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Abstract
Nuclear reactors operated with liquid fuel may have several remarkable advantages and
features. The most developed reactor system in this category is the molten salt reactor
(MSR). It represents an old concept, but its properties qualify it for advanced utilization;
these include inherent safety, excellent neutron economy, continuous or batch reprocessing
possibilities without fuel fabrication. The aim of this study is to characterize the MSR
physics, highlighting its unique fuel cycle advantages in several different neutron spectra by
using the ERANOS-based EQL3D procedure and ECCO-MATLAB- or Serpent-
MATLAB-based EQL0D procedures.
J. Krepel presented this paper at the Thorium Energy Conference Excellent Neutron Economy
2013 (ThEC13)
MSR fuel consists of a molten carrier salt mixed with the
J. Krepel (&) B. Hombourger V. Bykov C. Fiorina
K. Mikityuk A. Pautz salts of actinides and ssion products. Generally, two basic
Laboratory for Reactor Physics and System Behaviour,
Paul Scherrer Institute, 5232 Villigen PSI, Switzerland
salts types, foreseen for two different applications, are con- ssionability may already play an important role. The main
sidered in MSR research: ssile isotope, 239Pu, of the UPu cycle produces up to 2.9
neutrons per ssion in the fast spectrum and so the higher
1. Fluoride salts for the iso-breeding, low-waste-production parasitic capture probability of the chlorides may be
ThU cycle; acceptable. Furthermore, as the solubility of both U and Pu
2. Chloride salts for the high-conversion UPu cycle. is high, the chlorides are more suitable for the fast spectrum
UPu cycle. These conclusions may change in cases where
The fluorides have, in general, lower parasitic capture natural Cl is replaced by enriched 37Cl.
probability and provide, thanks to the high inelastic scat- The excellent neutron economy of the ThU fuel cycle is
tering cross section of 19F, a relatively softer spectrum. As predominantly based on the low neutron capture probability
232
Th has lower ssionability in the fast spectrum, and of the main ssile isotope, 233U. It is present at around 10 %
because 233U as a main ssile isotope produces only 2.5 in both thermal and fast MSR reactors (Fig. 1). Furthermore,
neutrons per ssion in any spectrum, fluorides are well the secondary ssile isotope, 235U, created subsequently
suited for the ThU cycle and its high neutron efciency. from the 10 % of parasitic captures, also has a low capture
This conclusion is also supported by the high solubility of probability. Moreover, if compared with the secondary s-
Th and U tetrafluorides in the carrier salt, whereas the sol- sile isotope, 241Pu, in the UPu cycle, 235U is stable, whereas
241
ubility of Pu, which forms trifluorides, is limited. Further- Pu decays and worsens the neutron economy. Figure 1
more, under certain conditions, U, Np, and partly also Pu, also illustrates that if the 239Pu ssion fails, 240Pu, a gateway
may form volatile hexafluorides and can be easily separated to minor actinides (MA) buildup, is created. In the ThU
from the rest of the fuel, by so-called volatilization. cycle, 239Pu is created through the 237Np and 238Pu path,
Accordingly, fluorides are usually proposed for a clean Th whereas in the UPu cycle it is created directly.
U cycle in thermal or fast spectra. The excellent neutron economy of the ThU cycle in both
The chlorides, on the other hand, have higher parasitic thermal and fast spectra was also proven by a spectral study [3].
capture probability; however, the high inelastic scattering The results of the ERANOS-based EQL3D procedure [4] and
cross section of 19F is absent and a relatively hard spectrum ECCO-MATLAB-based EQL0D procedure [5] are ex-tended
can be achieved. In such a spectrum, the 238U high here for the UPu cycle and chlorides (Figs. 2 and 3).
RR: 2.1%
23min
RR: 100% RR: 12.5% RR: 12.3% RR: 2.4% 7d
M: 100% C:11.0% M: 42.9% C:99.3% M: 14.2% C:18.8% M: 19.3% C:98.2%
U232 U233 U234 U235 U236 U237 U238 U239
M: 100% C: 9.2% M: 35.5% C:81.2% M: 9.3% C:26.7% M: 10.7% C:90.3%
half-live - n, n,2n
26h 22min
Fig. 1 Evolution of the isotopes under neutron irradiation in the ThU cycle using fast and thermal spectra MSR reactors with fluoride salts
Paul Scherrer Institutes Studies on 187
Reactivity (pcm)
15000 234 U
235-8 U
10000
Pu
MA
Salt Th-U
5000 Max. realistic equilibrium
Graphite
reactivity cycle,
NaCl
carrier salt
0
5 10 15 20 30 40 50 60 70 80 90 100 Nat. Cl Enr. Cl
Salt to graphite ratio, salt share in the core (%) Salt share 100%
20000
240 Pu
10000 241-2Pu
Am
MA U-Pu
0 Salt+graphite equilibrium
cycle,
Max. realistic NaCl
reactivity carrier salt
-10000
10 20 30 40 50 60 70 80 90 100 Nat. Cl Enr. Cl
Salt to graphite ratio, salt share in the core (%) Salt share 100%
Fig. 4 Flexibility of the MSR Online criticality maintenance Flexible fuel composition
fuel cycle and its possible (high availability) (without blending and fabrication,
applications enables actinides recycling)
because it is a robust and tested method, which can be simultaneously represent one of the biggest advantages from
operated remotely. a safety point of view. Even though it may increase the
In the UPu cycle, the recycling of Pu is not a techno- frequency of small localized incidents, at the same time, it
logical issue and has been industrially mastered. On the signicantly reduces the source term and may act as the
other hand, the MAs formed in the UPu cycle (Am and strongest pseudo-barrier against the release of ssion prod-
Cm) produce considerable decay heat and Cm also emits ucts during a severe accident. By using the Farmer graph
neutrons. The fabrication of a solid fuel may be, therefore, from Fig. 5 as an illustration, it can be seen that the risk
very complicated. Also in this case, liquid fuel can help to related to MSRs with liquid fuel is of a different nature than
overcome this issue and easily accommodate these actinides. the risk related to solid fuel reactors.
Any hypothetical severe accident possibly may not cause
substantial contamination outside of the power plant as the
Flexibility of the Fuel Cycle driving forces, for example, water pressure or chemical
reaction of the cladding, are missing in MSRs and as the
Thanks to the combination of excellent neutron economy most mobile ssion products are continuously decoupled
and of the liquid fuel not requiring fabrication, the MSR fuel from the major decay heat source and from the ssion chain
cycle can be very flexible. This statement is illustrated in reaction. This promising qualitative statement will need
Fig. 4. This flexibility may help overcome historical obsta- conrmation by stringent evaluation and quantication of
cles for MA burning and 233U breeding related to the heat the risks. After several MSR projects dedicated to techno-
release and radiation hazards mentioned above. The possi- logical issues and reactor-physics designing, this may be the
bility of on-line refueling and reprocessing might also help main direction for further MSR research.
the reactor to operate with high availability and virtually
eliminate reactivity swings and the need for an initial excess
reactivity. If the reactor is to be operated as an iso-breeder
Continuous removal of highly mobile FP
with fuel recycling, the fuel cost should be almost inde- (Ac and remaining FP are embedded in the salt)
pendent from the price of the resources. Furthermore, some
Possible reduction of classical barriers
MSR designs may also enable the recycling of its own or of (safety standards for reactor X reprocessing plant )
legacy MA. Accordingly, MSRs have the potential to serve
as a sustainable and clean energy source with high utilization
of resources and low waste production.
Solid-fuel reactors:
Liquid-fuel reactors:
Inherent Safety
Fissile region
As mentioned in the introduction, MSR advantages may be
partly sacriced to help to reduce the challenges. This is the
general idea adopted by many research teams and also in our
research, which is currently based mainly on MSc students,
PhD students, and post-docs works. The two main tech-
nological challenges are the structural material corrosion and
irradiation embrittlement and the demanding molten salt
reprocessing techniques.
The mitigation of corrosion of the structural materials will
require strict redox potential and impurities control. Never- Fig. 6 Illustration of the two-zone MSR core in the thermal case (left)
and in the extreme hybrid spectrum case (right). (Yellow or orange
theless, the modied Hastelloy-N, proposed at the end of corresponds to salt, gray to graphite)
MSR research at the Oak Ridge National Laboratory
(ORNL), seems to have been conrmed as a suitable mate-
rial for long-term operation after recent tests in Russia. change the conclusion about the advantages and disadvan-
The structural material irradiation embrittlement is related tages of the hybrid spectrum MSR. Another solution to
to the fact that the materials compatible with fluoride salts prevent irradiation embrittlement may be the shortening of
consist mainly of Ni. The natural isotope 58Ni can be irradiation time. This solution can be applied to the two-fluid
transmuted by two predominantly thermal neutron captures MSR (Fig. 8), where the wall between the salts is exposed to
to 59Fe and simultaneously produce one He nuclei. This a high fluence. The reactor should then be designed to allow
leads to embrittlement of the material. Accordingly, the simple exchange of the wall every few years, at best, toge-
He-based embrittlement can be reduced by: ther with the fuel salt.
30 20 50 20 cm
Fig. 7 Simple axially innite reactor design (left yellow = salt, gray = graphite, blue = hastelloy) and the resulting distribution of the normalized
neutron flux (right) in the energy spectrum and space in the radial direction) in the hybrid spectrum MSR
UF6
UF6
TRU&FP&
carrier salt
F2
F2
by the volatilization technique or fluorination. The The need to postpone the salt treatment may be also based
volatilization of fluoride salt mixtures is a robust and tested on the radiological protection of the reprocessing facility.
reprocessing method, which was patented in the US as early The activity of the ssion products and of the 232U decay
as 1958 (patent nr. US 2833617 A). It enables relatively chain left in the salt may require storage time from 10
simple separation of the selected elements from the irradiated 20 years. 228Th is a direct product of 232U decay and has a
carrier salt. As it can be remotely operated, it is also suitable half-life of 1.9 years; the other nuclides in the chain decay
for 232U recycling. As mentioned earlier, this isotope has in fast, for example, 208Tl and 212Bi; thus, the activity and the
its decay chain several hard gamma emitters, namely, 208Tl required storing time may be determined by the 1.9-year
and 212Bi. The idea of simplied reprocessing is illustrated in half-life of 228Th (Fig. 9).
Fig. 8. It is based on in situ fuel recycling by volatilization The volatilization technique has a feature that may make
and delayed, and probably ex situ, carrier salt clean-up or its separation of the elements easier; that is, that as a result of the
direct disposal by vitrication [8]. chemical potentials, UF6 is removed from the salt mixture
Paul Scherrer Institutes Studies on 191
8.E+14
7.E+14
6.E+14
Bq / kg 232U
5.E+14
U232
4.E+14 Daughters rebuilding
3.E+14 Leftover daughters
2.E+14
1.E+14
0.E+00
0 1 2 3 4 5 6 7 8 9 10
Time (years)
232
Fig. 9 Activity evolution for the separated U and its daughter products in the leftover salt
20 20
Removed mass from core (kg/year)
Fig. 10 Yearly removed amount of actinides from a 2600 GWth fast MSR reactor in the cases of U (left) or U and Np (right) recycling by
volatilization
rst, followed by NpF6 and PuF6. Accordingly, which mix- of these two nuclides is small, other criteria may be used for
ture of the three elements will be separated can be selected by recycling strategy selection.
the duration of the volatilization process. Furthermore, U and
Np can be removed from the salt with very high efciency,
whereas Pu only to a certain extent. Two ideal scenarios were Conclusion
simulated here: (1) removal of 100 % U only and (2) 100 %
U + Np separation by volatilization. The results in Fig. 10 It can be concluded that MSRs belong to a class of
show the mass of other actinides left in the irradiated salt after prospective advanced technologies that can help to cover
separation. In both scenarios, the mass will stay below future energy demand, minimize the hazards of severe
20 kg/year for a 2600 GWth fast MSR reactor. However, the accidents, and reduce the amount of radioactive waste pro-
actinide composition will strongly depend on the recycling duced. Their appealing properties may possibly enable
strategy [9]. In the case of U recycling, the main actinide left design of an inherently safe reactor with a flexible fuel cycle
in the irradiated salt will be 237Np (Fig. 10, left); in the case of and represent a strong motivation to overcome the difcul-
U and Np recycling, the main actinide left in the irradiated ties related to structural material corrosion and chemical
salt will be 238Pu (Fig. 10, right). As the neutronic importance technology.
192 J. Krepel et al.
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