Ruben Braas
Michael Koene
Steven Kortekaas
Mike van der Lans
Rutger van der Spek
Abstract
Thoriumfuelled molten salt reactors are up and coming in the field of nuclear
reactors. A thoriumfuelled molten salt reactor uses a molten fluoride salt containing
fissile materials and fertile material as a fuel. It operates in a thermal neutron
spectrum. Another design is a molten salt fast reactor, which is similar to an
ordinary molten salt reactor, but instead operates in a fast neutron spectrum. One
of the questions concerning the thoriumfuelled molten salt reactor and molten
salt fast reactor is whether or not they proliferation resistant. This depends on
the coproduction of 232U along with 233U in the thorium fuel cycle. While 233U
is suitable for making nuclear weapons, the coproduction of 232U may inhibit its
usability. This is because 208Tl is produced in the decay chain of 232U which emits
high energy gamma rays, causing difficulty in making a nuclear bomb with uranium
obtained from the thorium fuel cycle. It is stated in literature that a nuclear reactor
is proliferation resistant if the fraction of 232U to all other uranium isotopes is at
least 5.0 ppm. Since protactinium isotopes decay with a relatively short halflife to
uranium isotopes, the fraction of 232Pa to all other protactinium isotopes needs to
be at least 5.0 ppm as well for a nuclear reactor to be proliferation resistant.
The production of 232U in the thorium fuel cycle is investigated by developing a
mathematical model that simulates the nuclide concentrations in the thorium fuel
cycle for different neutron fluxes. Since no cross section values are available for a
molten salt reactor or a molten salt fast reactor, cross sections in a pressurized water
reactor have been used to approach those of a molten salt reactor (with thermal
neutrons) and cross sections in a liquid cooled metal reactor have been used to
approach those of a molten salt fast reactor (with fast neutrons).
The bestcase scenario for a molten salt reactor occurs for a neutron flux of
1 1014 n s1 cm2 , the expected neutron flux in the breeding blanket for the molten
salt reactor. In this scenario, the ratio of 232U exceeds 5.0 ppm within 21 days.
However, the ratio of 232Pa exceeds 5.0 ppm after 143 days, which is too long of a
time because protactinium can be separated from the reactor fuel before this ratio
reaches 5.0 ppm. Therefore it can be concluded that the molten salt reactor is not
proliferation resistant. The bestcase scenario for a molten salt fast reactor also
occurs for a neutron flux of 1 1014 n s1 cm2 , the expected neutron flux in the
breeding blanket for the molten salt reactor. In this scenario, the ratio of 232Pa is
only 2.54 ppm after one year. Therefore it can be concluded that the molten salt
fast reactor is not proliferation resistant either.
To obtain more reliable results, more research into the exact cross sections in a
molten salt reactor and a molten salt fast reactor has to be conducted. Experimental
verification of cross sections can only be done by building a molten salt reactor
or a close substitute. In this case, however, the proliferation resistance can also
be determined by experiments. Finally, finding a way to inhibit the separation of
protactinium from the reactor fuel is a big step in the direction of a proliferation
resistant nuclear reactor.
Contents
Introduction
1 Background
1.1 Basics of a nuclear fission reactor . . . .
1.2 Basics of a molten salt nuclear reactor .
1.3 Nuclear reactions . . . . . . . . . . . . .
1.4 Characteristics of the thorium fuel cycle
1.5 Production paths of 232U . . . . . . . .
1.6 Radiological properties of 232U . . . . .
1.7 Proliferation resistance . . . . . . . . . .
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2
. 2
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. 7
. 8
. 9
. 10
2 Numerical Research
2.1 Model . . . . . .
2.2 Assumptions . .
2.3 Verification . . .
2.4 Results . . . . . .
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12
12
14
14
15
3 Analysis
19
3.1 Discussion & Conclusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . 19
3.2 Recommendations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
References
21
A ODE system
22
B Data Model
23
C MATLAB Code
24
ii
Introduction
Nuclear reactors account for 10.9% of the worldwide energy production [9]. These nuclear
reactors are fuelled with enriched uranium (and sometimes partly with plutonium).
Nowadays, due to the high abundance of thorium, the thoriumfuelled nuclear reactor is
gathering interest. Unlike watercooled reactors, this nuclear reactor uses a molten salt
as reactor coolant and as carrier for the fuel and is therefore called a molten salt reactor.
A few important questions relating to the thorium fuel cycle arise, one of which is whether
it is proliferation resistant, meaning it is difficult to produce nuclear weapons from the
fissile products. In this fuel cycle 233U is produced, which is highly usable for nuclear
weapons. However, the coproduction of 232U could undermine the weapon usability. [6]
This is the case when the proportion of 232U reaches a critical point. In this report the
proliferation resistance of this uranium mixture is investigated by analyzing the decay
chain and calculating the amounts of 232U and 233U produced using a mathematical
model.
Firstly, the basics of a nuclear fission reactor are discussed, followed by an introduction
to molten salt nuclear reactors. Afterwards a few types of nuclear reactions are discussed.
Then the characteristics of the thorium fuel cycle in the molten salt reactor will be
covered, including its advantages and disadvantages. Thereafter the production paths
of 232U in the Thorium fuelled reactor are treated, followed by the analysis of the 232U
decay chain and its radiological properties. Afterwards, the proliferation resistance is
dealt with.
In the second part of this report, the numerical research is presented. The workings of the
model are discussed, after which the assumptions made creating the model are treated.
Then, the parameters used in the model are considered. This is followed by a validation
of the model. Finally, the found results are given, accompanied by an interpretation and
conclusion.
This report is a part of the first year end project of the BSc. programme Applied Physics
at the TU Delft.
Background
1.1
Before the production of 232U inside the thorium fuel cycle and molten salt reactors are
considered, an account of the basics of nuclear fission reactors is given. Nuclear fission
reactors generate electricity by harnessing the thermal energy released by controlled
nuclear fission. In a nuclear fission reaction, a fissile nucleus absorbs a neutron, after
which the nucleus becomes unstable. The parent nucleus can split into two or more
lighter nuclei, releasing free neutrons and energy. The free neutrons can cause additional
fissioning of other fissile nuclei, which in their turn can trigger further fission events. This
is known as a nuclear chain reaction.
To understand why fission occurs, the nuclear binding energy curve is shown in Figure 1.
This illustrates the average binding energy per nucleon in MeV. The bigger the binding
energy per nucleon, the more stable the nucleus is. From the figure it is clear that the
most stable nucleus is 56Fe. Fission occurs in nuclei with an atomic number greater than
56
Fe. For example, when 235U fissions, it splits into two lighter nuclei with higher binding
energies per nucleon, releasing energy in the process. Nuclear fission reactors come in
many forms, such as a pressurized water reactor (PWR). This is a type of light water
reactor (LWR) which constitutes the majority of fission reactors. A LWR uses water as
a moderator and coolant, as the name suggests. The use of a moderator is explained in a
further paragraph.
1
Wikimedia Commons. Binding energy curve  common isotopes. 2012. url: https://commons.
wikimedia.org/wiki/File:Binding_energy_curve__common_isotopes.svg
In a PWR, the fission reaction takes place inside the reactor core. The heat in the core
is absorbed by a coolant, namely water. The coolant is circulated through the core in
the primary loop, which is connected to the secondary loop by a heat exchanger. In the
secondary loop water is converted into steam to generate electricity using a turbine and a
generator. Another common type of LWR is the boiling water reactor (BWR). The main
difference of a BWR is that they do not employ a secondary loop to generate steam. A
schematic view of a pressurized water reactor (PWR) is shown in Figure 2.
Inside the reactor core, heat is generated in a number of ways. First of all, kinetic energy
of the fission products released in the fission reaction is converted to thermal energy
when these nuclei collide with nearby atoms. The reactor core materials also absorbs
most of the gamma radiation produced during fission and converts that into thermal
energy. Also, heat is produced by the radioactive decay of the fission products. Lastly,
heat is produced by the absorption of gamma radiation and beta particles produced in
this decay. This source of thermal energy will remain active for some time even after the
reactor has been shut down.
The number of neutrons that are able to cause additional fission can be regulated using
control rods, which contain neutron absorbers such as boron. By sliding them in between
the fuel rods in the core, the number of neutrons that can cause fission is reduced, slowing
down the fission chain reaction. The multiplication factor k is defined as the ratio of the
number of neutrons in the next generation Ng+1 to the number in the current generation
Ng .
Ng+1
k=
(1)
Ng
When k = 1, the number of neutrons does not change over time, and the reactor is said
to be critical. When k > 1 it is supercritical. Control rods are used to keep the reactor
2
critical.
Another important feature of a nuclear fission reactor is the moderator. It causes fast
neutrons that are released from fission to lose energy and become thermal neutrons.
Thermal neutrons have energies below 1 eV and have a larger probability to cause fission
than fast neutrons. Using a moderator, the power output of a reactor can be increased.
1.2
Molten salt reactors (MSR) are a type of nuclear reactor in which the fissile and fertile
material are dissolved in molten fluoride salt of high boiling point (over 1400 C) and
operate in an thermal neutron spectrum. They operate at a temperature of around 450 C
to 800 C, which is higher than a LWR does, providing improved thermal efficiency. [6]
The core of a MSR is usually a cylindrical graphite block which can act as a moderator.
Holes are drilled through that core, in which the molten fluoride salt containing fissile
and fertile material such as uranium and thorium circulates. The molten salt acts as
primary coolant, which flows to a primary heat exchanger. There the heat is transferred
to a secondary molten salt loop, after which the primary coolant flows back to the reactor
core. The secondary loop then transfers the heat to the power cycle where electricity is
generated. A schematic view of a MSR is shown in Figure 3.
Figure 3. Schematics of a thermal molten salt reactor with a thermal neutron spectrum.3
3
B. Abrams et al. A Technology Roadmap for Generation IV Nuclear Energy Systems. Report. Nuclear
Energy Research Advisory Committee, 2003
Another design is a molten salt fast reactor (MSFR), a further development of the Oak
Ridge National Laboratory molten salt breeder reactor. This reactor is based on the
same principles as an MSR, but operates in a fast neutron spectrum instead of a thermal
neutron spectrum. The biggest advantage in comparison to a ordinary MSR is the
amount of salt that needs to be cleaned from lanthanides and actinides. This is only 40
litres per day in comparison to 4 000 litres per day in an ordinary molten salt reactor. A
schematic layout of a MSFR is shown in figure 4.
Figure 4. Schematic layout of a molten salt fast reactor, showing the location of the system for
cleaning and draining of the fuel salt, and the three containment barriers (pink, yellow, grey).4
A MSR includes some major advantages compared to the current LWR. Most importantly,
a MSR is walkaway safe; i.e. they have an inherent safe design. In the case of a loss of
coolant the fuel itself is removed from the core, forcing the reaction to stop. If the coolant
overheats, the resulting expansion pushes some of the fuel out of the core, decreasing
the fission rate also. Even if a MSR were to overheat for some reason, a freezeplug at
the bottom of the reactor would melt and the molten salt would drain into emergency
cooling tanks.
4
J.L. Kloosterman. A Paradigm Shift in Nuclear Reactor Safety with the Molten Salt Fast Reactor
(SAMOFAR). in: Projectvoorstel H2020 (Sept. 2014)
The molten salt does not produce hydrogen in case of overheating such as a LWR or a
BWR do, nor is the coolant under high pressure (a MSR operates under atmospheric
pressure), excluding the possibility of any explosion releasing radiotoxic material.
Another major advantage of a MSR is the continuous removal of volatile fission products
such as krypton and xenon in a chemical processing plant. In this way the closed fuel
cycle can be tailored for the efficient burn up of plutonium and minor actinides. As
a result of this, a MSR only produces nuclear waste with a relative short lifespan, see
Section 1.4.
Compared to other types of reactors, a thermal spectrum MSR has a low inventory of
fissile materials. They are thermal reactors requiring less fuel than fast reactors. Little
excess reactivity is needed to compensate for burn up as fuel is added while it is operating.
Direct heat deposition in the coolant allows high specific power. And lastly, in the
chemical processing plant high neutron absorption fission products such as xenon can be
continuously removed.
There are some disadvantages, however. Compared to other Gen IV designs (reactors
currently being researched), little development has been made. An onsite chemical plant
is needed to manage the fission products in the molten salt. Corrosion may occur over
many decades of operation and neutron damage to solid moderator materials can limit
the core lifespan. Finally, there is a necessity for regulatory changes to deal with the
different design features.
1.3
Nuclear reactions
This section concerns the nuclear reactions happening inside a molten salt reactor. The
first type is radioactive decay, in which an unstable nucleus (parent) loses energy by
emitting gamma, beta or alpha particles. The resulting nucleus is called the daughter
nucleus. An example of radioactive decay in the decay chain of 232Th is given by 233Th.
233
Th
Pa +
233
Other types of reactions include neutron induced reactions. A type of neutron induced
reactions is neutron capture, or (n,). A good example of this is neutron capture by
232
Th.
232
Th + 10n
233
Th +
U + 10n
6
232
U + 2 10n
1.4
When thorium is used as fuel, a MSR operates slightly differently. The thorium fuel cycle
uses thorium fluoride and lithium fluoride salts. The reactor starts with 232Th. The
fuel cycle needs start up fuel, such as 233U or 239Pu, to obtain the neutrons required to
initiate and sustain the reaction. This reactor is operating at 630 C and does not need a
graphite moderator inside the core, because lithium is an effective moderator if the 233U
concentration is increased. The core has special neutron reflectors to ensure that 80% of
the neutron flux is absorbed [12].
Thorium is significantly more prevalent in nature compared to uranium. It has not been
exploited commercially and can be stored relatively easy because it is hardly radioactive.
In Figure 5 the discovered supplies of thorium around the world are displayed.
Another major advantage of the thorium fuel cycle in combination with the design of a
MSR is that the amount of radioactive waste is much lower than for the uranium fuelled
reactor. The radiotoxicity of the fission products drops below the level of uranium ore in
a timespan of 300 years, compared to 300 000 years for actinides such as plutonium. This
reduced radioactivity would mean great savings on the size and the costs of geological
storage [6].
Because 232Th has a higher capture cross section, 232Th has a higher possible conversion
to 233U than 238U has to 239Pu. This means thorium is a better material in thermal
reactors and a weaker material in fast reactors.
Typically, a hundred to a thousand times less plutonium and minor actinides are formed
in the thorium fuel cycle compared to the 238U 239Pu fuel cycle and therefore more energy
5
S.F. Ashley et al. Nuclear energy: Thorium fuel has risks. In: Nature 492 (Dec. 2012), pp. 3133
can be produced.[6] This means that the uranium fuel cycle is potentially more radiotoxic
than the thorium fuel cycle. On the other hand radionuclides such as 231Pa, 229Th and
230
U are created which may be radiotoxic too. [6]
Molten fluoride salts such as ThF4 are used as fuel but work as a coolant at the same
time. This means that this reactor does not need water as a coolant, excluding the
possibility of steam explosions or hydrogen production within the containment  a much
safer design [13].
In the thorium decay chain also 232U is produced. These nuclei greatly affect the
proliferation resistance, see Section 1.7. In the next section the production paths of 232U
is discussed.
1.5
232
Production paths of
There are two production paths of 232U with 232Th as starting point. It starts with one
of two possible neutron interactions. The first is a (n,2n) reaction into 231Th, which
undergoes several processes ending in 232U. The other option is the (n,) reaction into
233
Th. This decays into 233Pa, which either decays into 233U, reacting via (n,2n) into
232
Pa; or reacts via (n,) into 234Pa. 231Th decays into 231Pa, which reacts via a (n,)
reaction into 232Pa. This then decays to 232U. 233Pa reacts via (n,) into 234Pa, which
decays into 234U. 233U reacts via (n,2n) into 232U and reacts via (n,) into 234U. 235U is
produced by the (n,) reaction from 234U. This will decay by emitting an alpha particle
into 231Th, which follows the decay process written above.
232
U via
231
Th is shown below.[6]
1
0n
+ 232
90Th
231
90Th
1
0n
231
90Th
+ 231
91Pa
231
91Pa
232
91Pa
1
0n
+ 232
91Pa
+ 2 10n
232
92U
The probability of this neutron capture occurring depends on the cross sections of the
thorium isotopes and the velocity of the neutrons [16].
The other way to decay into
232
1
0n
U is by decaying into
+ 232
90Th
233
233
233
90Th 91Pa
232
U,
+ 10n
233
233
91Pa 92U
232
91Pa
+ 2 10n
232
92U
+ 2 10n
232
92U
233
Pa can also capture a neutron to turn into 232Pa, this depends on the cross section.
An overview of the production paths of 232U and its decay chain are shown in Figure 6.
n,2n
232 U
70
s
ar
s
ar
ye
1.
3
da
ys
10
6
ye
1.
231 Pa
+n
233 U
5
0
1
2.5
+n
27
da
ys
232 Pa
10
7
n,2n
229 Th
230 Th
n,2n
234 Pa
+n
22
231 Th
235 U
6.
7
ho
ur
s
233 Pa
1.
1
da
ys
228 Th
+n
234 U
232 Th
in
ut
es
+n
233 Th
1.9 years
224 Ra
,3.6d
0.24 MeV
224 Rn
,55s
0.54 MeV
216 Po
,0.15s
none
212 Pb
,10.6h
0.30 MeV
212 Bi
,60m
0.78 MeV
208 Tl
,3m
2.6 MeV
208 Pb
Stable
1.6
Radiological properties of
232
232
232
228
90Th (68.9 y)
224
88Ra (1.9 y)
220
86Rn (3.6 d, 0.24 MeV)
216
84Po (55 s, 0.54 MeV)
212
82Pb (0.15 s)
212
212
82Pb 83Bi
(10.64 h).
The statements in parentheses indicate the halflife and in case of gamma rays being
emitted the photon energy in electronvolt. In the above equations, the branching fraction
(the fraction of particles which decay by an individual decay mode with respect to the
212
83Bi
212
84Po
And into
208
81Tl
212
84Po
208
82Pb
212
83Bi
(61 m)
(0.30 s).
208
81Tl
208
208
81Tl 82Pb
(3 m, 2.6 MeV).
As seen above, intense gamma radiation is being produced in the decay of 208Tl, a decay
product of 232U. Since 232U and 233U cannot be chemically separated and it cannot be
prevented that 232U is produced in the thorium fuel cycle, these gamma rays may cause
difficulties in producing nuclear weapons with the acquired uranium [8].
1.7
Proliferation resistance
ratio of 232U to 233U will converge to the initial ratio of 232Pa to 233Pa and 234Pa. From
this, we can conclude that if the ratio of 232Pa to 233Pa is more than 5.0 ppm when
protactinium is separated from the reactor fuel, the ratio of 232U will also exceed the
threshold of 5.0 ppm.
11
Numerical Research
In this second part of the report, the proliferation resistance of the thorium fuelled reactor
is investigated by answering the question: How does the coproduction of 232U affect
the proliferation resistance of the thorium fuel cycle?. The analysis of the thorium fuel
cycle is done by developing a model in MATLAB, which calculates the amount of 232U
in 233U, 234U and 235U as well as the amount of 232Pa in 233Pa and 234Pa by looking at
the decay chain of thorium. The outcome will be compared to the maximum allowed
concentration of 232U mentioned in Section 1.7.
2.1
Model
In this section, a basic explanation of the model is given. The model adopts the general
ordinary differential equation (ODE) used in radioactive decay. In general the rate of
change of the number of a nucleus Ni depends on production terms and loss terms. This
gives the basic ODE of fuel depletion as used in the model
dNi
= j Nj + k Nk + yi f i Ni i Ni
{z
}
dt

{z
}
production
(2)
loss
with the decay constant, the neutron flux and the microscopic cross section. Nj is
the number of parent nuclei, which decay into Ni , and Nk is the number of nuclei which
can transform into Ni via neutron capture. f represents the total fission rate and yi is
the fraction of the fissions that produce Ni as one of the fission fragments [2].
The first term j Nj is the production of Ni via decay of the parent nucleus Nj . The term
k Nk is the neutron capture of another parent nucleus Nk . For completeness the term
yi f is included, which is the production of Ni isotope by fission. In the model none of
the nuclei are produced by fission, so this term is not used. The last two terms are the
loss of Ni via decay and neutron capture of Ni itself. An overview of the constants used
in the model can be found in Appendix B.
The model uses the decay chain shown in Figure 6. With this decay chain and Equation 2,
a set of differential equations is made to model the production of 232U in the thorium
fuel cycle. These ODEs are shown in Appendix A.
To solve these ODEs, they are written in matrixvector notation as
N = A N
12
(3)
dN1
dt
dN
dt2
N1
N
2
N :=
..
.
N := .
..
dNn
dt
Nn
A is a n n matrix with the relevant decay constants and microscopic cross sections. n
is the number of ODEs, in our case n = 14.
As an illustration of the elements ai,j , of the matrix A, the production rate of
used as an example. The ODE of 234U is
234
U is
dNU234
= Pa234 NPa234 + (n,),U233 NU233 U234 NU234 (n,)U234 NU234
dt
In the model 234U is the 8th nucleus, 234Pa the 7th and 233U the 9th . This gives
a8,7 = P a234 , a8,9 = U 233 and a8,8 = (U 234 + U 234 ). Furthermore a8,j = 0
for j 6= 7, 8, 9. The full numbering of the nuclei can be seen in the list of ODEs in
Appendix A.
MATLAB provides powerful numerical algorithms for solving first order differential
equations. One of these is the RungeKutta algorithm. The Matlab toolbox that provides
the implementation of this algorithm is called ode45. The basic syntax of ode45 as used
in the model is:
options = odeset(RelTol,1e8,AbsTol,1e8);
[t, N] = ode45(@(t,N)radiodecay(t,N,sc,s2n,lambda,phi),tspan,Nstart,options);
The input arguments of ode45 are formed by a function defining the ODE, a timespan
over which ode45 solves the ODE, a vector containing the initial values and a options
argument. ode45 can contain some numerical errors when used over a large timespan.
In order to reduce this error significantly, the odeset command is used. This sets a
maximum tolerance of error for ode45.
The function is called radiodecay, and implements Equation 3. radiodecay takes as
input arguments the time t; the number of nuclei N; a list sc; which contains the cross
sections for the neutron capture; a list s2n, which contains the cross sections for the
(n,2n) reactions; a list of decay constants lambda; and the neutron flux phi. The part
with @(t,N) is to make sure that ode45 interprets radiodecay as a Matlab function,
with t and N the input arguments in the context of ode45. The other arguments of
radiodecay are treated by ode45 as fixed parameters.
The output of ode45 is formed by t, which is a vector containing the times t(1), t(2),
. . . , t(p) at which Matlab has evaluated numerical solutions of N , and by a p n matrix
13
N containing the numerical solutions. Each element of this matrix contains the quantity
of nucleus Nn at time tp .
With this solution the evolution of the production of 232U and
can easily be plotted, as well as the fraction of 232U.
233
U as a function of time
2.2
Assumptions
Because creating a model that mimics reality is impossible, some assumptions had to be
made. These assumptions are made with to let the model simulate reality as closely as
possible. Only isotopes in the decay chain of 232Th that are relevant in calculating the
232
U ratio and 232Pa ratio are considered. Isotopes with a decay time of more than 10 000
years are not taken into consideration if the decay products are not isotopes of thorium,
protactinium or uranium. This includes 232Th, 231Pa, 233U, 234U and 235U. The halflife
and cross sections of 228Th, 229Th and 230Th are also not taken into account, because
the abundance and decay products of these isotopes do not affect the computed ratios.
This also includes the decay chain of 228Th as can be read in Section 1.6.
Since (n,2n) cross sections are generally small in comparison to (n,) cross sections,
(n,2n) cross sections are neglected if the isotope that is produced itself does not produce
a relevant uranium isotope or protactinium isotope. This is the case for 231Pa, 233U and
234
U. The decay of 233U, 234U and 235U could have been left out too because of the
exceptionally long halflife times, but since these do not result in technical difficulties,
they are left in. As for the decays, it is assumed the branching ratio of these decays
is 100% for the considered decay mode. Finally, it is assumed that the neutron flux in
the reactor is at a constant level, and no neutrons are captured or released in neutron
interactions.
2.3
Verification
Before confidence can be placed in the results, the model needs to be verified. This is
done by running the model with extreme values of cross sections and decayconstants
and checking the results. These verifications are tested with the standard neutron flux of
1 1013 s1 cm2 and with cross sections of the PWRMOX reactor.
The cross sections are changed first. In the first situation all cross sections of the (n,2n)
reactions are set to 0. Consequently, the only way to produce 232U is through the decay
of 235U to 231Th. The halflife of 235U is 7 108 yr which is a lot larger than the other
halflives so a small amount of 232U is expected to be created. This is indeed the case,
running the model with these parameters results 232U production not exceeding 1 109
ppm. Other isotopes which are not visible also not exceeding 1 109 ppm are: 231Th,
231
Pa, 232Pa, 228Th and 232U.
14
In the second situation, the cross section of 232Th is set to 0, meaning that the isotopes
233
Pa, 234Pa, 233U, 234U, 235U, 229Th and 230Th are not produced. This results in a large
concentration of 232U  the only visible isotope in the plot of the uranium isotopes (not
shown).
The model gives physically sensible results, as discovered by inputting extreme values
and comparing to expected physical behaviour.
2.4
Results
By running the model with different parameters, the abundances of thorium, protactinium
and uranium isotopes have been calculated for a period of 1 year, as well as the fraction of
232
U and 232Pa. A detailed explanation on the calculation and importance of these ratios
can be found in Section 1.7. The parameters that have been varied are the cross sections
and the neutron flux. Since no cross section data is available for a MSR or a MSFR, the
model has been run for cross sections of two different types of nuclear reactors, namely a
pressurized water reactor (PWR) and liquid metal cooled reactor (LMR). The difference
between these reactor types is the neutron energy. In a PWR, thermal neutrons initiate
neutron interactions, whereas in an LMR these interactions are initiated by fast neutrons.
Since the cross sections depend on neutron energy, the cross sections from these reactors
differ, as shown in Appendix B. The cross sections for a MSR and a MSFR are expected
to be somewhere in between. For a MSR, those are expected to approach those of an
PWR and for a MSFR, those are expected to approach those of an LMR.
Additionally, the neutron flux has been varied, because the actual value is unknown. The
typical neutron flux in a nuclear reactor is 1 1012 n s1 cm2 to 1 1014 n s1 cm2 .
Here the bold n denotes the number of neutrons.
Below, for each of combination of these parameters, a graph of the fraction of 232U and a
graph of the fraction of 232Pa is shown. These graphs are shown to compare the fractions
to the literature as stated in Section 1.7. Since the reactor fuel is irradiated with neutrons
for a few months to one year, the time span is chosen to be one year.
15
Fraction of elements
101
Th
Pa
U
233
U
232
U
103
107
1011
1015
100
200
Time [d]
300
400
Figure 7. The change in the proportion of all isotopes for the duration of a year for a neutron
flux of 1 1012 n s1 cm2 with PWRMOX cross sections.
In Figure 7 a plot of how the proportion of isotopes changes as a whole for a neutron
flux of 1 1012 n s1 cm2 is shown. The cross sections have been chosen to be those for
PWRMOX fuel.
Fraction of elements
104
Pa
U
233
U
232
U
106
108
1010
1012
1014
0
100
200
Time [d]
300
400
Figure 8. The change in the proportion of all uranium and protactinium isotopes for the duration
of a year for a neutron flux of 1 1012 n s1 cm2 with PWRMOX cross sections.
In Figure 8 a plot of how the proportion of isotopes except for thorium changes as a
whole for a neutron flux of 1 1012 n s1 cm2 is shown. The cross sections have been
chosen to be those for PWRMOX fuel. Thorium has been left out since the abundances
of 231Th, 232Th and 233Th remain almost constant and the abundances of 228Th, 229Th
16
and
230
Pa, [ppm]
OX
M
0.5
OX
LMRM
0
100
200
Time, [d]
232
300
233
U to
0.1
PW
232
RPW
Fraction of
Fraction of
232
U, [ppm]
1.5
U,
5 102
OX
LMRM
0
400
234
OX
M
R
100
232
200
Time, [d]
233
Pa to
300
400
Pa
Figure 9. For a neutron flux of 1 1012 n s1 cm2 and a duration of one year, with cross sections
for LMRMOX and PMRMOX.
For a neutron flux of 1 1012 n s1 cm2 , with PWRMOX cross sections, the fraction of
232
U is 1.55 ppm and the fraction of 232Pa is 0.13 ppm after one year, with LMRMOX
cross sections, the fraction of 232U is 0.31 ppm and the fraction of 232Pa is 0.026 ppm
after one year as shown in Figure 9.
Pa, [ppm]
OX
R
LMRM
0
100
200
Time, [d]
232
U to
OX
M
R
PW
232
PW
10
Fraction of
Fraction of
232
U, [ppm]
15
OX
300
233
U,
400
234
0.5
OX
LMRM
0
100
200
Time, [d]
232
Pa to
300
233
400
Pa and
Figure 10. For a neutron flux of 1 1013 n s1 cm2 and a duration of one year, with cross
sections for LMRMOX and PMRMOX.
For a neutron flux of 1 1013 n s1 cm2 , with PWRMOX cross secions, the fraction of
232
U exceeds 5.0 ppm in 84 days and after one year, fraction of 232Pa is 1.29 ppm. With
LMRMOX cross sections, after one year, the fraction 232U is 3.09 ppm and the fraction
17
of
232
Pa, [ppm]
OX
M
R
232
PW
100
Fraction of
Fraction of
232
U, [ppm]
150
50
OX
LMRM
0
100
200
Time, [d]
232
U to
300
233
U,
400
234
12
OX
10
M
R
PW
8
6
4
OX
LMRM
2
0
100
200
Time, [d]
232
Pa to
300
233
400
Pa and
Figure 11. For a neutron flux of 1 1014 n s1 cm2 and a duration of one year, with cross
sections for LMRMOX and PMRMOX.
For a neutron flux of 1 1014 n s1 cm2 , with PWRMOX cross sections, the fraction
of 232U exceeds 5.0 ppm in 3.4 days and the fraction of 232Pa exceeds 5.0 ppm in 143
days. With LMRMOX cross sections, the fraction of 232U exceeds 5.0 ppm in 21 days
and after one year, the fraction of 232Pa is 2.54 ppm as shown in Figure 11.
18
3
3.1
Analysis
Discussion & Conclusion
From these results, we can draw the following conclusions for a MSR, assuming the cross
sections approach those of PWRMOX fuel and for a MSFR, assuming the cross sections
approach those of LMRMOX fuel.
At a neutron flux of 1 1012 n s1 cm2 , after one year the ratio of 232U is 1.55 ppm in
a MSR, 0.31 ppm in a MSFR, the ratio of 232Pa is 0.13 ppm in MSR and 0.026 ppm in a
MSFR.
At a neutron flux of 1 1013 n s1 cm2 , in a MSR the ratio of 232U exceeds 5.0 ppm
after 84 days. However in a MSFR, after one year the ratio of 232U is just 3.09 ppm.
After one year, the ratio of 232Pa is 1.29 ppm in a MSR and 0.25 ppm in a MSFR.
At a neutron flux of 1 1014 n s1 cm2 , in a MSR the ratio of 232U exceeds 5.0 ppm
after 3.4 days and in a MSFR this ratio exceeds 5.0 ppm after 21 days. The ratio of
232
Pa exceeds 5.0 ppm after 143 days in a MSR and after one year, this ratio is 2.54 ppm
in a MSFR.
This indicates that neither a MSR nor a MSFR is proliferation resistant for a neutron
flux of 1 1012 n s1 cm2 . Over the full cross section range both fractions do not
exceed 5.0 ppm within one year. A MSR and a MSFR are also not proliferation resistant
for a neutron flux of 1 1013 n s1 cm2 , because over the full cross section range the
fraction of 232Pa does not exceed 5.0 ppm within one year. Finally, for a neutron flux
of 1 1014 n s1 cm2 , a MSR may or may not be proliferation resistant and a MSFR
is not proliferation resistant. In a MSR, the fraction of 232U exceeds 5.0 ppm within 21
days, but the fraction of 232Pa exceeds 5.0 ppm after 143 days. In a MSFR, the fraction
of 232Pa is just 2.54 ppm after one year.
The results have been obtained with a degree of confidence, since the model has been
verified. The results seem plausible for the fact that it was expected that the fractions
of 232Pa and 232U increase with time. Besides, the total abundances of all isotopes sum
up to the starting value of 232Th and remains constant. The assumptions do not have
a significant impact and the numerical error is very small. The only issue is that it
is impossible to compare the results to results of other research. Since no exact cross
sections for a MSR and a MSFR are available, these had to be approached by cross
sections for other nuclear reactors. Consequently, the results are an approach of the
reality. In the best case scenario it takes at least 143 days until both ratios exceed
5.0 ppm in a MSR. This is a relatively long time; long enough to conclude the MSR is
not proliferation resistant, mainly due to the possibility to separate protactinium from
the reactor fuel before the ratio of 232Pa reaches 5.0 ppm. In a MSFR, only 2.54 ppm
232
Pa is accumulated after one year in the best case scenario. Therefore, we can conclude
a MSFR is not proliferation resistant.
19
3.2
Recommendations
First of all, more research into the exact cross sections of a MSR and a MSFR has
to be conducted before conclusions about its proliferation resistance can be drawn.
Experimental verification of the cross sections is only possible when a molten salt reactor
or a close substitute is built. However, once this is built the proliferation resistance can
directly be determined by measuring the proportion of 232U.
In order to make a MSR or a MSFR proliferation resistant, another design of the breeding
blanket with a higher neutron flux is needed. This higher neutron flux will accelerate
232
U production. It is recommended to use a lowenergy neutron spectrum, such as the
thermal neutron spectrum.
Finally, another way to make a MSR proliferation resistant, is to design the reactor
in a way that inhibits the separation of protactinium. The obtained results show the
concentration of 232Pa in the reactor fuel is always lower than the concentration of 232U
and therefore this is the limiting factor in designing a proliferation resistant nuclear
reactor. A MSR of this design will be proliferation resistant at the expected neutron flux
of 1 1014 n s1 cm2 .
20
References
[1]
[2]
[3]
[4]
[5]
[6]
[7]
[8]
[9]
[10]
[11]
[12]
[13]
[14]
[15]
[16]
21
ODE system
1
2
3
4
5
6
7
8
9
10
11
12
13
14
dNTh232
dt
dNTh233
dt
dNTh231
dt
dNPa233
dt
dNPa231
dt
dNPa232
dt
dNPa234
dt
dNU234
dt
dNU233
dt
dNU232
dt
dNU235
dt
dNTh228
dt
dNTh229
dt
dNTh230
dt
= Th232 NTh232
= Th232 NTh232 Th233 NTh233
= U235 NU235 + Th232 NTh232 Th231 NTh231
= Th233 NTh233 Pa233 NPa233 Pa233 NPa233
= Th231 NTh231 Pa231 NPa231
= Pa231 NPa231 + Pa233 NPa233 U232 NU232
= Pa233 NPa233 Pa234 NPa234
= Pa234 NPa234 + U233 NU233 U234 NU234 U234 NU234
= Pa233 NPa233 U233 NU233 U233 NU233
= Pa232 NPa232 + U233 NU233 U232 NU232
= U234 NU234 U235 NU235
= U232 NU232
= U233 NU233
= U234 NU234
22
Data Model
In Table 1 all relevant data for the model is shown, including halflives [14], (n,) cross sections and (n,2n) cross sections for PWRMOX fuel and LMRMOX fuel, respectively [11].
The MSR cross sections are expected to be somewhere in between. Note that Table 1 only
contains data used in the model, not all data concerning the isotopes. See Section 2.2 for
more details.
Table 1. Relevant halflives, (n,) cross sections and (n,2n) cross sections for PWRMOX fuel
and LMRMOX fuel.
Isotope
t1
Th228
Th229
Th230
Th231
Th232
Th233
Pa231
Pa232
Pa233
Pa234
U232
U233
U234
U235
1.1 d
22 m
1.3 d
27 d
6.7 h
70 yr
1.6105 yr
2.5105 yr
7.0108 yr
PWRMOX
n, (b)
2.6889
25.6550
21.2970
3.8628
16.5080

23
n,2n (mb)
8.9617
2.4558
4.5238

LMRMOX
n, (b)
0.3958
2.9801
1.0564
0.2610
0.6015

n,2n (mb)
2.2377
0.6121
1.1373

C
1
2
3
4
5
6
MATLAB Code
%% UNIT CONVERSION
day = 1;
year = 365.25*day;
hour = day/24;
minute = hour/60;
second = minute/60;
7
8
9
%% PARAMETERS
10
11
12
% Reactor type
Type = PWR; % MOX, to select cross sections
13
14
15
16
17
18
19
20
21
22
23
% Cross sections
if strcmp(Type,PWR) % PWRMOX type
% Capture [m^2]
sc = 1e28*[2.6889 1 1 21.2970 25.6550 1 1 16.5080 3.8628 1 1 1 1 1];
24
% n,2n [m^2]
s2n = 1e28*1e3*[8.9617 1 1 2.4558 1 1 1 1 4.5238 1 1 1 1 1];
25
26
27
end
28
29
30
31
32
% n,2n [m^2]
s2n = 1e28*1e3*[2.2377 1 1 0.6121 1 1 1 1 1.1373 1 1 1 1 1];
33
34
35
end
36
37
38
% Time span
tspan = [0 year];
39
40
41
42
43
44
%% SOLVE ODE
45
24
46
47
options = odeset(RelTol,1e8,AbsTol,1e8);
[t, N] = ode45(@(t,N)radiodecay(t,N,sc,s2n,lambda,phi),tspan,Nstart,options);
48
49
N = N/1e10; % Normalization
50
51
52
53
54
55
%% Fractions
56
57
58
59
60
61
62
63
64
%% PLOT
65
66
67
68
69
70
71
72
73
74
75
76
77
78
79
80
81
82
83
84
85
86
87
88
89
90
91
92
25
93
94
95
96
97
98
99
100
101
102
103
104
105
106
107
108
109
110
111
112
113
114
115
116
117
118
119
120
121
122
123
124
125
126
% Fractions to ppm
FracU = 1e6*FracU;
FracPa = 1e6*FracPa;
127
128
129
130
131
132
133
134
135
136
137
138
139
140
141
26
142
143
xlabel($t$ (d),Interpreter,latex)
ylabel($Fraction$ (ppm),Interpreter,latex)
144
145
146
%% Critical ppm
147
148
149
150
151
152
153
154
155
156
157
158
159
160
161
162
163
164
27
1
2
3
4
5
6
7
8
9
10
11
12
13
14
15
16
17
18
19
20
21
22
23
24
25
26
27
28
29
30
31
function dN = radiodecay(t,N,sc,s2n,lambda,phi)
%% DECAY MATRIX
A = zeros(14);
A(1,1) =
(sc(1)+s2n(1))*phi;
A(2,1) =
sc(1)*phi;
A(2,2) = lambda(2);
A(3,1) =
s2n(1)
*phi;
A(3,3) = lambda(3);
A(4,2) = lambda(2);
A(4,4) = lambda(4)
(sc(4)+s2n(4))*phi;
A(5,3) = lambda(3);
A(5,5) =
sc(5)*phi;
A(6,4) =
s2n(4)*phi;
A(6,5) =
sc(5)*phi;
A(6,6) = lambda(6);
A(7,4) =
sc(4)*phi;
A(7,7) = lambda(7);
A(8,7) = lambda(7);
A(8,8) = lambda(8)
sc(8)*phi; %
A(8,9) =
sc(9)*phi;
A(9,4) = lambda(4);
A(9,9) = lambda(9)
(sc(9)+s2n(9))*phi; %
A(10,6) = lambda(6);
A(10,9) =
s2n(9)*phi;
A(10,10) = lambda(10);
A(11,11) = lambda(11);
A(11,8) =
sc(8)*phi;
A(3,11) = lambda(11);
A(12,10) = lambda(10);
A(13,9) = lambda(9);
A(14,8) = lambda(8);
32
33
34
35
%% Differential equation
dN = A*N;
end
28
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