenarios of the optimal development of human civiliza-

tion leads inevitably to the conclusion that the future production of energy on a
large scale will be based on nuclear methods [1]. The main reason is that nuclear-
power plants do not consume oxygen, which is one among the most important ele-
ment of our biosphere and so do not disturb the ecological balance of our planet.
They also do not produce carbon dioxide, which, being amassed in ocean waters,
may also cause fatal consequences for the biosphere [2]. But at the same time nuclear
power must be safe and not produce hazardous radioactive-waste (RW). At the
present stage of our knowledge, this is quite achievable in the so-called accelerator-
driven sub-critical (ADS) reactors when the effective multiplication factor of neu-
trons may not exceed
0.95 and the RW may be incinerated and transmuted to the
acceptable rate [3]. In this way, one can also considerably diminish the huge amount
of more than 200,000 tons of up till now accumulated RW, which derives mostly
from the operation of nuclear reactors and military devices and is growing by some
10,000 tons every year. Moreover, it is anticipated to reach about 300 kilotons by
the year 2010 [4]. This mass of RW represents at present very serious problems both
from the economic and ecological points of view.

* Corresponding author. Fax: +48-22-810-59-60.

E-mail addresses: sch@cyf.gov.pl (S. Chwaszczewski); slowb@hp2.cyf.gov.pl (B. S•owiński).

0306-2619/03/$ - see front matter # 2003 Elsevier Science Ltd. All rights reserved.
doi:10.1016/S0306-2619(03)00022-9
88 S. Chwaszczewski, B. Slowiński / Applied Energy 75 (2003) 87–96

Nomenclature

ADS accelerator driven system

CR capture rate
EA energy amplifier
JINR Joint Institute for Nuclear Research
LHE Laboratory of High Energy
LLFF long-lived fission fragments
RW radioactive waste
RWT transmutation of radioactive waste
TARC transmutation by adiabatic resonance crossing
TN transuranic nuclide
TR transmutation rate

So, the effective destruction (i.e. incineration and/or transmutation, depending on

the concrete management strategy for spent fuel [5]) of RW and, in particular, plu-
tonium isotopes, minor actinides and long-lived fission products, becomes the key-
stone problem for future generation of nuclear power. The fact that each isotope has
different properties signifies that there is no universal method and individual
approaches should be established for each of them.
Nowadays one can consider as commonly accepted that the best way for the
transmutation of most of the RW to stable or short-lived nuclides leads to the use of
the intense and higher than thermal energy neutron fluxes (51016n/cm2s) [1]. To
produce such intense fluxes, a beam of
1 GeV protons interacting with heavy
extended targets (Pb, W, U, Pb/Bi eutectic, mercury) should be applied [6], but other
ways (ion, electron and gamma beams, and even underground nuclear explosions
[7]) are also discussed.
Although our knowledge about nuclear reactions is extensive enough, the thor-
ough and systematic investigation of RW transmutation (RWT) started relatively
not long ago and so far the problem of RWT still remains on the level of scientific
investigation and some experimental set-ups have been constructed and successfully
applied (for example, [8–10]).
In this work, we present the physics background of optimal RWT and overview
the main results of such studies conducted at several nuclear centers [8–10] and, in
particular, in the Joint Institute for Nuclear Research (Dubna), where it has been
shown that, even by means of a simple and cheap experimental assembly, it is pos-
sible to get useful results and practical suggestions for further investigation. We also
indicate that the basic problem, which must be studied, is the more precise determi-
nation of neutron fields produced by different relativistic particles.
 S. Chwaszczewski, B. Slowiński / Applied Energy 75 (2003) 87–96 89

2. Radioactive nuclides destined for transmutation

Although there exists a rich variety of sufficiently long-lived radioactive nuclides

created in nuclear reactors (for example, [4,11,12]) as well as in other nuclear-devices
(mostly, in military ones), a few of them are especially hazardous both on account of
their radiotoxicity and as dangerous materials. Therefore the International Com-
mission on Radiation Protection published a list of the most important long-lived
fission fragments (LLFF) and transuranic nuclides (TN) and their radiation prop-
erties. We reproduce it in Table 1.
Two parallel ways of reduction of RW have recently been delineated: (1) trans-
mutation (or transformation) of radioactive LLFF, such as 99Tc, 129I and 135Cs,
which are useless for further gain of energy, by neutron capture and following b
decay into stable ones, and (2) incineration or burning up of TN by means of
nuclear fission induced in nuclear reactors (or the so-called energy amplifiers—EA)
causing energy release and emission of secondary neutrons. Note that transuranic
nuclides decay basically by a emission, i.e. they are much more radiotoxic than fis-
sion products, which are b emitters. Moreover, it is worth emphasizing that the main
LLFF, 99Tc and 129I, which represent
95% of the LLFF volume, are soluble in
water and consequently can contaminate the biological chain of our planet.

3. Conceptual background of optimal transmutation

In principle, the transmutation of RW can be realized by means of different par-

ticles, mainly charged particles (electrons, protons, ions), hard gamma rays and
neutrons. Nevertheless, neutrons are the most efficient owing to their favourable
cross-section and lack of Coulomb barrier.

Table 1
Data concerning the most important long-lived fission fragments and transuranic nuclides, published by
the International Commission on Radiation Protection (after [13])

Nucleus Half-life Dose factor Activity Radiotoxicity

(years) (Sv/Bq) (Bq/kg) (Sv/kg)
99
Tc 2.111105 0.78109 6.31011 4.9102
129
I 0.157108 0.11106 6.5109 0.7103
135
Cs 0.230107 0.20108 4.21010 0.8102
237
Np 0.214107 0.11106 2.61010 0.3104
233
U 0.159106 0.25106 3.61011 0.9105
238
Pu 0.877102 0.23106 6.31014 1.4108
239
Pu 0.241105 0.25106 6.31012 0.6106
240
Pu 0.656104 0.25106 8.31012 2.1106
241
Pu 0.143102 0.47108 3.81015 1.8107
242
Pu 0.373106 0.24106 1.51011 0.4105
241
Am 0.433103 0.20106 1.31014 0.3108
243
Am 0.737104 0.20106 7.41012 1.5106
241
Cm 0.291102 0.20106 1.91015 0.4109
244
Cm 0.181102 0.16106 3.01015 0.5109
245
Cm 0.850104 0.30106 6.31012 1.9106
90 S. Chwaszczewski, B. Slowiński / Applied Energy 75 (2003) 87–96

At present one can consider as available the complex solution of the following
mutually-related problems: ecologically safe and commercially competitive produc-
tion of energy with the simultaneous transmutation and incineration of the created
RW. This requires the construction of ADS. The first complex analysis of the
problem has been done in Ref. [3], although the suggestions of this kind have a long
history (for example [14], and the references quoted therein). In this way, one can
also realize validly the process of nuclear breeding when isotopes 238U and 232Th are
transformed into easily fissile nuclides 239Pu and 233U. However, for this purpose, it
is necessary to have at least one extra neutron simply to sustain the ordinary chain
fission reaction. Just due to these, extra neutron new fissile nuclei 239Pu or 233U are
produced in the (n,
) type reaction. Such favourable operating conditions for the
nuclear reactor are to be achieved with the help of a high-current (about 50–100
mA)
1 GeV proton accelerator as a source of additional energetic (i.e. 51 MeV)
neutrons. Indeed, as shown in Fig. 1, the neutron yield significantly increases with
increasing primary neutron energy at E51 MeV.

Fig. 1. (a) Dependence on neutrons energy of average neutron yield in the reaction (n,l) for 1 neutron
causing fission of nuclides pointed in the figure. (b) Typical neutron energy distributions in (1) thermal
reactors, and (2) fast reactors; (3) energy distribution of fission neutrons (after [14]).
 S. Chwaszczewski, B. Slowiński / Applied Energy 75 (2003) 87–96 91

127
Fig. 2. Transmutation scheme of I and 129I (after [16]).

At the same time, using intense and higher than thermal energy neutron fluxes
(
1016n/cm2s), it is possible to transmute much more effectively the long-lived
radioactive nuclei of nuclear waste to become stable or short-lived ones [15], even in
a parasitic mode to minimize in this way the cost of the process [8]. Nevertheless, it
should be stressed that as a consequence of the different properties of nuclides, there
is no universal method for their transmutation and the relevant individual approa-
ches for each of them should also take into account the specific conditions of irra-
diation. As an example, Fig. 2 demonstrates a simplified transmutation scheme of
129
I and 127I for actual experimental conditions [16].

4. Experiments and results

Valuable and instructive experimental information about the main LLFF and TN
transmutations has been collected for heavy extended-targets irradiated with high
enough energy proton and ion beams. So, the estimations of the yield of some pro-
cesses have been obtained for the major long-lived nuclides: 99Tc, 129I, 237Np and
239
Pu occurring in acceptable conditions via the following reactions [9,17]:
99



Tc t1=2 ¼ 2:11105 yr:Þ þ n ! 100 I t1=2 ¼ 15:8 s ! 100 RuðstableÞ;
129



I t1=2 ¼ 1:57107 yr: þ n ! 130 Tc t1=2 ¼ 12:4 h ! 130 XeðstableÞ;
237




Np t1=2 ¼ 2:14106 yr: þ n ! 238 Np t1=2 ¼ 2:12 d ! 238 Pu t1=2 ¼ 88 yr: ;
239


Pu t1=2 ¼ 2:41104 yr: þ n ! fragments
91


Sr;92 Sr;97 Zr;99 Mo;103 Ru;105 Ru;132 Te;133 I;135 I and 143 Ce
having half-life times of several hours up to several days:
92 S. Chwaszczewski, B. Slowiński / Applied Energy 75 (2003) 87–96

Moreover, the neutron flux-measurements have also been performed: this is neces-
sary for the optimization of the transmutation process, especially when on a large
scale. Below, we present a short insight into three such experiments: TARC (CERN)
[8], LHE JINR (Dubna) [9,17] and Brookhaven AGS Spallation Target Experiment
[10].

4.1. Experiment TARC [8]

In Fig. 3, a general view of the set-up used in the experiment TARC for the
investigation of the capture rate (CR) of neutrons for 99Tc is depicted schematically.
The basic idea of this experiment consists in the use of adiabatic resonance cross-
ing for transmutation when a block (3.33.33 m3) of pure lead was taken as a
moderator of spallation neutrons and dense neutron ‘‘storage’’ medium [8]. The
doubly magic structure of the 52.4% 208Pb nucleus makes such a target one of the
most transparent at 41 keV. The CR of neutrons (from 2.5 and 3.57 GeV/c proton
beams) for 99Tc, 129I and 127I were measured in different places of the lead block. So,
for example, the CR for 99Tc is 2.67( 0.43)105 per 109 protons. Similar values of
CR for 129I and 127I in the same place are 26,100 2600 and 14,900 1500 per 109
protons, correspondingly [8]. The neutron flux over 8 orders of magnitude in neu-
tron energies from thermal up to
2 MeV was also measured in detail. It appears

Fig. 3. General view of the TARC experiment (lower left) as well as 99Tc neutron capture cross-section vs.
neutron energy En (left-hand scale) and typical neutron fluence energy distribution (hole 10. z=+7,5 cm)
vs. En for 3.5 GeV/c protons (right-hand scale). Energy distribution of neutrons from the spallation pro-
cess (in arbitrary units) ([8]).
 S. Chwaszczewski, B. Slowiński / Applied Energy 75 (2003) 87–96 93

possible to destroy large amounts of 99Tc or 129I at a rate exceeding the production
rate and, therefore, to reduce the existing stockpile of LLFF [8].

4.2. JINR Experiment [9]

The experimental assembly for transmutation of some long-lived RW nuclides

(129I, 237Np and 239Pu) built at LHE JINR (Dubna) is sketched in Fig. 4. Several
target materials (Pb, U-Pb and Hg) were used to study the effect of the target
material on the thermal neutron yield at various proton energies in the range 0.5–1.5
GeV. This experimental assembly for the Pb target consisted of 20 Pb discs, each of
diameter 8 cm and thickness 1 cm, surrounded by 6 cm paraffin (CH2) as the
moderator. The second target was composed of U-Pb and consisted of two U foils
each of diameter 3.6 and 10.5 cm length. The two U foils were slid inside 21 lead
cylinders, each of 1 cm thickness, 3.6 cm inner diameter and 8 cm outer diameter.
The lead cylinders were also surrounded by 6 cm thickness of paraffin as the
moderator. The mercury target was fitted to the cylindrical stainless-steel container
of diameter 4.2 cm. It was held inside the paraffin moderator with the aid of two thin
Perspex rings and the space between the Hg-target and paraffin was occupied by air.
Spallation neutrons were produced as a result of the interaction between the rela-
tivistic protons and the heavy extensive targets. One of the most effective methods of
measuring the distribution of spallation neutrons around the target is via the activ-
ities of two radiochemical sensors through the (n,
) and (n,f) reactions. Two radio-
chemical sensors, 139La and natural uranium, were used, as having suitable cross
sections with thermal neutrons and the daughter nuclei have acceptable half-life
times. Since natural uranium consists of two different isotopes 235U and 238U (with
isotopic abundance 0.720 and 99.275%, respectively) and spallation neutrons have a
wide energy range, the neutrons interact with the 238U nuclei through two channels:
238
U(n,
)239U () 239Np and 238U(n, 2n)237U depending on the neutron energies.

Fig. 4. Experimental assembly of the LHE JINR (Dubna) [9].

94 S. Chwaszczewski, B. Slowiński / Applied Energy 75 (2003) 87–96

Since 238U is a fission material as well as 235U, it follows that the natural uranium
will fission into four fragments: 91Sr, 132Te, 133I and 97Zr. In the case of the 139La
sensor, the activation reaction 139La(n,
) 140La takes place.
Five natural uranium sensors in the form of uranium-oxide (UO3–H2O) and eigh-
teen lanthanum sensors in the form of lanthanum–chloride (LaCl37 H2O), each of
about 1 g filled in small bottles, were installed around the surface of the paraffin mod-
erator. Five La sensors were placed at 1 cm depth on the top surface of the paraffin
moderator and separated by 5 cm. Five U sensors were arranged in the same manner at
20
to the La sensors. Other La sensors (from 6 to 10) were distributed around the
paraffin moderator at angles of 60
and two La samples were placed at the end of the
moderator. To study the radial distribution of neutrons around the target (inside and
outside), six La sensors were used. All this sensor topography is demonstrated in Fig. 5.
After the irradiation is finished, the gamma rays spectra of the radiochemical
sensors were measured using several HPGe detectors and analyzed to estimate the
relevant transmutation rates (TRs).
Finally, the following macroscopic TR of LLFF has been deduced under condi-
tions that a Pb target set-up was exposed to the 1 GeV and 10 mA proton beam
(using 1 g samples) [9]:

6.7 mg of 239Pu is transmuted per day,

3.3 mg of 238U is transmuted in one month,
21 mg of 237Np is transmuted in one month,
3 mg of 129I is transmuted in one month.

4.3. AGS spallation target experiment [10]

In this experiment, the characteristics of spallation neutrons produced in a mer-

cury target by protons of 1.94, 12 and 24 GeV energies were investigated using the

Fig. 5. Positioning of La and U sensors in the LHE JINR (Dubna) experimental set-up for transmutation
investigations: plane (left) and front (i.e. along the beam axis) projections (right) [9].
 S. Chwaszczewski, B. Slowiński / Applied Energy 75 (2003) 87–96 95

Alternating Gradient Synchrotron facility of BNL. The application of a large vari-

ety of activation detectors (indium, niobium, aluminum, cobalt, nickel and bismuth)
made it possible to obtain detailed information about neutron energy-spectra
between 0.33 and 40.9 MeV [10].

5. Trends

One can distinguish the following worthwhile lines of investigation in the field of RWT:

1. Selection of the optimal means for the most effective transmutation of RW, as
well as the investigation of radiation hardness of the materials used for RWT.
2. What RW is to be effectively transmuted by means of the nuclear unit
(reactor and/or ADS)?
3. How to produce energy in such a way that the amount of created RW would
be minimal.
4. Determination of requirements imposed upon the RW after transmutation
from the viewpoint of its further utilization or management.

6. Conclusions

Summing up, one can make the following conclusions (se also [18]):
The experimental estimation of transmutation rates of the main long-lived radio-
active nuclides performed in different laboratories shows that it appears possible to
passivate large amounts of 99Tc or 129I at a rate exceeding the production rate and,
therefore, to reduce the existing stockpile of RW [19]. This conclusion seems to refer
equally well to other RWs and, in particular, to 237Np and 239Pu [9].
The small, flexible and inexpensive experimental assembly used for transmutation
studies at the LHE, JINR (Dubna), as shown in Fig. 4, may also be very useful in
providing valuable information about the main characteristics of nuclear reactions,
which occur within extended heavy targets. But it is well to bear in mind that the
number of spallation neutrons is strongly dependent on the target composition and
size (length and diameter) and, to a much lower extent, on the energy of the relati-
vistic incident particle.
As during the irradiation of a slice of concrete nuclide, the produced stable product
may be excited again to the radioactive state. It is necessary therefore to stop the
process after some optimal time in order to remove, by means of radiochemical
methods, these products and only then to continue with the transmutation [20].
It should be added that irradiation of extended materials, comprised of heavy
unstable nuclides, leads to complicated phenomena. So, for example, it was demon-
strated by modeling that as a consequence of permanent incineration of Am and Cm
radioactive nuclides in a thermal neutron fluency of 1014 s1 cm2, the radiotoxicity
reaches its maximum value (several times greater then the former one) after only 5
years [21]. Therefore the optimal transmutation of actinides should be conducted in
96 S. Chwaszczewski, B. Slowiński / Applied Energy 75 (2003) 87–96

a steady-state regime, during which the fission products are progressively removed
and new fissile material added (see also [4]).
It is pertinent to note that a simple probabilistic Monte Carlo simulation of the
direct intranuclear cascading combined with pre-equilibrium and compound nuclear
models cannot be considered as reliable with such a large interval of energy (from
thermal to relativistic) of primary and secondary particles [22]. The more so, as there
exists a fully quantum-mechanical microscopic approach (RQMD code) able to
predict much more precisely all the different reaction channels [22,23].
Although great efforts have been made up to now in the field of transmutation of
long-lived fission products and incineration of transuranic nuclides, we are at pre-
sent still far from being ready to construct a highly-effective installation for waste
processing and much more needs to be done to achieve this end. Nevertheless the
successful solution of this problem seems to be inevitable.

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