Nuclear Engineering and Design 313 (2017) 53–72

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Nuclear Engineering and Design

journal homepage: www.elsevier.com/locate/nucengdes

Target fuels for plutonium and minor actinide transmutation in

pressurized water reactors
J. Washington a, J. King a,⇑, Z. Shayer b
a
Nuclear Science and Engineering Program, Colorado School of Mines, 1500 Illinois St., Golden, CO 80401, USA
b
Department of Physics, Colorado School of Mines, 1500 Illinois St., Golden, CO 80401, USA

h i g h l i g h t s g r a p h i c a l a b s t r a c t

 We evaluate transmutation fuels for

plutonium and minor actinide
destruction in LWRs.
 We model a modified AP1000 fuel
assembly in SCALE6.1.
 We evaluate spectral shift absorber
coatings to improve transmutation
performance.

a r t i c l e i n f o a b s t r a c t

Article history: The average nuclear power plant produces twenty metric tons of used nuclear fuel per year, containing
Received 7 May 2016 approximately 95 wt% uranium, 1 wt% plutonium, and 4 wt% fission products and transuranic elements.
Received in revised form 23 November 2016 Fast reactors are a preferred option for the transmutation of plutonium and minor actinides; however, an
Accepted 28 November 2016
optimistic deployment time of at least 20 years indicates a need for a nearer-term solution. This study
Available online 18 December 2016
considers a method for plutonium and minor actinide transmutation in existing light water reactors
and evaluates a variety of transmutation fuels to provide a common basis for comparison and to deter-
mine if any single target fuel provides superior transmutation properties. A model developed using the
NEWT module in the SCALE 6.1 code package provided performance data for the burnup of the target fuel
rods in the present study. The target fuels (MOX, PuO2, Pu3Si2, PuN, PuUZrH, PuZrH, PuZrHTh, and PuZrO2)
are evaluated over a 1400 Effective Full Power Days (EFPD) interval to ensure each assembly remained
critical over the entire burnup period. The MOX (5 wt% PuO2), Pu0.31ZrH1.6Th1.08, and PuZrO2MgO (8 wt
% Pu) fuels result in the highest rate of plutonium transmutation with the lowest rate of curium-244 pro-
duction. This study selected eleven different burnable absorbers (B4C, CdO, Dy2O3, Er2O3, Eu2O3, Gd2O3,
HfO2, In2O3, Lu2O3, Sm2O3, and TaC) for evaluation as spectral shift absorber coatings on the outside of
the fuel pellets to determine if an absorber coating can improve the transmutation properties of the tar-
get fuels. The PuZrO2MgO (8 wt% Pu) target fuel with a coating of Lu2O3 resulted in the highest rate of
plutonium transmutation with the greatest reduction in curium-244 production.
Ó 2016 Elsevier B.V. All rights reserved.

1. Introduction

The average nuclear power plant produces twenty metric tons

of used nuclear fuel per year, containing approximately 95 wt%
⇑ Corresponding author.
uranium, 1 wt% plutonium, and 4 wt% fission products and
E-mail addresses: jwashing@gmail.com (J. Washington), kingjc@mines.edu
(J. King), zshayer@mines.edu (Z. Shayer).
transuranic elements (Bruno and Ewing, 2006). The transuranic

http://dx.doi.org/10.1016/j.nucengdes.2016.11.033
0029-5493/Ó 2016 Elsevier B.V. All rights reserved.
54 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72
elements contained within this used fuel produce 33% of the total
activity remaining after 20 years of cooling (Department of Energy,
2002). Since 90–100% of the residual heat produced by used fuel
after the first sixty years originates from the radioactive decay of
the actinides (specifically plutonium and americium), the design
basis lifetime of storage or disposal facilities could be greatly
reduced if the actinide components of used fuel did not require
storage or disposal (Wigeland et al., 2006).
Radiotoxicity is a measure of a radioactive substance’s ability to
do damage to a person through radiation emitted inside of a body
(International Standard, 1999). Radiotoxicity is calculated as the
mass sum of a set of radionuclides each multiplied by a dose con-
version factor, and is one of the factors which is considered during
the storage and disposal of radioactive materials (Piet, 2013). One
of the ways to reduce the requirements for a storage or disposal
facility is to recycle and fission the plutonium from used LWR fuel,
which can reduce the radiotoxicity of the fuel by a factor of up to
ten (Salvatores, 2004). The removal or fission of the minor acti-
nides from used fuel can further reduce the radiotoxicity of the
residual used fuel by up to a factor of one hundred (Salvatores,
2004). The fission of these actinide products can be accomplished
in nuclear reactors, in particle accelerators, or by simply letting
radioactive decay occur.
The potential for plutonium refinement from used fuel causes
concern from a nuclear weapons proliferation standpoint
(Peryoga et al., 2005). Although plutonium may be used for nuclear
weapons, it is also a potential source of fissile fuel for nuclear reac-
tors, resulting in a more efficient neutron economy than uranium
or thorium in a reactor environment (Duderstadt and Hamilton,
1976). The combined separation of plutonium and minor actinides
(americium, curium, and neptunium) from the uranium and fission
products in used fuel improves proliferation resistance compared
to the extraction of plutonium alone, as the combination of minor
actinides and plutonium requires additional refinement before the
plutonium can be used for a fissile nuclear weapon (Chang, 2009;
Sahin et al., 2009). The combination of plutonium and minor acti-
nides can be fabricated into a transmutation fuel with reduced pro-
liferation risks compared to pure plutonium fuel (Chang, 2009).
Fast reactors are generally a preferred option for the transmuta-
tion of plutonium and minor actinides; however, an optimistic
deployment time of at least 20 years indicates a need for a
nearer-term solution (Salvatores and Palmiotti, 2011). As an
interim solution to the nuclear waste problem, this study assesses
the feasibility of incorporating plutonium and minor actinide bear-
ing target fuel rods into existing Pressurized light Water Reactor
(PWR) fuel elements, in order to reduce the stockpile of these
materials. To determine if it is reasonable to use current or
advanced LWR technology to transmute actinides, various fuel
types and configurations are evaluated with respect to their trans-
mutation properties. The evaluation is performed using the West-
inghouse AP1000 17  17 XL Robust Fuel Assembly design
(described in Section 3), which is representative of the numerous
operating PWRs in the United States. This evaluation considers pri-
marily the transmutation of plutonium and secondarily the trans-
mutation of minor actinides in a twice-through fuel cycle. The
objective of this study is to reduce the quantity of plutonium while
minimizing the production of minor actinides to improve reposi-
tory performance (Kessler, 2002).
This paper provides an overview of sixteen fuels, with and with-
out initial minor actinides, as potential transmutation target fuels.
The fuels evaluated in this study represent the spectrum of fuels
used in other studies for transmutation purposes. These target
fuels are placed in the central instrumentation channel of an
AP1000 Robust Fuel Assembly to provide similar simulation condi-
tions for each fuel. The target fuels with initial minor actinides are
simulated by replacing a portion of the plutonium in the fuel with
a mixture of minor actinides that would be present in reprocessed
used fuel rods. For the purposes of this study, the minor actinides
consist of neptunium, americium, and curium.
The three target fuels with the most significant plutonium and
minor actinide transmutation rates are also evaluated with a spec-
tral shift coating. A spectral shift coating is a material which
absorbs neutrons of a specific energy window, thereby adjusting
the overall neutron energy spectrum seen by the underlying mate-
rial, in this case, a target fuel. Spectral shift absorbers may be used
to shift the effective neutron energy spectrum of a reactor core by
increasing the absorption of neutrons in a certain energy range, at
the penalty of decreasing the overall flux (Duderstadt and
Hamilton, 1976). A spectral shift absorber with a high cross-
section in a specific energy range will tend to remove neutrons
of that energy from the system (Duderstadt and Hamilton, 1976;
Trellue, 2006; Tsvetkov et al., 2008). The removal of these neutrons
from the energy spectrum results in a ‘‘shift” towards the energy
ranges which are less affected by the burnable absorber
(Duderstadt and Hamilton, 1976; Trellue, 2006; Tsvetkov et al.,
2008). Fuel choice may also be used to shift the neutron energy
spectrum, as transuranic fueled systems tend to exhibit a spectral
shift towards a harder neutron spectrum compared to uranium
fueled systems (Trellue, 2006; Tsvetkov et al., 2008). Spectral shift
absorbers are used in this study to provide a method to increase
the relative amount of fast flux seen by the target fuels in an
attempt to mimic a fast reactor environment. Eleven different
spectral shift coatings are evaluated to determine if the application
of these materials on the target fuels will increase the rate of acti-
nide transmutation.
2. Background
Previous studies have considered these fuels for either pluto-
nium transmutation alone or a combination of plutonium and
minor actinide transmutation. A brief overview of the AP1000
Robust Fuel Assembly is included as it serves as the basis for the
models used in the present study.
The use of plutonium fuel in light water reactors may be consid-
ered as a partial solution for used nuclear fuel disposition, and as
an alternative to vitrification and disposal (Galperin, 1995). Pluto-
nium may be retrieved from used nuclear fuel through a standard
PUREX reprocessing method which can separate uranium and plu-
tonium from used fuel and provides the source material for recy-
cled or transmutation fuel (Özdemir et al., 2011). Though
reprocessing used nuclear fuel for the purposes of plutonium
extraction poses a proliferation risk, the ratio of even numbered
plutonium isotopes to odd numbered isotopes in the used fuel
can mitigate this risk (Peryoga et al., 2005; Sagara et al., 2005). A
quantity of plutonium-238 is especially useful as a large source
of thermal energy which makes handling the fuel more difficult
(Chang, 2009; Peryoga et al., 2005; Sagara et al., 2005). Studies
have shown that an addition of plutonium-238 which is 5 wt% of
the total mass of plutonium can prevent the use of a bare pluto-
nium sphere for explosives development (Peryoga et al., 2005).
The IAEA considers any plutonium which contains 80 wt% or more
of plutonium-238 to be exempt from proliferation concerns
(Peryoga et al., 2005). The inclusion of minor actinides in pluto-
nium fuel also increases the proliferation resistance of the repro-
cessed fuels by diluting the plutonium as well as providing
additional heat generation from americium-241 (Chang, 2009;
Peryoga et al., 2005; Ronen et al., 2010; Sagara et al., 2005).
Currently, Mixed OXide (MOX) fuel is the only transmutation
fuel commonly used in LWRs (Galperin, 1995). Though MOX fuel
may be useful in existing PWR reactors in the United States, it is
only routinely used in reactors in other countries (Trellue, 2006).
 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72
While MOX is the only transmutation fuel currently used in exist-
ing nuclear reactors, a variety of other transmutation fuels have
been evaluated in nuclear reactor simulations by an equal variety
of authors. Many of the previous studies contrast the transmuta-
tion fuels with MOX as a comparison to a real world transmutation
fuel. The following sub-sections discuss these other transmutation
fuels.
2.1. Candidate fuels
Various configurations of MOX fuel have been evaluated for use
in LWRs (Galperin, 1995; Kessler, G., 2002). MOX usually has a plu-
tonium content of less than 12 wt%, typically 5–8 wt% (Trellue,
2006). The plutonium ratios in MOX fuel vary depending on the
initial uranium enrichment, reactor type, and the fuel’s discharge
burnup (Bairiot et al., 1991; Fridman and Kliem, 2011; Özdemir
et al., 2011). Although MOX fuel is the only transmutation fuel cur-
rently used in nuclear reactors, it is not the only fuel undergoing
research nor is it without potential problems. One problem with
MOX fuel is the production of additional plutonium from the ura-
nium portion of the fuel during irradiation (Fetterman, 2009;
Fridman and Kliem, 2011). Replacing the uranium oxide portion
of MOX fuel with thorium oxide eliminates the generation of addi-
tional plutonium (Fridman and Kliem, 2011). The use of thorium
MOX fuels would require a higher initial fissile loading when com-
pared to uranium MOX fuels but would result in a higher pluto-
nium transmutation rate (Fridman and Kliem, 2011; Galperin,
1995). An evaluation of thorium MOX fuel in a conventional West-
inghouse PWR, compared to both standard uranium oxide and
MOX fuels, indicated transuranic transmutation rates which were
a factor of 1.5 higher than a standard MOX core (Fridman and
Kliem, 2011). The thorium MOX fuel produced a significant quan-
tity of uranium-233, but resulted in the destruction of nearly sixty
percent of the initial plutonium in the fuel (Fridman and Kliem,
2011).
A plutonium uranium zirconium hydride fuel (PUZH) was com-
pared to MOX fuels in an AP1000 PWR core (Ganda, 2008; Ganda
and Greenspan, 2009; Greenspan et al., 2009). Varying the pitch
to diameter ratio of these two fuels produced a maximum burnup
of 75 GWd/tHM for MOX and 125 GWd/tHM for PUZH (Ganda,
2008; Ganda and Greenspan, 2009; Greenspan et al., 2009). The
optimum pitch to diameter ratio was smaller for the PUZH fuel
than for the MOX fuel, 1.5–1.7 compared to 1.7–1.9, respectively,
due to the increased quantity of hydrogen and the lower inventory
of initial heavy metals in the PUZH fuel (Ganda, 2008; Ganda and
Greenspan, 2009; Greenspan et al., 2009). The PUZH fuel produced
a quantity of neptunium-237, americium-243, and curium-245
which was 39 wt% smaller than that produced by the MOX fuel
while transmuting approximately 53 wt% of the initial plutonium
(Ganda, 2008; Ganda and Greenspan, 2009; Greenspan et al.,
2009). The highest rate of plutonium transmutation, 57.7 wt%,
was achieved with PUZH fuel with a pitch to diameter ratio of
1.7 (Ganda, 2008; Ganda and Greenspan, 2009; Greenspan et al.,
2009). The optimized configuration of the theoretical PWR core
fueled with PUZH produced approximately twice the plutonium
transmutation of MOX in a similar configuration (115 GWd/tHM
vs 55 GWd/tHM) (Ganda, 2008; Ganda and Greenspan, 2009;
Greenspan et al., 2009).
Plutonium thorium hydride fuels were evaluated with respect
to their performance as transmutation fuels with a range of tho-
rium hydride fractions (Ganda, 2008; Greenspan et al., 2009). Tho-
rium hydride replaced various fractions of the zirconium hydride,
from zero to one hundred percent, to determine if the addition of
thorium hydride improved the plutonium transmutation rates in
the fuel (Ganda, 2008; Greenspan et al., 2009). The higher volume
fractions of thorium hydride in the plutonium thorium zirconium
55
hydride fuels resulted in correspondingly higher fractions of trans-
uranic transmutation (Ganda, 2008; Greenspan et al., 2009). A
thorium-free plutonium zirconium hydride fuel achieved a trans-
uranic destruction of nearly 64 wt% and the zirconium-free, pluto-
nium thorium hydride fuel transmuted nearly 36 wt% of its initial
transuranic content (Ganda, 2008; Greenspan et al., 2009).
Plutonium zirconium hydride (PuZrH) was evaluated with a
neptunium hydride fraction replacing the fertile thorium hydride
component contrasting the effectiveness of the fuel with and with-
out thorium hydride (Ganda, 2008; Greenspan et al., 2009). This
fuel type provides higher transuranic destruction ratios compared
to PUZH or thorium plutonium zirconium hydride fuel (Ganda,
2008; Greenspan et al., 2009). In comparison with MOX fuel, at
comparable conditions, PuZrH results in a lower quantity of fissile
plutonium isotopes, 22 wt% for PuZrH compared to 25 wt% for
MOX (Ganda, 2008; Greenspan et al., 2009). The uranium-free
hydride allows for multiple recycles of plutonium in PWRs
(Ganda, 2008; Greenspan et al., 2009). As a recyclable fuel, PuZrH
results in a plutonium transmutation rate of 64 wt% for the first
recycle, which reaches an equilibrium rate of 20 wt% after multiple
recycles (Ganda, 2008; Greenspan et al., 2009).
Another method for the transmutation of plutonium makes use
of inert matrix oxide fuels, such as PuO2-ThO2-Al2O3-MgO and
PuO2-ZrO2(Y,Gd)-Al2O3-MgO, rather than uranium oxide contain-
ing fuels (Akie et al., 1995). A uranium-free inert matrix fuel can
result in up to 2.5 times the destruction of plutonium when com-
pared with MOX fuel, primarily due to the lack of plutonium gen-
eration (Lombardi et al., 2008). A two-dimensional core calculation
predicted the transmutation of 83 wt% of the total plutonium in a
plutonium inert matrix fuel, PuO2-ZrO2(Y,Gd)-Al2O3-MgO, during a
1400 day irradiation period (Akie et al., 1995).
Each of the fuel types mentioned in this section was evaluated
under different simulation conditions. A detailed comparison
requires these fuels to be simulated under similar conditions. The
fuel assembly for the AP1000 PWR was selected as a representative
system for this comparison because it is a modern fuel design for
current generation pressurized water reactors.
2.2. Robust fuel assembly
The Westinghouse Advanced Passive PWR (AP1000) is an itera-
tive design based on the AP600 (Westinghouse, 2003). The AP1000
design operates at 3400 MWth and contains 157 XL Robust fuel
assemblies (Westinghouse, 2011). The XL Robust fuel assembly
design evolved from the Robust fuel assembly and from the VAN-
TAGE+, VANTAGE 5, and VANTAGE 5 HYBRID designs
(Westinghouse, 2011). The AP1000 XL Robust fuel assemblies have
an active fuel length of 4.27 m but also employ four of the interme-
diate flow mixing grids found in the Robust fuel assembly
(Westinghouse, 2011). The XL Robust fuel assembly is arranged
in a 17 by 17 grid with 264 fuel rod positions, 24 guide thimbles
for control rods, and one central guide thimble for core instrumen-
tation (see Fig. 2.1) (Westinghouse, 2011). The fuel rods are filled
with uranium oxide fuel pellets at 95.5% of theoretical density with
2.35, 3.40, or 4.45 wt% enrichment depending on the location of
the assembly within the core (Westinghouse, 2011). The UO2 fuel
pellets are 0.98 cm (0.387 in.) in length with a diameter of
0.82 cm (0.3225 in.) (Westinghouse, 2011). The gap between the
fuel pellet and cladding is 0.02 cm (0.0065 in.) in length. The clad-
ding is composed of ZIRLOTM and has a thickness of 0.06 cm
(0.0225 in.) (Westinghouse, 2011). The fuel rods are pitched at
1.26 cm (0.496 in.) and a full reactor core contains 41448 fuel rods
for a UO2 weight of 95.97 metric tons. The design control docu-
ment for the AP1000 provided the parameters to develop the
model of the Westinghouse robust fuel assembly use in the present
study (Westinghouse, 2011).
56 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72
Fig. 2.1. AP1000 robust fuel assembly layout.
3. Model
A model developed using the NEWT module of the SCALE 6.1
reactor analysis package provided performance data for the burnup
of the target fuel rods in the present study (Chadwick et al., 2006;
Oak Ridge National Laboratory, 2011). The NEWT model is a two-
dimensional, discrete-ordinate, reflected model using 16th order
symmetric quadrature. The model included each ZIRLOTM clad tar-
get fuel rod in the central channel of an AP1000 17  17 XL Robust
Fuel Assembly. The remaining fuel rods each contain 3 wt% (wt%)
enriched uranium dioxide fuel (Schulz, 2006; Westinghouse
Electric Corp et al., 1992). The model uses the prepackaged
ENDF/B-VII.0 cross-section libraries for all simulations.
Table 3.1. lists the dimensions of the fuel assembly and compo-
nents included in the model shown in Fig. 3.1. The radius of the
fuel pellets is 0.410 cm with a gap thickness of 0.017 cm, a ZIRLOTM
cladding thickness of 0.057 cm, and fuel rod pitch of 1.260 cm
(Schulz, 2006). A standard 17  17 XL Robust Fuel Assembly is
21.417 cm on a side and contains 264 fuel rods with 24 control
rod channels and one central instrumentation channel (Schulz,
2006). The simulations were performed at 293.5 K for all materials.
The water moderator did not contain chemical shim. In this study,
the target fuel rod replaces the central instrumentation channel.
Table 3.2 presents the target fuel compositions without minor
actinides at Beginning of Life (BOL). Several target fuels were
Table 3.1
AP1000 Robust fuel assembly parameters used in the present study (Schulz, 2006).
Component Parameter
Fuel pellet 0.410 cm radius
Gap thickness 0.017 cm radius
Clad thickness 0.057 cm radius
Fuel rod pitch 1.260 cm
Assembly pitch 21.417 cm
Assembly thermal power 21.66 MW
simulated at very high initial plutonium concentrations for the
purpose of determining trends. Table 3.3 presents the isotopic con-
centrations of the plutonium used in the present study; Table 3.4
presents the target fuel compositions with minor actinides at
BOL. The fuel types selected for evaluation cover a spectrum of
the fuel types discussed in Section 2.1.
A fraction of the plutonium in the minor actinide bearing fuels
is replaced by the minor actinides (americium, curium, and neptu-
nium), based on isotope ratios determined for an average PWR fuel
assembly with a burnup of 41200 MWd/MTHM at 3.75 wt% enrich-
ment after 23 years of decay (Department of Energy, 2002).
Table 3.5 shows the isotopic ratios, as weight percent, used to
determine the composition of the minor actinide containing target
fuels. Comparing these transmutation fuels with each other will
reveal if any one fuel type has inherent properties which would
make it a superior transmutation fuel. A comprehensive evaluation
of the potential transmutation fuels using a common methodology
will also provide a basis for cross-comparison. The current quantity
of plutonium and minor actinides added to the assembly is not
expected to have a significant impact on the neutronic perfor-
mance of the assembly.
The NEWT sequence employed the prepackaged 238 group
ENDF/B-VII.0 cross-section library with a 34 by 34 global grid
and a 20 by 20 local grid over the target fuel rod. The model
employed a reflective assembly boundary condition. The burnup
Composition Density
3 wt% enriched uranium oxide 10.96 g/cm3
Vacuum 0 g/cm3
1.25 wt% Nb, 1.1 wt% Sn, 0.105 wt% Fe, 0.055 wt% Ni, 0.055 wt% Cr, 6.56 g/cm3
0.00022 wt% C, 97.43 wt% Zr
 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72 57

Fig. 3.1. SCALE 6.1 AP1000 assembly model with a central transmutation fuel rod.

Table 3.2
Target fuel composition without minor actinides at beginning of lifetime.

Fuel Constituents (wt%)

232
Th U Pud O Zr H Y/Mg
a,c
MOX (5% PuO2) 0.00 83.72 4.43 11.86 0.00 0.00 0.00
MOX (7% PuO2)a,c 0.00 81.93 6.21 11.86 0.00 0.00 0.00
MOX (10% PuO2)a,c 0.00 79.27 8.86 11.87 0.00 0.00 0.00
MOX (12% PuO2)a,c 0.00 77.50 10.63 11.87 0.00 0.00 0.00
PuO2 0.00 0.00 88.23 11.77 0.00 0.00 0.00
PuN 0.00 0.00 94.47 0.00 0.00 0.00 0.00
Pu3Si2 0.00 0.00 92.76 0.00 0.00 0.00 0.00
PuUZrHc 0.00 43.05 8.59 0.00 47.43 0.91 0.00
Pu0.31ZrH1.6b 0.00 0.00 44.47 0.00 54.54 0.96 0.00
Pu0.31ZrH1.6Th0.48b 39.98 0.00 26.68 0.00 32.74 0.58 0.00
Pu0.31ZrH1.6Th0.72b 49.99 0.00 22.24 0.00 27.27 0.48 0.00
Pu0.31ZrH1.6Th1.08b 59.97 0.00 17.79 0.00 21.83 0.39 0.00
PuZrO2Y2O3 (8%) 0.00 0.00 8.08 23.62 64.30 0.00 3.98
PuZrO2Y2O3 (15%) 0.00 0.00 15.00 21.75 57.90 0.00 5.35
PuZrO2MgO (8%) 0.00 0.00 7.99 28.93 40.87 0.00 22.19
PuZrO2MgO (15%) 0.00 0.00 15.00 26.74 37.76 0.00 20.50
a
MOX compositions are from Trellue, 2006.
b
Zirconium hydride compositions are from Olander et al., 2009.
c
Uranium is natural uranium.
d
Plutonium isotopic concentrations are shown in Table 3.3.

Table 3.3 2006). Each target fuel case contains only a single target fuel rod
Plutonium isotopic concentrations used in the present in the center of the fuel assembly with the remaining fuel rods
study.
modeled as 3 wt% enriched UO2 fuel. The target fuels are evaluated
Isotope Weight percent over a 1400 EFPD interval to verify that each would remain critical
Plutonium-238 2.37 over the entire burnup period. The normalized masses demon-
Plutonium-239 61.38 strate the relative effectiveness of each fuel for the transmutation
Plutonium-240 25.97 of a particular actinide.
Plutonium-241 4.81
Eleven different burnable absorbers, shown in Table 3.6, were
Plutonium-242 5.47
selected for evaluation as spectral shift absorber coatings in this
study. The eleven different potential spectral shift absorbers
model simulated 1400 Effective Full Power Days (EFPD), assuming were evaluated as burnable absorbers in previous work to
a total assembly power of 21.66 MWth, based on 3400 MWth evenly reduce initial excess reactivity in a very high temperature reac-
distributed across the 157 fuel assemblies of an AP1000 (Schulz, tor by incorporating the absorbers as a layer in modified TRISO
58 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72

Table 3.4
Target fuel composition with minor actinides at beginning of lifetime.

Fuel Constituents (wt%)

232
Th U Pud 241
Am 243
Am 244
Cm 237
Np O Zr H Y/Mg
a,c
MOX (5% PuO2) 0.00 83.72 3.73 0.37 0.06 0.01 0.27 11.86 0.00 0.00 0.00
MOX (7% PuO2)a,c 0.00 81.93 5.23 0.52 0.08 0.01 0.37 11.86 0.00 0.00 0.00
MOX (10% PuO2)a,c 0.00 79.27 7.46 0.74 0.11 0.02 0.53 11.87 0.00 0.00 0.00
MOX (12% PuO2)a,c 0.00 77.50 8.95 0.88 0.13 0.02 0.64 11.87 0.00 0.00 0.00
PuO2 0.00 0.00 74.37 7.33 1.11 0.17 5.28 11.77 0.00 0.00 0.00
PuN 0.00 0.00 79.57 3.83 7.84 0.19 5.65 0.00 0.00 0.00 0.00
Pu3Si2 0.00 0.00 78.12 7.70 1.17 0.18 5.55 0.00 0.00 0.00 0.00
PuUZrHc 0.00 43.05 7.24 0.71 0.11 0.02 0.51 0.00 47.43 0.91 0.00
Pu0.31ZrH1.6b 0.00 0.00 37.08 3.66 0.55 0.09 2.63 0.00 54.54 0.96 0.00
Pu0.31ZrH1.6Th0.48b 39.98 0.00 22.47 2.22 0.34 0.05 1.60 0.00 32.74 0.58 0.00
Pu0.31ZrH1.6Th0.72b 49.99 0.00 18.73 1.85 0.28 0.04 1.33 0.00 27.27 0.48 0.00
Pu0.31ZrH1.6Th1.08b 59.97 0.00 14.98 1.48 0.22 0.04 1.06 0.00 21.83 0.39 0.00
PuZrO2Y2O3 (8%) 0.00 0.00 6.73 0.66 0.10 0.02 0.48 23.62 64.30 0.00 3.98
PuZrO2Y2O3 (15%) 0.00 0.00 12.63 1.25 0.19 0.03 0.90 21.75 57.89 0.00 5.35
PuZrO2MgO (8%) 0.00 0.00 6.73 0.66 0.10 0.02 0.48 28.93 40.87 0.00 22.19
PuZrO2MgO (15%) 0.00 0.00 12.90 1.25 0.19 0.03 0.90 26.74 37.76 0.00 20.50
a
MOX compositions are from Trellue, 2006.
b
Zirconium hydride compositions are from Olander et al., 2009.
c
Uranium is natural uranium.
d
Plutonium isotopic concentrations are shown in Table 3.3.

Table 3.5 4. Uncoated transmutation fuel pin results

Composition of higher actinides in LWR fuel at 41200 MWd/MTHM burnup and
23 years of decay. This study evaluated sixteen potential target fuel compositions
Isotope Weight percent Isotope Weight percent (see Table 4.1) with and without initial concentrations of minor
238 243 actinides. The candidate fuels were evaluated with respect to the
Pu 1.99 Am 1.26
239
Pu 541.69 237
Np 5.98 relative quantity of plutonium transmutation over the fuel operat-
240
Pu 21.87 242
Cm 4.96E 5 ing cycle as well as the relative change in the quantity of the minor
241 243
Pu 4.05 Cm 3.42E 3 actinides over the same period. The ideal target fuel should reach
242 244
Pu 4.60 Cm 1.98E 1 the end of an operating cycle with no plutonium, americium, nep-
241 245
Am 8.30 Cm 2.19E 2
242
Am 1.87E 2 246
Cm 2.78E 3
tunium, or curium remaining in the target fuel. As described in Sec-
tion 3, the target fuel rod for this study is positioned in the central
instrumentation channel of the AP1000 robust fuel assembly. The
composition of this single, centered target fuel pin is varied to pro-
fuel particles (Washington et al., 2014). Though the materials vide a baseline of data for comparison purposes.
were evaluated in a different reactor environment, the require- This study evaluated plutonium oxide, plutonium silicide, and
ments for melting temperature, stability, natural abundance of plutonium nitride as plutonium-only target fuels. The Mixed Oxide
absorbing isotope, and extended decay time still apply to this (MOX) target fuels had a variety of plutonium oxide weight frac-
study. The spectral shift absorbers are applied as a coating of tions (5, 7, 10, 12 wt%). The two versions of hydride target fuels
either 4.25 lm or 144.25 lm thickness around the target fuel were plutonium zirconium hydride and plutonium zirconium
pellets. The 4.25 lm thickness was selected by rounding to the hydride with thorium (40, 50, and 60 wt% thorium). The plutonium
nearest hundredths decimal place on the outer diameter of the oxide target fuel was selected as a uranium-free comparison fuel
fuel pellet. The 144.25 lm thickness was selected from the lar- because is more commonly found in research than the other two
gest coating thickness evaluated in preliminary feasibility simu- plutonium-only fuels (Kloosterman, 2003; Peryoga et al., 2005;
lations performed for this study. The gap between the fuel pellet Sagara et al., 2005). The MOX fuels were selected for their preva-
and cladding is reduced to make space for the spectral shift lence in plutonium transmutation studies and to serve as a com-
absorber coating. mon denominator (Fetterman, 2009). The plutonium zirconium

Table 3.6
Spectral shift absorbers evaluated in the present study.

Absorber Density (g/cm3) @ 1200 K Melting point (K) Isotope of interest Absorption cross-section ra (barns) Resonance integral (barns)
B4C 2.49 2623a 10
B 3837b 1722b
CdO 8.07 1773a 113
Cd 20,600b 390b
Dy2O3 7.75 2501a 164
Dy 2650b 340b
Er2O3 8.57 2617a 167
Er 659b 2970b
Eu2O3 7.35 2564a 151
Eu 9200b 3300b
Gd2O3 7.35 2612a 157
Gd 254,000b 700b
HfO2 9.62 3073a 177
Hf 380b 7173b
In2O3 7.12 2185a 115
In 215b 3300b
Lu2O3 9.34 2700a 176
Lu 2090b 1087b
Sm2O3 7.54 2542a 149
Sm 40,140b 3390b
TaC 14.21 4153a 181
Ta 21b 660b
a
Lide (2009).
b
Dunford and Kinsey (1998).
 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72 59

Table 4.1 results in the buildup of plutonium-238 which does not occur in
Target fuels in this study and their designations. the minor actinide-free 5 wt% MOX fuel. The addition of the initial
Fuel Designation Designation with minor actinides minor actinides to a 5 wt% MOX target fuel rod resulted in an over-
PuO2 PuO [Pu + ma]O all decrease in the quantity of minor actinides, by 36% of their ini-
PuN PuN [Pu + ma]N tial mass, for the irradiation period used in this study.
Pu3Si2 PuSi [Pu + ma]Si Fig. 4.3 shows the transmutation of the combined minor acti-
MOX (5% PuO2) MOX (5%) [MOX + ma] (5%) nides (neptunium, americium, and curium) as a function of time
MOX (7% PuO2) MOX (7%) [MOX + ma] (7%)
MOX (10% PuO2) MOX (10%) [MOX + ma] (10%)
for each of the MOX with minor actinide target fuels evaluated in
MOX (12% PuO2) MOX (12%) [MOX + ma] (12%) this study. The quantity of plutonium oxide in these fuels varied
Pu0.31ZrH1.6 PuZrH [Pu + ma]ZrH between 5, 7, 10, and 12 wt% of the MOX fuel. The minor actinide
Pu0.31ZrH1.6Th0.48 PuZrHTh (40%) [Pu + ma]ZrHTh (40%) net mass in these MOX target fuels increased with the percentage
Pu0.31ZrH1.6Th0.72 PuZrHTh (50%) [Pu + ma]ZrHTh (50%)
of plutonium oxide in the initial fuel. The final transmutation ratio
Pu0.31ZrH1.6Th1.08 PuZrHTh (60%) [Pu + ma]ZrHTh (60%)
PuZrO2Y2O3 (8%) Pu(Zr,Y)O (8%) [Pu + ma](Zr,Y)O (8%) for the 7 wt% target fuel rod was essentially equal to that of the
PuZrO2Y2O3 (15%) Pu(Zr,Y)O (15%) [Pu + ma](Zr,Y)O (15%) 5 wt% target fuel rod (29.2 wt% and 30.4 wt%, respectively). The
PuZrO2MgO (8%) Pu(Zr,Mg)O (8%) [Pu + ma](Zr,Mg)O (8%) 10 and 12 wt% MOX target fuels had slightly worse transmutation
PuZrO2MgO (15%) Pu(Zr,Mg)O (15%) [Pu + ma](Zr,Mg)O (15%) ratios (27.1 wt% and 25.7 wt%, respectively) than the 5 wt% fuel.
PuUZrH PuUZrH [Pu + ma]UZrH

4.2. Plutonium target fuels

hydride fuels are a variation of the plutonium uranium zirconium
hydride fuels (PUZH) which have been previously evaluated for use
in PWRs (Ganda and Greenspan, 2009). Previous studies on pluto-
nium hydride and uranium zirconium hydride fuels determined
the compositions of the Pu0.31ZrH1.6 fuels (Ganda and Greenspan,
2009; Olander et al., 2009; Simnad, 1981).
4.1. Mixed oxide target fuels
Fig. 4.1 displays the plutonium and minor actinide normalized
masses (M/M0) as a function of time, at 21.66 MWth, for a MOX fuel
containing 5 wt% plutonium oxide. As a MOX fuel without initial
minor actinides, this fuel serves as an initial point for further com-
parison with the other potential fuels. In Fig. 4.1, all the isotopes
except plutonium are represented on the secondary axis. The only
isotopes of plutonium which had a net depletion during the simu-
lation are plutonium-238, plutonium-239, and plutonium-240.
From a non-proliferation perspective, the decrease of the
plutonium-238 content of the fuel to 63% of its initial mass is less
optimal than an increase (Chang, 2009; Peryoga et al., 2005; Sagara
et al., 2005).
The quantity of plutonium-240 in the 5 wt% MOX fuel remains
relatively stable, reaching 97% of its initial mass by the end of the
irradiation period. A significant number of the actinides in this fuel
trend towards an equilibrium state by the end of the evaluation
period (1400 EFPD); but, plutonium-242 and curium-245 show
an increasing trend as a function of time. The increase of these
long-lived isotopes is not ideal from the perspective of long term
storage and disposal (Alajo and Tsvetkov, 2011; Bunn et al., 2003).
Fig. 4.2 shows the development of the selected actinides as a
function of time for 5 wt% plutonium oxide MOX fuel containing
minor actinides. Irradiation of this target fuel results in the net
destruction of neptunium-237, americium-241, plutonium-239,
and plutonium-240. The over twofold increase in the quantity of
plutonium-238 and the relatively stable quantity of plutonium-
240, ending at 97 wt% of its initial mass, increases the proliferation
resistance of the target fuel rod. Although the majority of the minor
actinides are not depleted during the irradiation period, the total
quantity of minor actinides does decrease by 30 percent of its ini-
tial mass as a result of the transmutation of neptunium-237 and
americium-241.
During irradiation, the MOX target fuel with 5 wt% PuO2
resulted with a net increase in the quantity of americium-241
and neptunium-237. For the same irradiation period, the MOX
with 5 wt% PuO2 and minor actinide target fuel resulted in a net
decrease in the quantity of americium-241 and neptunium-237.
The irradiation of the 5 wt% MOX with minor actinide fuel also
Three ‘‘purely” plutonium target fuels, plutonium dioxide, plu-
tonium silicide, and plutonium nitride, were evaluated in this
study. Though the initial concentration of plutonium in each of
these fuels had a wide range, 74–94.5 wt% of the fuel mass, they
are the least complex of the target fuels evaluated in this study
and result in similar reductions in both plutonium and minor acti-
nide content. The plutonium oxide target fuel yielded a depletion
of 13 wt% of its initial plutonium-238 and 25 wt% of its initial
plutonium-239 but otherwise resulted in an increase of all other
plutonium and minor actinide isotopes over the 1400 Effective Full
Power Days (EFPD) irradiation time (Fig. 4.4). This irradiation per-
iod is not long enough for any of the minor actinides to reach equi-
librium, in which the rate of their generation equals the rate of
their transmutation. Similar trends are seen with the plutonium
nitride and plutonium silicide target fuels. Over the 1400 EFPD
irradiation period, 12 wt% of the initial plutonium-238 and 20 wt
% of the plutonium-239 were transmuted in the plutonium nitride
fuel. Irradiation of the plutonium silicide target fuel resulted in a
reduction in the quantity of plutonium-238 and plutonium-239
by 13 wt% and 25 wt% of their initial value. The quantity of
plutonium-242, Fig. 4.5, remained nearly constant during the irra-
diation period in the plutonium nitride fuel and increased slightly
in the plutonium oxide and plutonium silicide fuels. The nearly
steady state behavior of the plutonium-242 in the plutonium
nitride fuel is unusual, as all other target fuel types resulted in
an increasing quantity of this isotope. The smallest increase in
plutonium-242 occurred in the plutonium oxide and plutonium
silicide fuels (increasing approximately 1 wt% over its initial
value). The remaining isotopes of plutonium and the minor acti-
nides all increased in concentration during the irradiation period
for the plutonium nitride fuel. Irradiation of the plutonium silicide
fuel also results in an increase in the other plutonium isotopes and
the minor actinides all increased in quantity over this irradiation
period.
Irradiation of the three plutonium-only target fuels, with initial
minor actinides, results in a decrease in the total quantity of minor
actinides over the 1400 EFPD irradiation period. The irradiation of
the plutonium oxide target fuel with initial minor actinides
(Fig. 4.6) resulted in an increase in the quantity of plutonium-
238 by 88 wt% compared to its initial value while still transmuting
26 wt% of the initial plutonium-239. The remaining isotopes of plu-
tonium also increased during the irradiation period though at a sig-
nificantly reduced rate compared to the target fuel containing only
plutonium. Compared to the plutonium-only oxide target fuel, the
plutonium plus minor actinide oxide fuel resulted in the transmu-
tation of minor actinides and a net decrease in the quantity of
minor actinides at the end of the 1400 EFPD irradiation period.
60 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72

Fig. 4.1. MOX (5% PuO2) isotopic data as a function of time at 21.66 MWth per assembly.

Fig. 4.2. MOX (5% [Pu + ma]O2) isotopic data as a function of time at 21.66 MWth per assembly including minor actinides.

The irradiation of the plutonium plus minor actinide target fuel
resulted in an 18 wt% decrease in the quantity of americium-241
and a 17 wt% decrease in the quantity of neptunium-237. The
remainder of the minor actinides increased during this irradiation
period; however, the large quantity of americium-241 and
neptunium-237 transmuted resulted in a net decrease in the total
quantity of minor actinides.
Irradiation of the plutonium and minor actinide nitride target
fuel also resulted in an 87 wt% increase in the quantity of
plutonium-238. This target fuel transmuted 26 wt% of the
plutonium-239 with the remaining isotopes of plutonium increas-
ing in quantity during the irradiation period. Reduction of the
minor actinides only occurred with respect to americium-241
and neptunium-237, with a decrease of 18 wt% and 27 wt% from
their initial values, respectively. Irradiation of the plutonium sili-
cide with initial minor actinide target fuel resulted in an increase
in the quantity of plutonium-238 by 86 wt%, a decrease in the
quantity of plutonium-239 by 25 wt%, as well as a decrease in
americium-241 by 18 wt%, and a decrease of 16 wt% in
neptunium-237. Irradiation of all three of the plutonium with
minor actinide target fuels resulted in an increase in the quantity
of curium in the fuel. In each of the three minor actinide cases,
the total quantity of minor actinides decreased during the irradia-
tion period; however, the inclusion of initial minor actinides in
each of these three target fuels increased the quantity of minor
actinides produced, with the exception of americium-241 and
neptunium-237, compared to the plutonium-only target fuels.
In each of the minor actinide cases, the plutonium-only fuels
produced less americium-243, and less curium than the 5 wt%
MOX fuel with initial minor actinides. Irradiation of the three plu-
tonium and minor actinide target fuels transmuted a greater quan-
tity of plutonium-238, plutonium-241, and plutonium-242 than
the target MOX fuel rod. The three plutonium and minor actinide
target fuel rods did not result in a superior transmutation ratio
for neptunium-237, americium-241, plutonium-239, and
plutonium-240 compared to the 5 wt% MOX fuel rod. Though tar-
get fuels composed of mostly plutonium are simple, they are unli-
kely to be used in a reactor environment without some form of
 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72 61

Fig. 4.3. Minor actinide content in the MOX target fuels with minor actinides as a function of time at 21.66 MWth per assembly.

Fig. 4.4. PuO2 isotopic data as a function of time at 21.66 MWth per assembly.

dilution. The dilution of the plutonium serves to increase the pro-
liferation resistance of the fuel, to reduce power peaking, hot spots,
and reactivity swing, and to produce a more stable reactor environ-
ment (Peryoga et al., 2005; Pistner et al., 2006; Sagara et al., 2005).
4.3. Plutonium-uranium zirconium hydride target fuels
A target fuel rod composed of plutonium uranium zirconium
hydride transmuted of 54 wt% of the total plutonium in the fuel
rod, including any additional plutonium generated by the uranium
in the mix. Fig. 4.7 shows the normalized masses of plutonium and
minor actinides in the PuUZrH target fuel as a function of time at
21.66 MWth per assembly. Irradiation of this target fuel achieved
the transmutation of 46 wt% of the plutonium-238, 85 wt% of the
plutonium-239, and 27 wt% of the plutonium-240. Additionally,
70 wt% of the uranium-235 was depleted during the course of
the irradiation. The isotopes of plutonium-241 and plutonium-
242 increased in quantity during the irradiation of this target fuel,
by 70 wt% and 52 wt%, respectively.
Fig. 4.8 shows the isotopic data for the plutonium uranium zir-
conium hydride with minor actinide target fuel as a function of
irradiation time. Irradiation of the PuUZrH target fuel rod with ini-
tial minor actinides resulted in the transmutation of 45% of the
total plutonium in the target fuel rod, again including the pluto-
nium generated from the uranium component of the fuel. The
decrease in total plutonium concentration results from the trans-
mutation of 83 wt% of the plutonium-239 and 27 wt% of the
plutonium-240 in the target fuel rod. The remainder of the pluto-
nium isotopes increased in quantity over the irradiation period,
including an increase in the plutonium-238 concentration by a fac-
tor of 2.7. The total quantity of minor actinides was reduced by
37 wt% during the irradiation period. During irradiation, the quan-
tity of americium-241 in the target fuel rod decreased by 77 wt%,
the quantity of curium-244 decreased by 35 wt%, and the quantity
of neptunium-237 decreased by 45 wt% with the remainder of the
minor actinides increasing. Similar to the PuUZrH target fuel with-
out initial minor actinide, the quantity of uranium-235 decreased
by 70 wt% during irradiation.
62 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72

Fig. 4.5. Normalized mass of plutonium-242 as a function of time at 21.66 MWth per assembly for the plutonium target fuels.

Fig. 4.6. [Pu + ma]O2 isotopic data as a function of time at 21.66 MWth per assembly.

Fig. 4.7. PuUZrH isotopic data as a function of time at 21.66 MWth per assembly.
 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72 63

Fig. 4.8. [Pu + ma]UZrH isotopic data as a function of time at 21.66 MWth per assembly.

Contrasting the PuUZrH target fuel with the 5 wt% MOX fuel,
both with initial minor actinide, reveals the PuUZrH fuel to be a
slightly superior transmutation fuel. The PuUZrH target fuel
resulted in an average 3% higher net destruction rate, considering
all of the plutonium and minor actinide isotopes. The majority of
the increased transmutation came from the 40% increase in
plutonium-239 destruction and the 7% increase in americium-
243, curium-244, and plutonium-241 transmutation.
4.4. Plutonium zirconium hydride target fuels
Irradiation of the plutonium zirconium hydride target fuel
(Fig. 4.9) resulted in an end-of-life transmutation of 29 wt% of
the initial plutonium in the target fuel rod. The transmutation
included 22 wt% of the plutonium-238, and 52 wt% of the
plutonium-239. Though production of plutonium-240 occurred
during the majority of the irradiation time, the final 200-day time
step resulted in a decrease in the total quantity of this isotope.
Plutonium-241 and plutonium-242 were produced at a continuous
rate over the course of the irradiation and reached 57 wt% and
24 wt%, respectively, over their initial values by the end of the irra-
diation. This target fuel type did not result in the net transmutation
of any of the minor actinides.
The plutonium zirconium hydride target fuel with initial minor
actinide (Fig. 4.10) achieved the transmutation of 25 wt% of the ini-
tial plutonium within the target fuel rod as well as the transmuta-
tion of 20 wt% of the minor actinides. During the irradiation period,
the quantity of plutonium-238 increased to 250 wt% of its initial
value while the quantity of plutonium-239 decreased to 46 wt%
of its initial value. The plutonium-240 concentration reached a
peak value at around 1100 days and then declined to only 2 wt%
above its initial value by the end of the simulation. The masses
of plutonium-241 and plutonium-242 also increased during this
simulation to a peak of 57 wt% and 25 wt%, respectively, above
their initial values. The irradiation of this target fuel resulted in
the transmutation of 40 wt% of the americium-241 and 28 wt% of

Fig. 4.9. PuZrH isotopic data as a function of time at 21.66 MWth per assembly.
64 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72

Fig. 4.10. [Pu + ma]ZrH isotopic data as a function of time at 21.66 MWth per assembly.

the neptunium-237 contained and generated in the target fuel. The
remainder of the minor actinides all increased in quantity during
irradiation.
Contrasting the plutonium zirconium hydride fuel with the
5 wt% MOX fuel, both with initial minor actinide, reveals pluto-
nium zirconium hydride to be a good curium transmutation fuel
but a net generator of plutonium-238. Though the fuel transmutes
40% less plutonium-239 than the MOX target fuel, it produces 21%
less curium-242, 36% less curium-243, 48% less curium-244, and
36% less americium-243. Though the PuZrH fuel is effective in
reducing the quantity of curium, its average performance is 15%
worse than the 5 wt% MOX target fuel with the majority of the
isotopic difference resulting from smaller reductions of
americium-241, plutonium-239, and neptunium-237 and slight
increases in plutonium-240 and plutonium-243.
4.5. Plutonium zirconium hydride with thorium hydride target fuels
This study also considered plutonium zirconium hydride fuel
containing a fraction of thorium hydride. The three versions of
the fuel considered had 40, 50, or 60 wt% of the total plutonium
zirconium hydride replaced with thorium hydride. Fig. 4.11 shows
the isotopic data as a function of irradiation time for the plutonium
zirconium hydride target fuel with 50 wt% of thorium hydride. The
total plutonium transmutation for each of these fuels, which did
not contain initial minor actinides, was 35 wt%, 39 wt%, and
43 wt% for the fuels containing 40 wt%, 50 wt%, and 60 wt% of tho-
rium hydride, respectively. In the 40 wt% thorium hydride target
fuel, 25 wt% of the plutonium-238 and 62 wt% of the plutonium-
239 were transmuted during the irradiation. The plutonium-240
isotope ended at the initial mass and the quantity of isotopes of
plutonium-241 and plutonium-242 increased by 63 wt% and
18 wt% respectively. The transmutation of plutonium in the
50 wt% thorium hydride version of the fuel comes from the trans-
mutation of 28 wt% of plutonium-238, 68 wt% of plutonium-239,
and 2 wt% of plutonium-240. By the end of the irradiation period,
the isotopes of plutonium-241 and plutonium-242 increased by
66 wt% and 23 wt% over their initial values, respectively. Irradia-
tion of the third version of the plutonium zirconium hydride fuel,
containing 60 wt% thorium hydride, resulted in the transmutation

Fig. 4.11. PuZrHTh (50%) isotopic data as a function of time at 21.66 MWth per assembly.
 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72
of 32 wt%, 74 wt%, and 5 wt% of the plutonium-238, plutonium-
239, and plutonium-240, respectively. Irradiation of the 60 wt%
thorium hydride fuel resulted in the quantity of plutonium-241
and plutonium-242 increasing over the irradiation period and
reached a maximum of 69 and 30 wt% over their initial values at
the end of the irradiation period.
The three versions of the plutonium zirconium hydride with
thorium hydride fuel were also tested with initial minor actinide
within the plutonium portion of the target fuel. Fig. 4.12 shows
the isotopic data for the plutonium with minor actinide zirconium
hydride target fuel with 50 wt% of thorium hydride. The irradiation
of these fuels resulted in the transmutation of 30 wt%, 33 wt%, and
39 wt%, respectively, of the total plutonium for each of the three
fuel types (40, 50, and 60 wt% thorium hydride). The total quantity
of minor actinides also decreased by 24, 27, and 31 wt% of their
total values for each of the three fuel types (40, 50, and 60 wt% tho-
rium hydride) respectively. In the 40 wt% thorium version of these
target fuels with minor actinide, the net plutonium destruction
resulted from the depletion of 63 wt% of the plutonium-239. The
quantity of plutonium-240 remained relatively constant over the
course of the simulation, reaching a maximum at 800 days and
then depleting back to its original value by the end of the simula-
tion. Plutonium-238, plutonium-241, and plutonium-242
increased in concentration over the course of the irradiation by
163 wt%, 66 wt%, and 33 wt% over their initial values, respectively.
Minor actinide depletion in the 40 wt% thorium plutonium zirco-
nium hydride target fuel occurred for americium-241 and
neptunium-237, which were depleted by 48 wt% and 31 wt%,
respectively. Similar results are seen in the 50 wt% and 60 wt% ver-
sions of the fuel where the destruction of the plutonium-239 iso-
tope was 62 wt% and 76 wt%, respectively. The quantity of
plutonium-240, at the end of the irradiation period, decreased in
both of these cases by 2 wt% and 6 wt%, respectively, for the
50 wt% and 60 wt% thorium hydride fuels.
The 50 wt% thorium hydride target fuel achieved 53 wt% and
33 wt% transmutation of americium-241 and neptunium-237,
respectively. Irradiation of the 60 wt% thorium hydride target fuel
resulted in the transmutation of 60 wt% of the americium-241 and
37 wt% of the neptunium-237. The 50 wt% and 60 wt% thorium
hydride target fuels produced additional quantities of the remain-
ing plutonium and minor actinide isotopes.
Fig. 4.12. [Pu + ma]ZrHTh (50%) isotopic data as a function of time at 21.66 MWth per assembly.
65
Compared to the 5 wt% MOX fuel, the plutonium zirconium tho-
rium hydride fuels with initial minor actinide are superior for the
transmutation of curium; however, these three fuels performed
worse on average than the MOX target fuel in terms of plutonium
and minor actinide transmutation. The plutonium thorium hydride
fuels produced 23%, 20%, and 14% less curium than the 5 wt% MOX
target fuel. The plutonium thorium fuels also produced, on average,
a third less americium-243 than the MOX target fuels but approx-
imately double the quantity of americium-241.
4.6. Plutonium zirconium oxide target fuels
Inert matrix fuels that did not contain initial minor actinide
resulted in a net reduction in plutonium with the greatest deple-
tion achieved from the magnesium oxide stabilized zirconia fuel
with 8 wt% of initial plutonium. Each of the minor actinide bearing
target fuels also resulted in a reduction of total plutonium concen-
tration though at a reduced amount when contrasted with the pure
target fuel. The minor actinide containing target fuels all resulted
in a net decrease in minor actinide concentrations (from 7% in a
plutonium oxide fuel compared to 33% with the 8 wt% PuZrO2MgO
target fuel). When the 8 wt% PuZrO2MgO target fuel contains initial
minor actinides, it still results in the highest plutonium depletion,
44 wt% of the initial plutonium mass, as well as resulting in the
greatest reduction in total minor actinide concentration, transmut-
ing approximately one third of the initial minor actinide inventory.
Fig. 4.13 shows the specific isotopic data as a function of time
for the 8 wt% PuZrO2MgO target fuel without initial minor acti-
nides. Similar to the 5 wt% MOX fuel shown in Fig. 4.1, the
plutonium-238, plutonium-239, and plutonium-240 isotopes are
the only ones that show depletion over the evaluated time period.
Compared to the 5 wt% MOX target fuel, the 8 wt% PuZrO2MgO
target fuel has a greater swing in the normalized mass of
plutonium-240 over the same irradiation period but still retains
84% of its initial mass at the end of the irradiation. The concentra-
tion of plutonium-241 reaches a maximum around 760 EFPD, at
approximately 1.8 times its initial concentration, and begins to
be depleted near the end of the evaluation period. The rate of
plutonium-242 accumulation in the 8 wt% PuZrO2MgO fuel rod is
similar to that in the 5 wt% MOX target fuel rod ending at nearly
1.5 times the initial concentration. None of the minor actinide
66 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72

Fig. 4.13. PuZrO2MgO 8% isotopic data as a function of time at 21.66 MWth per assembly.

isotopes in the 8 wt% PuZrO2MgO fuel rod reach equilibrium over
the evaluated depletion period, nor are they depleted.
The isotopic data as a function of irradiation time for the 8 wt%
PuZrO2MgO target fuel with initial minor actinide are presented in
Fig. 4.14. As with the 5 wt% minor actinide containing MOX target
fuel, plutonium-243 and curium-242 are produced in the target
fuel and the americium-242 mass again reaches a maximum
around 300 EFPD and then begins to decrease. Only plutonium-
239, plutonium-240, americium-241, and neptunium-237 show a
net depletion during this simulation, and 83% of the plutonium-
239 is transmuted by the end of the irradiation period. Compared
to the 5 wt% MOX fuel containing minor actinides, the rate of
depletion for plutonium-239 (76 wt% depletion vs 95 wt% for the
inert matrix fuel) and plutonium-240 (19 wt% vs 41 wt%) is greater
in the inert matrix fuel. The 8 wt% PuZrO2MgO fuel with minor
actinides also produces curium-243 at a higher rate, 12 wt% more
by the end of cycle, than the MOX fuel.
The addition of minor actinides to the 8 wt% PuZrO2MgO target
fuel reduces the overall destruction of plutonium by 12 wt% but
results in the transmutation of a third of the initial minor actinides.
Similar to the 5 wt% MOX target fuel with minor actinide, the
addition of minor actinides to the 8 wt% PuZrO2MgO target fuel
results in the net destruction of americium-241 and neptunium-
237. The rates of minor actinide transmutation for the 8 wt%
PuZrO2MgO target fuel are slightly higher compared to the rate
in the 5 wt% MOX target fuel, 33 wt% and 30 wt%, respectively.
The inert matrix fuels performed better than the 5 wt% MOX
target fuel both on average and considering the individual isotopes.
The 8 wt% inert matrix fuels transmuted 10% more of the pluto-
nium and minor actinides than the MOX fuel where the 15 wt%
inert matrix fuels only achieved a 3–4% increase over the MOX fuel.
The inert matrix with minor actinide fuels worked especially well
for the transmutation of plutonium-239 achieving nearly double
the ratio of plutonium-239 transmuted than the 5 wt% MOX with
minor actinide target fuel. The 15 wt% inert matrix with minor
actinide target fuels transmuted less americium-241 than the
MOX target fuel, 74 wt% and 78 wt%, respectively.
4.7. Target fuel observations
Fig. 4.15 provides a summary of the normalized masses of the
minor actinide as a function of time for sixteen of the minor

Fig. 4.14. [Pu + ma]ZrO2MgO 8% isotopic data as a function of time at 21.66 MWth per assembly with minor actinides.
 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72 67

actinide containing target fuels evaluated in this study. Table 4.2 Table 4.2
lists the change in weight percent of plutonium and minor acti- Change in weight percent of plutonium and minor actinides from BOL to EOL for each
target fuel.
nides from BOL to EOL for each target fuel evaluated in this study.
Table 4.3 provides the end-of-life data for the target fuels evalu- Fuel Without minor actinides With minor actinides
ated in this study without initial concentrations of minor actinides DPu DMA DPu
and Table 4.4 provides the end-of-life data for the target fuels with MOX (5% PuO2) 34.95 30.36 26.37
initial concentrations of minor actinides. In terms of minor actinide MOX (7% PuO2) 34.80 29.18 27.39
transmutation rates, the zirconium oxide fuels with 8 wt% initial MOX (10% PuO2) 32.85 27.05 26.57
plutonium are the superior fuels for the depletion period used in MOX (12% PuO2) 31.26 25.65 25.54
PuO2 9.84 7.23 8.14
this study. Interestingly, the target fuels in Fig. 4.15 are graded
PuN 8.21 7.19 8.10
with respect to initial plutonium loading. The rate of transmuta- Pu3Si2 9.59 7.05 7.91
tion of plutonium and minor actinides in each of these target fuels PuUZrH 40.88 30.65 34.29
is inversely proportional to their initial concentration. This rela- PuZrH 20.05 15.24 17.11
Pu0.31ZrH1.6Th0.48 24.39 18.24 21.05
tionship allows for the selection of a target fuel for a particular irra-
Pu0.31ZrH1.6Th0.72 27.11 20.06 23.47
diation period. Pu0.31ZrH1.6Th1.08 30.57 23.17 27.71
Fig. 4.16 shows the relative change in minor actinide contents PuZrO2Y2O3 (8%) 48.49 32.72 42.34
as a function of the initial plutonium concentration. Fig. 4.16 PuZrO2Y2O3 (15%) 39.36 28.01 34.29
shows a higher minor actinide transmutation rate over 1400 EFPD PuZrO2MgO (8%) 50.02 33.29 43.73
PuZrO2MgO (15%) 41.31 29.09 36.03
for those fuels that have the lower initial loading of plutonium. The
relationship between these target fuels and their concentrations of
plutonium is roughly logarithmic and relatively independent of the
type of target fuel. This indicates a potential for tuning of the rate Three of the evaluated fuels, 5 wt% MOX, plutonium 60 wt%
of minor actinide transmutation by adjusting the initial fuel com- thorium zirconium hydride, and 8 wt% plutonium magnesium
position. Tuning the quantity of plutonium in the target fuel for oxide inert matrix, were selected for evaluation with a spectral
the cycle length of the fuel assembly could maximize the quantity shift absorber coating to determine if the fuel’s transmutation per-
of minor actinides transmuted. formance could be further improved. The 5 wt% MOX with minor
Fig. 4.17 shows the activity of one target fuel for each of the actinide was selected for the purposes of comparison as well as
matrix types as well as the activity of a uranium oxide fuel pin its transmutation performance. The 60 wt% thorium hydride fuel
as a function of time in the central coolant channel of the simu- with minor actinide achieved the greatest quantity of transmuta-
lated AP1000. The small quantities of minor actinides contained tion of the thorium hydride fuels and was also selected to broaden
in the target fuels do not result in an irradiated material that is the variety of fuels evaluated. The 8 wt% PuZrO2MgO fuel with
more active than the same fuels without minor actinides. Only minor actinide was selected because it achieved the greatest quan-
the PuZrO2MgO target fuels produced an activity that was less than tity of plutonium and minor actinide transmutation of the fuels
that of a uranium oxide fuel pin irradiated in the same position. evaluated in this study.
The end of life activity for the 8 wt% PuZrO2MgO with minor acti-
nide target fuel was 1.04  104 TBq compared to 1.73  104 TBq for 5. Spectral shift absorber coated transmutation fuel pin results
a uranium oxide target fuel rod. Though the PuZrO2MgO target
fuels started their cycle with a higher activity than a uranium oxide The three target fuels, 5 wt% MOX, 60 wt% thorium plutonium
fuel pin, they were sufficiently depleted after approximately 440 zirconium hydride, and 8 wt% PuZrO2MgO, with an initial concen-
EFPD that they had an overall lower activity from that time tration of minor actinides, were simulated with the spectral shift
onward. absorber coatings shown in Table 3.6. The coatings were placed

Fig. 4.15. Target fuel minor actinide concentration as a function of time at 21.66 MWth per assembly.
68 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72

Table 4.3
End-of-life composition of the target fuels without minor actinides.

Fuel Constituents (wt%)

232 235 238 238 239 240 241 242 241 243 244 237
Th U U Pu Pu Pu Pu Pu Am Am Cm Np
MOX (5% PuO2) 0.00 0.27 82.07 0.07 0.94 1.11 0.42 0.35 0.03 0.05 0.01 0.01
MOX (7% PuO2) 0.00 0.29 80.36 0.10 1.33 1.60 0.56 0.46 0.04 0.07 0.02 0.01
MOX (10% PuO2) 0.00 0.31 77.77 0.15 2.07 2.35 0.76 0.62 0.05 0.08 0.02 0.01
MOX (12% PuO2) 0.00 0.32 76.03 0.18 2.67 2.86 0.89 0.71 0.07 0.09 0.02 0.01
PuO2 0.00 0.00 0.00 1.89 44.90 23.42 4.56 4.84 0.52 0.22 0.03 0.00
PuN 0.00 0.01 0.00 2.04 49.96 24.96 4.63 5.16 0.55 0.21 0.02 0.00
Pu3Si2 0.00 0.01 0.00 1.99 47.47 24.60 4.74 5.09 0.54 0.23 0.03 0.00
PuUZrH 0.00 0.15 42.06 0.13 1.45 2.05 0.79 0.66 0.05 0.09 0.03 0.00
Pu0.31ZrH1.6b 0.00 0.00 0.00 0.88 16.96 11.79 3.07 2.52 0.28 0.23 0.04 0.00
Pu0.31ZrH1.6Th0.48b 39.51 0.00 0.00 0.51 8.94 7.17 1.98 1.58 0.17 0.16 0.03 0.00
Pu0.31ZrH1.6Th0.72b 49.42 0.00 0.00 0.42 6.78 5.96 1.70 1.35 0.14 0.14 0.03 0.00
Pu0.31ZrH1.6Th1.08b 59.31 0.00 0.00 0.32 4.77 4.74 1.41 1.12 0.11 0.13 0.03 0.00
PuZrO2Y2O3 (8%) 0.00 0.00 0.00 0.11 0.87 1.81 0.69 0.63 0.05 0.09 0.03 0.00
PuZrO2Y2O3 (15%) 0.00 0.00 0.00 0.24 2.46 3.78 1.25 1.07 0.09 0.14 0.04 0.00
PuZrO2MgO (8%) 0.00 0.00 0.00 0.11 0.80 1.75 0.69 0.65 0.05 0.10 0.03 0.00
PuZrO2MgO (15%) 0.00 0.00 0.00 0.24 2.71 3.85 1.24 1.04 0.09 0.13 0.03 0.00
a
Zirconium hydride compositions are from Olander et al. (2009).

Table 4.4
End-of-life composition of the target fuels with minor actinides.

Fuel Constituents (wt%)

232 235 238 238 239 240 241 242 241 243 244 237
Th U U Pu Pu Pu Pu Pu Am Am Cm Np
MOX (5% PuO2) 0.00 0.27 82.07 0.23 0.88 0.94 0.37 0.33 0.13 0.09 0.04 0.18
MOX (7% PuO2) 0.00 0.29 80.36 0.32 1.20 1.35 0.49 0.44 0.21 0.11 0.05 0.26
MOX (10% PuO2) 0.00 0.31 77.77 0.45 1.81 1.98 0.66 0.59 0.34 0.15 0.07 0.38
MOX (12% PuO2) 0.00 0.32 76.03 0.53 2.29 2.41 0.77 0.68 0.43 0.17 0.08 0.46
PuO2 0.00 0.00 0.00 2.80 37.53 19.90 3.82 4.28 6.42 1.13 0.33 4.68
PuN 0.00 0.00 0.00 2.99 40.20 21.29 4.08 4.57 6.87 1.21 0.35 5.01
Pu3Si2 0.00 0.00 0.00 2.92 39.68 20.88 3.97 4.49 6.78 1.18 0.34 4.93
PuUZrH 0.00 0.15 42.06 0.45 1.28 1.71 0.68 0.63 0.27 0.16 0.08 0.35
Pu0.31ZrH1.6a 0.00 0.00 0.00 1.82 14.02 9.99 2.60 2.32 2.60 0.62 0.24 2.13
Pu0.31ZrH1.6Th0.48a 39.50 0.00 0.00 1.17 7.35 6.06 1.68 1.47 1.44 0.39 0.16 1.25
Pu0.31ZrH1.6Th0.72a 49.41 0.00 0.00 1.01 5.57 5.03 1.45 1.26 1.13 0.33 0.14 1.02
Pu0.31ZrH1.6Th1.08a 59.26 0.00 0.00 0.84 3.73 3.98 1.21 1.07 0.81 0.28 0.12 0.79
PuZrO2Y2O3 (8%) 0.00 0.00 0.00 0.41 0.77 1.50 0.59 0.60 0.23 0.15 0.07 0.31
PuZrO2Y2O3 (15%) 0.00 0.00 0.00 0.76 2.07 3.15 1.08 1.02 0.53 0.26 0.12 0.62
PuZrO2MgO (8%) 0.00 0.00 0.00 0.42 0.71 1.44 0.60 0.62 0.22 0.16 0.08 0.31
PuZrO2MgO (15%) 0.00 0.00 0.00 0.75 2.27 3.22 1.06 1.00 0.56 0.25 0.12 0.63
a
Zirconium hydride compositions are from Olander et al. (2009).

Fig. 4.16. Initial plutonium wt% as a function of change in minor actinide wt%.
 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72 69

Fig. 4.17. Activity of selected target fuel rods as a function of time at 21.66 MWth per assembly.

between the fuel rod cladding and on the outside of the fuel pellet
with two different thicknesses, 4.25 lm and 144.25 lm. The two
thicknesses are used to allow for extrapolation of transmutation
rates for intermediate thicknesses of the spectral shift absorbers.
The relative transmutation rates, or percent difference between
coated and uncoated target fuels, were calculated as the difference
in mass of each isotope in the coated fuel and the uncoated fuel
divided by the mass of the isotope in the uncoated fuel at end-
of-life. Tables 5.1, 5.2, and 5.3 present the percent difference in
the transmutation rates between the coated and uncoated target
fuels with minor actinide for each of the spectral shift absorbers
considered in this study. The two thicknesses of the spectral shift
absorber coating are shown with respect to the effects the coating
had on plutonium-239 transmutation and curium-244 production.
In these tables, negative values indicate the spectral shift absorber
coating improved the transmutation performance of the target
fuel. The ideal coating would result in a value of 100% for both
the curium-244 and plutonium-239.
The highest rates of plutonium-239 and curium-244 transmuta-
tion in the 5 wt% MOX fuel occurred with a 144.25 lm coating
thickness (see Table 5.1). Four of the eleven coatings (B4C, Dy2O3,
Eu2O3, and In2O3) applied to the MOX target fuel significantly
increased the curium-244 transmutation rate. The best perfor-
mance was achieved with a coating of indium oxide, which
reduced the production of curium by 39% with a 13% decrease in
the rate of destruction of plutonium-239, compared to the
uncoated 5 wt% MOX fuel. The dysprosium oxide coating resulted
in a 17% reduction in curium-244 production with a 27% reduction
in plutonium-239 destruction. A coating of europium oxide
achieved nearly the same curium-244 reduction as the dysprosium
oxide coating but at a higher cost to the rate of plutonium-239
transmutation, 34%. The final significant improvement in curium-
244 production was a 12% reduction with a boron carbide coating
but also with a significant penalty, 37%, to the plutonium transmu-
tation fraction. The hafnium oxide coating was the only coating
which resulted in the net production of curium-244.
A 4.25 lm coating thickness had minor impacts on the rates of
plutonium and curium transmutation with the 5 wt% MOX fuel
(see Table 5.1). The most significant difference between the fuel
with a 4.25 lm coating thickness and the uncoated fuel is a
2.62% increase in curium-244 destruction with the In2O3 coating.
The 4.25 lm In2O3 coating decreased the plutonium-239 transmu-
tation by 0.22%. Of the thin coatings, this is the most significant
reduction in curium production. The remainder of the coatings,
aside from HfO2, reduced the production of curium-244 by less
than 1%. Interestingly, the thin HfO2 coating resulted in the MOX
fuel producing curium-244 at a higher rate than the thicker coat-
ing, a 1.03% increase, but also transmuted plutonium-239 at a
higher rate than the thicker coating.
The 144.25 lm coating thickness on the 60 wt% thorium pluto-
nium zirconium hydride resulted in greater rates of transmutation
than the thin coating (see Table 5.2). The greatest difference in the
coated and uncoated version of the fuel resulted from the In2O3
coating. The 144.25 lm In2O3 coating resulted in a 30% reduction
in curium-244 production as well as a 17% reduction in the rate
of plutonium-239 transmutation. The second greatest reduction

Table 5.1
5 wt% MOX target fuel coating results (percent difference from uncoated target fuel).

SSA Cm-244 (4.25 lm) Pu-239 (4.25 lm) Cm-244 (144.25 lm) Pu-239 (144.25 lm)
B4C 0.28% 0.69% 12.45% 37.26%
CdO 0.04% 0.14% 2.58% 9.33%
Dy2O3 0.71% 0.72% 17.25% 26.56%
Er2O3 0.08% 0.18% 2.89% 7.60%
Eu2O3 0.48% 0.62% 15.90% 34.01%
Gd2O3 0.08% 0.18% 6.90% 19.07%
HfO2 1.03% 0.22% 0.32% 3.11%
In2O3 2.62% 0.22% 39.06% 13.21%
Lu2O3 0.28% 0.14% 8.01% 4.59%
Sm2O3 0.52% 0.04% 0.83% 9.48%
TaC 0.16% 0.00% 2.42% 2.32%
70 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72

Table 5.2
60 wt% thorium plutonium zirconium hydride target fuel coating results (percent difference from uncoated target fuel).

SSA Cm-244 (4.25 lm) Pu-239 (4.25 lm) Cm-244 (144.25 lm) Pu-239 (144.25 lm)
B4C 0.23% 1.36% 9.03% 54.35%
CdO 0.05% 0.35% 1.41% 16.74%
Dy2O3 0.64% 1.22% 13.76% 36.96%
Er2O3 0.08% 0.35% 2.32% 12.39%
Eu2O3 0.40% 1.27% 11.65% 48.91%
Gd2O3 0.62% 4.58% 4.03% 32.07%
HfO2 0.53% 0.48% 0.87% 9.24%
In2O3 2.56% 0.51% 30.10% 16.96%
Lu2O3 0.25% 0.33% 6.03% 8.67%
Sm2O3 0.31% 0.46% 1.24% 20.33%
TaC 0.19% 0.22% 3.38% 5.67%

Table 5.3
8 wt% PuZrO2MgO target fuel coating results (percent difference from uncoated target fuel).

SSA Cm-244 (4.25 lm) Pu-239 (4.25 lm) Cm-244 (144.25 lm) Pu-239 (144.25 lm)
B4C 0.32% 1.67% 12.49% 94.42%
CdO 0.04% 0.37% 2.63% 23.93%
Dy2O3 0.75% 1.70% 17.57% 65.21%
Er2O3 0.07% 0.43% 2.95% 17.15%
Eu2O3 0.50% 1.69% 16.15% 89.68%
Gd2O3 0.18% 1.08% 6.83% 49.38%
HfO2 0.78% 0.67% 0.57% 14.33%
In2O3 2.45% 0.63% 37.14% 28.93%
Lu2O3 0.28% 0.39% 7.86% 11.52%
Sm2O3 0.50% 0.51% 1.39% 31.12%
TaC 0.18% 0.24% 2.60% 6.61%

in curium-244 production, 14%, resulted from a Dy2O3 coating, but
this coating also reduced the plutonium-239 transmutation rate by
37% compared to an uncoated fuel. A 144.25 lm coating of Eu2O3
reduced the production of curium-244 by 12% but resulted in a 49%
reduction in the rate of plutonium-239 transmutation. In contrast
to the coating on the 5 wt% MOX fuel, the HfO2 coating did not
result in an increase in the rate of curium-244 production.
A thin (4.25 lm) coating on the 60 wt% thorium plutonium
zirconium hydride fuel resulted in small changes in the transmuta-
tion rates similar to the 5 wt% MOX fuel, with a few interesting
exceptions (see Table 5.2). The In2O3 coating resulted in the
greatest reduction in curium-244 production, 2.56%, with a small
decrease in plutonium-239 transmutation, 0.51%. Both the Gd2O3
and HfO2 coatings resulted in an increase in the rate of production
of curium-244, 0.62%, and 0.53%, respectively. While the HfO2
coating continued to reduce the rate of plutonium-239
transmutation by 0.48%, the Gd2O3 coating actually increased the
rate of plutonium transmutation by 4.58% compared to the
uncoated fuel.
The 144.25 lm coating thickness on the 8 wt% PuZrO2MgO fuel
resulted in patterns similar to the other two fuel types evaluated in
this portion of the study (see Table 5.3). The In2O3, Dy2O3, and
Eu2O3 coatings resulted in the highest reduction in curium-244
production. A coating of In2O3 reduced the rate of curium-244 pro-
duction by 37% with a decrease in the rate of plutonium-239 trans-
mutation by 29%. The Dy2O3 and Eu2O3 coatings resulted in similar
reductions in the rate of curium-244 production, 18% and 16%,
respectively, with significant differences in the rate of
plutonium-239 transmutation, 65% and 90%, respectively. The high
reduction in plutonium-239 transmutation with the Dy2O3 and
Eu2O3 coatings indicates that the spectral shift absorbers pre-
vented the majority of the neutrons from reaching the underlying
fuel.
The 4.25 lm coating thickness on the 8 wt% PuZrO2MgO fuel
resulted in changes similar to that of the coated 60 wt% thorium
plutonium zirconium hydride fuel (see Table 5.3). The In2O3
coating resulted in the greatest reduction in curium-244 produc-
tion, 2.45%, with a 0.63% decrease in the plutonium-239 transmu-
tation rate. The Gd2O3 coating resulted in an increase in the rate of
plutonium-239 transmutation by approximately 1% with a mini-
mal increase in curium-244 production, 0.18%. The HfO2 coating
resulted in an increase in the rate of production of curium by less
than 1%.
Of the eleven spectral shift absorbers evaluated in this study,
the In2O3 coating resulted in the largest average decrease in cur-
ium production with the smallest average loss in plutonium trans-
mutation. Although the Dy2O3 and Eu2O3 coatings resulted in the
second and third highest average reduction in curium production,
the loss of plutonium transmutation prevents them from being
ideal spectral shift absorber coatings for the purposes of this study.
Though the thicker coatings of Gd2O3 tended to heavily shield the
fuel, the thinner coatings resulted in an increase in plutonium
transmutation, and, thus Gd2O3 is the second choice for a spectral
shift absorber coating on the evaluated transmutation fuels.
6. Summary and conclusions
This paper evaluated sixteen different fuel compositions, with
and without minor actinide (neptunium, americium, and curium)
additions, for the transmutation of plutonium and minor actinides
in a modified AP1000 17  17 Robust Fuel Assembly as a near-term
solution to the disposition of plutonium and minor actinides. The
fuels evaluated in this study consist of MOX, PuO2, Pu3Si2, PuN,
PuUZrH, PuZrH, PuZrHTh, and PuZrO2. The target fuel rods were
evaluated with and without minor actinides to determine an opti-
mal fuel type for actinide transmutation. The ratio of minor acti-
nides added to each fuel type was proportional to the ratio of
americium, neptunium, and curium found in an average PWR fuel
assembly with a burnup of 41200 MWd/MTHM at 3.75 wt% enrich-
ment after 23 years of decay. A fuel rod of each fuel type was
placed in the central instrumentation channel of the AP1000 fuel
 J. Washington et al. / Nuclear Engineering and Design 313 (2017) 53–72
assembly. The fuel compositions were evaluated for the depletion
of fissile plutonium and minor actinides, as well as for the produc-
tion of plutonium-240 and plutonium-242 which increase prolifer-
ation resistance. The evaluation considered 1400 effective full
power days of energy production at 21.66 MWth per assembly in
order to compare each fuel on a similar basis.
The addition of minor actinides to the target fuels results in a
decrease in the rate of plutonium destruction by an average of
16 wt%. Various minor actinides react differently to different levels
of initial plutonium concentration, which produces a method for
tuning minor actinide transmutation rates. In all of the cases con-
taining initial minor actinide, the overall mass of the minor acti-
nides decreases, though the mass of specific minor actinide
isotopes may increase. The minimum decrease in minor actinide
mass was 7.23 wt% in the plutonium oxide case and the maximum
decrease in minor actinide mass was 33.29 wt% in the 8 wt%
PuZrO2MgO case.
The MOX fuels transmuted an average of 28.06 wt% of the minor
actinides and 26.47 wt% of the plutonium. The 7 wt% MOX fuel
transmuted the greatest quantity of plutonium (27.39 wt%) and
the 5 wt% MOX fuel transmuted the greatest quantity of minor acti-
nides (27.39 wt%). These MOX fuels also have the benefit of being
much more familiar to the nuclear industry than any of the other
fuel types in this study. The PuUZrH with minor actinide fuel had
the next highest percentage of transmutation when considering
both minor actinides (30.65 wt%) and plutonium (34.29 wt%). The
inert matrix fuels, specifically the 8 wt% PuZrO2MgO target fuel
with minor actinide, transmuted the greatest percentage of the ini-
tial minor actinides (43.73 wt%) and plutonium (33.29 wt%). These
fuels contained the smallest quantity of actinides and produced the
greatest reduction in both minor actinide and plutonium mass.
In comparison to a uranium oxide fuel pin, the zirconium oxide
inert matrix fuels were the only fuels that resulted in a decrease in
total activity of the target fuel rod under similar irradiation condi-
tions. The end of life activity for the 8 wt% PuZrO2MgO with minor
actinide target fuel was 1.04  104 TBq compared to 1.73  104
TBq for a uranium oxide target fuel rod. The 8 wt% PuZrO2MgO tar-
get fuel achieved the greatest reduction in minor actinides and plu-
tonium concentrations over a 1400 EFPD irradiation period, as well
as having the lowest end-of-life activity of any of the fuels evalu-
ated in this study.
Three of the target fuels, 5 wt% MOX, 60 wt% thorium pluto-
nium zirconium hydride, and 8 wt% PuZrO2MgO, were evaluated
with a variety of spectral shift absorber coatings, including B4C,
CdO, Dy2O3, Er2O3, Eu2O3, Gd2O3, HfO2, In2O3, Lu2O3, Sm2O3, and
TaC. These simulations revealed that improvements in the trans-
mutation rates of plutonium and minor actinides are possible with
the correct application of a spectral shift absorber. Unlike previous
research these coatings are not used as burnable absorbers but to
tune the neutron energy spectrum observed by the target fuels
for the purposes of improvement in transmutation properties. In
these simulations, an indium oxide coating of 144.25 lm provided
the greatest improvement in transmutation rates. The indium
oxide coating produced a reduction in the production of curium-
244 by 30–39% in the 5 wt% MOX, 60 wt% plutonium thorium zir-
conium hydride, and the 8 wt% PuZrO2MgO fuels with a reduction
of 13–30% in the overall rate of plutonium transmutation. While
not as effective as In2O3, Gd2O3 is a potential second choice as a
spectral shift absorber coating on the transmutation fuel rods.
Future work entails the use of these target fuels and the
spectral shift absorber coatings in more advanced simulations.
The fuels and coatings will be evaluated in multiple pin configura-
tions with the objective of optimizing the reduction in plutonium
and the transmutation of minor actinides. Evaluation of these fuels
and coatings in a test reactor environment is not planned at this
time.
71
Acknowledgements
Jeremy Washington was supported by a Colorado School of
Mines Nuclear Science and Engineering Fellowship with funding
provided by the U.S. Nuclear Regulatory Commission under grant
number NRC-38-10-952.
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