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Paul Scherrer Institutes Studies on Advanced

Molten Salt Reactor Fuel Cycle Options

J. Krepel, B. Hombourger, V. Bykov, C. Fiorina, K. Mikityuk,


and A. Pautz

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.

Introduction 2. Specic thermal-hydraulics, dynamics, and limited gra-


phite lifespan, if applied;
The molten salt reactor (MSR) is an old concept [1, 2], which 3. Demanding molten salt reprocessing techniques;
is presently re-viewed because of its appealing features: 4. Fuel salt selection, treatment, and possible proliferation
risks.
1. Excellent neutron economy of the molten salt and of the
thorium fuel cycle; The advantages may enable the design, from the neu-
2. Liquid fuel does not need fabrication and enables, for tronics point of view, of an inherently safe MSR with flex-
example, curium recycling; ible fuel cycle and may represent a strong motivation to
3. Flexibility of the fuel cycle thanks to the previous two overcome the challenges. Furthermore, the advantages may
advantages; be partly sacriced to reduce the challenges. This is the
4. Inherent safety based on negative feedback coefcients general idea adopted by many research teams and also in our
and continuous salt clean-up from highly mobile gaseous research. It is based mainly on MSc students, PhD stu-
and volatile ssion products. dents, and post-docs works, which can be integrated into a
students reactor design project. It may be, in the future,
Contemporary research reopens the discussion about the extended into other relevant elds (thermal-hydraulics, salt
advantages and disadvantages of the technology. The main chemistry, materials behavior, etc.) and supported also by
challenges related to MSRs are: senior researchers.

1. Structural material corrosion and irradiation embrittle-


ment; Appealing MSR Features

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

Springer International Publishing Switzerland 2016 185


J.-P. Revol et al. (eds.), Thorium Energy for the World, DOI 10.1007/978-3-319-26542-1_29
186 J. Krepel et al.

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: 0.9% Gateway


RR: 2.3% RR: 2.2% to
Equilibrium U233 chain Pu241
RR: total reaction rate M: 4.7% C:94.0% M: 0.6% C:37.7% M: 0.3% C:99.9% Pu242
Pu238 Pu239 Pu240
Am
with neutrons relative M: 3.1% C:42.6% M: 0.9% C:34.2% M: 0.8% C:77.4% and
to U233 (without n,2n). RR: 0.3% Cm
RR: 1.9% RR: 0.8% build-up
M: mass relative to U233.
C: capture probability. RR: 2.4% 2d 2.3d
Light blue: thermal MSR M: 4.2% C:99.6%
Dark blue: fast MSR Np237 Np238 Np238
M: 2.7% C:92.1%

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%

RR: 100% RR: 11.0% RR: 8.9% RR: 2.4%


1d 27d

Pa231 Pa232 Pa233

half-live - n, n,2n
26h 22min

Th231 Th232 Th233

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

Fig. 2 MSR flexibility in the 25000


Th-U equilibrium cycle, LiF carrier salt Fast Spectrum
ThU cycle using fluoride (left)
and chloride (right) salts; Thermal Epithermal Fast spectra
break-down of the innite-lattice
reactivity reduction by the 20000 Max. theoretical
equilibrium fuel composition 233 U reactivity

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%

Fig. 3 MSR flexibility in the U 40000


Pu cycle using fluoride (left) and U-Pu equilibrium cycle, LiF carrier salt Fast Spectrum
chloride (right) salts; break-down Thermal Epithermal Fast spectra
of the innite-lattice reactivity Max. theoretical
reduction by the equilibrium fuel 30000
reactivity 239
composition Pu
Reactivity (pcm)

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%

Figures 2 and 3 show the break-down of reactivity No Need for Fabrication


reduction by each nuclide from the equilibrium fuel com-
position, for an innite lattice. As can be seen, in all cases Both fluoride and chloride salts are in liquid form and do not
the maximal realistic reactivity is reached for the fast spec- need fabrication. This simple characteristic may help to
trum. In both the ThU and UPu cycles, enriched 37Cl recycle the U from the ThU cycle. As can be seen in Fig. 1,
provides the highest reactivity, thanks to its low absorption the U vector in ThU cycle includes some amount of 232U.
and harder spectrum. Natural Cl shows higher reactivity than This isotope produces the same decay chain as 232Th, with
fluorides in the UPu cycle; however, it shows lower reac- several hard gamma emitters (e.g., 208Tl); however, its
tivity in the ThU cycle. Accordingly, the hard spectrum of half-life is much shorter. Accordingly, to process any irra-
chloride salts is more suitable for the UPu cycle [6]. The diated Th-based fuel will be demanding in terms of radiation
fluorides are suitable for the ThU cycle and can be used in protection. The previously mentioned volatilization of
both thermal and fast spectra. mixed fluoride salts may help to overcome this issue,
188 J. Krepel et al.

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)

Categories : Low fuel load


Fuel in liquid state, no fabrication (low excess reactivity)
Safety
Flexibility
Economics
Low source term
Excellent neutron economy (low radiotoxic risk)
Sustainability

Available excess neutrons Fuel presence in salt


(thorium breeding and/or (negative thermal feedback coefficient)
actinide burning,
fixed fuel cost)

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

MSRs may be designed as inherently safe reactors thanks to


the negative temperature feedback coefcients and continu-
Fig. 5 Relationship between probability and consequences of risks
ous salt clean-up of highly mobile gaseous and volatile s-
(Farmer graph) illustrated in a loglog scale. In the forbidden area, the
sion products. The removal of gaseous and volatile ssion product of frequency and consequences is not acceptable (Background
products is a technological requirement, which may chart: http://www.iaea.org/ns/tutorials/regcontrol/assess/assess3212.htm)
Paul Scherrer Institutes Studies on 189

Direction of Own MSR Research: Reduction Active core

of Challenges Fertile region

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.

1. Finding new resistant materials without 58Ni;


2. Reduction of the thermal fluence to the material; Simplification of the Reprocessing Strategy
3. Shortening of the irradiation time. in the ThU Cycle

The ultimate aim of almost every fuel reprocessing is to


separate the ssion products and recycle, at best, everything
Reduction of Structural Material Irradiation else. The irradiated MSR fuel consists of:
Embrittlement
1. Carrier salt (LiF, LiFBeF2, NaFBeF2, etc.);
One of the ideas to reduce the thermal fluence, is the hybrid 2. Fertile actinides (232Th);
spectrum MSR [7]. It is an old idea already applied to the 3. Fuel (U vector);
Molten Salt Breeder Reactor (MSBR) at the ORNL. It is 4. By-products (Np and Pu);
based on a two-zone or multi-zone core with one fuel salt, 5. Fission products.
where the moderator determines the criticality in each core
zone (Fig. 6). The outer zone is usually subcritical to reduce From a sustainability point of view, in the ThU cycle it
leakage from the core and, thus, the fluence on the structural may be important to recycle the main fertile element, Th, and
materials. The hybrid spectrum MSR is nothing more than possibly also some rare elements (Li, Be).
an extreme case of this idea, where the small critical thermal From an economical point of view, it may be interesting
zone around the graphite acts as a driver for the big, sub- to recycle all components. Nevertheless, it will depend on
critical, fast zone in the salt. In the pool-type MSR it may their price and on the reprocessing costs. In some cases their
also help to localize the ssion reaction in the center. direct disposal, for example, by vitrication, may be
The idea of a hybrid spectrum MSR was preliminarily cheaper.
evaluated for a simple axially innite reactor design from From a reactor physics point of view, it is important to
Fig. 7 (left) and the resulting radial and spectral flux distri- recycle U as the main ssile element of the ThU cycle; the
bution can be seen in Fig. 7 (right). This gure also justies other components are not substantive.
the title hybrid spectrum MSR. The initial results are The fluorides foreseen for MSRs have one important
promising. Nevertheless, the ssion products, which are not feature. Some elements, such as U, Np, and to certain extent
accounted for in the presented results, may completely Pu, form volatile hexafluorides and can be separated/recycled
190 J. Krepel et al.

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

Fig. 8 Simplied in situ fuel online criticality


recycling by the volatilization in maintenance
the two-fluid MSR. The
remaining carrier salt can be New
directly disposed or reprocessed carrier salt
later and probably ex situ

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)

Removed mass from core (kg/year)


18 18
16 16
14 14
12 NP237 12 NP237
10 10
PU238 PU238
8 8
PU239 PU239
6 6
4 4
2 2
0 0
0 10 20 30 40 50 60 70 80 90 100 0 10 20 30 40 50 60 70 80 90 100
Burned mass (t) or 2.6GW th reactor operation (EFPY) Burned mass (t) or 2.6GW th reactor operation (EFPY)

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.

References 6. Hombourger, B., et al.: Fuel cycle analysis of a molten salt reactor
for breed-and-burn mode. ICAPP 2015. May 0306, Nice, France,
2015
1. MacPherson, H.G.: The molten salt reactor adventure. Nucl. Sci. 7. Kepel, J., et al.: Hybrid spectrum molten salt reactor. Physor (2014).
Eng. 90, 374380 (1985) Kyoto, Japan, September 28October 3, 2014
2. Taube, M.: Fast reactors using molten chloride salts as fuel. Report 8. Kepel, J., et al.: Molten salt reactor with simplied fuel recycling
Nr. 332, Wrenlingen, AG, Switzerland: Eidgenssisches Institut fr and delayed carrier salt cleaning. ICONE 22. July 711, 2014,
Reaktorforschung (EIR) (1978) Prague, Czech Republic, 2014
3. Kepel, J., et al.: Fuel cycle advantages and dynamics features of 9. Kepel, J., et al.: Comparison of several recycling strategies and
liquid fueled MSR. Ann. Nucl. Energy 64, 380397 (2013) relevant fuel cycles for molten Salt reactor. ICAPP 2015. May 03
4. Kepel, J., et al.: EQL3D: ERANOS-based equilibrium fuel cycle 06, Nice, France, 2015.
procedure for fast reactors. Ann. Nucl. Energy 36, 550561 (2009)
5. Hombourger, B.: Parametric lattice study for conception of a molten
salt reactor in closed thorium fuel cycle, MSc Thesis, Joint
EPFL-ETHZ MSc in Nuclear Engineering (2013)

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