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Annals of Nuclear Energy 77 (2015) 74–82

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Annals of Nuclear Energy


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Minor actinide transmutation on PWR burnable poison rods


Wenchao Hu a,b, Bin Liu a,b,⇑, Xiaoping Ouyang a,c, Jing Tu c, Fang Liu a,b,c, Liming Huang a,b, Juan Fu a,b,
Haiyan Meng a,b
a
School of Nuclear Science & Engineering, North China Electric Power University, Beijing 102206, China
b
Beijing Key Laboratory of Passive Safety Technology for Nuclear Energy, Beijing 102206, China
c
Northwest Institute of Nuclear Technology, Xian, Shanxi 710024, China

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

Article history: Minor actinides are the primary contributors to long term radiotoxicity in spent fuel. The majority of
Received 18 August 2014 commercial reactors in operation in the world are PWRs, so to study the minor actinide transmutation
Received in revised form 22 October 2014 characteristics in the PWRs and ultimately realize the successful minor actinide transmutation in PWRs
Accepted 29 October 2014
are crucial problem in the area of the nuclear waste disposal. The key issues associated with the minor
Available online 22 November 2014
actinide transmutation are the appropriate loading patterns when introducing minor actinides to the
PWR core.
Keywords:
We study two different minor actinide transmutation materials loading patterns on the PWR burnable
Minor actinides
Transmutation
poison rods, one is to coat a thin layer of minor actinide in the water gap between the zircaloy cladding
Pressurized water reactor and the stainless steel which is filled with water, another one is that minor actinides substitute for burn-
Burnable poison rod able poison directly within burnable poison rods. Simulation calculation indicates that the two loading
patterns can load approximately equivalent to 5–6 PWR annual minor actinide yields without disturbing
the PWR keff markedly. The PWR keff can return criticality again by slightly reducing the boric acid
concentration in the coolant of PWR or removing some burnable poison rods without coating the minor
actinide transmutation materials from PWR core. In other words, loading minor actinide transmutation
material to PWR does not consume extra neutron, minor actinide just consumes the neutrons which
absorbed by the removed control poisons.
Both minor actinide loading patterns are technically feasible; most importantly do not need to modify
the configuration of the PWR core and composition of nuclear fuel. Furthermore, the two minor actinide
loading patterns completely isolate minor actinide transmutation materials from nuclear fuel, so it also
facilitates fuel reprocessing after discharged from PWR core. We believe that loading minor actinide to
PWR burnable poison rods for transmutation is an optimal minor actinide loading pattern.
Ó 2014 Elsevier Ltd. All rights reserved.

1. Introduction Approximately 0.4 wt% of spent fuel mass is in the form of long
lived fission products cesium, strontium, technetium, and iodine;
Production of electric energy by nuclear reactors entails pro- About 1 wt% of spent fuel composed of plutonium and minor acti-
duction of plutonium and radioactive nuclear waste. A typical nide isotopes (Madic et al., 2007).
1000 MW (e) pressurized water reactor (PWR) generates about Despite their relatively small fractions in spent fuel, transuranic
20–30 tons of spent fuel per year. The basis of environment con- elements such as plutonium, neptunium, americium, and curium,
cern lies in whether the harmful components of these nuclear are the primary contributors to long term radiotoxicity and long
wastes can be isolated from the biosphere for at least tens of thou- term heat generation in spent fuel. Nuclear transmutation is the
sands of years or even longer. Most of the spent fuel (generally conversion of one chemical element or isotope into another. In
more than 98.5%) is composed of uranium and short lived fission other words, atoms of one element can be changed into atoms of
products, which do not pose a long term radiological hazard. other element by transmutation. This occurs either through
nuclear reactions, or through radioactive decay. The nuclear trans-
mutation is the only way to reduce the radioactive hazard of the
⇑ Corresponding author at: School of Nuclear Science & Engineering, Campus
high level long-lived radioactive minor actinides (MA) and long
Box 78, North China Electric Power University, Beijing 102206, China. Tel.: +86 10
61773174; fax: +86 10 61773156. lived fission products (LLFP) to our environment. Transmutation
E-mail address: Liu_Bin@ncepu.edu.cn (B. Liu). of neptunium, americium, and curium has the potential to help

http://dx.doi.org/10.1016/j.anucene.2014.10.036
0306-4549/Ó 2014 Elsevier Ltd. All rights reserved.
W. Hu et al. / Annals of Nuclear Energy 77 (2015) 74–82 75

solve the problems posed by the management of radioactive waste The study shows that the cross sections of the MA nuclides in
by reducing the proportion of long-lived isotopes it contains. In the thermal energy regions are much greater than in the fast
transmutation of the minor actinides in the depleted reactor fuel neutron energy regions (Iwasaki, 2002; Iwasaki and Hirakawa,
the intention is to convert the minor actinides into fission products 1994; Sohail et al., 2014). As a matter of fact, Np-237, Am-241
or some useful transuranic materials. The fission products are also and Am-243 have very large thermal neutron capture cross sec-
very radioactive, but the majority of the activity will decay away tions in the thermal energy region, these MA nuclides can capture
within a short time. By doing so, people may converse minor neutrons and become Pu-239, Am-242m, Cm-243 and Cm-245
actinides and LLFPs to some useful materials or short lived radioac- which have very large fission cross sections. Minor actinides may
tive materials, at the same time people may make use of the energy be transmuted in the thermal rectors very effectively, so people
released from the nuclear transmutation to generate power (Liu should consider transmuting MA nuclides in the pressurized water
et al., 2014). reactors seriously.
Although thermal reactors (Liu et al., 2014; Shwageraus et al., Liu et al. studied the minor actinide transmutation characteris-
2004), fast reactors (Meiliza et al., 2008; Nishihara et al., 2010), tics in the high flux thermal reactor (Liu et al., 2013). As the neu-
subcritical reactor (Ismailov et al., 2013; Yapici et al., 2008) all tron flux in the high flux thermal reactors can parallel the
can be used to transmute the minor actinides and LLFPs, only the neutron flux in the fast reactors and the MA nuclides have very
technology of thermal reactors is mature, the majority of commer- large thermal neutron capture cross sections in the thermal energy
cial reactors in operation in the world are pressurized water reac- region, their simulation calculation results show that the transmu-
tors, so to study the minor actinide transmutation characteristics tation rate of the minor actinides in the high flux thermal reactors
in the pressurized water reactors are crucial problem in the area can match that of in the fast reactors. Their simulation calculation
of the nuclear waste disposal. Actually, tremendous research works results also indicate that the MA nuclides actually can act as the
about the transmutation of minor actinides and LLFPs in different burnable poisons in the thermal reactors; this is a distinct advan-
types of reactors have been done in the past a couple of decades, tage to transmute the MA nuclides in the high flux thermal reactor.
these research works mainly focus on comparing the transmuta- However, to build a high flux thermal reactor just to transmute
tion characteristics of MA and LLFPs in different types of reactors, minor actinides or other nuclear wastes is economically unfeasible.
that is to compare the advantage and disadvantage of the To achieve a good economy in the transmutation of MA nuclides,
transmutation characteristics of MA and LLFPs in different types the reactors should transmute minor actinides and generate power
of reactors (Artisyuk et al., 2005; Beller et al., 2001; Herrera- simultaneously.
Martnez et al., 2007; Iwasaki and Hirakawa, 1994; Takeda et al., Liu et al. also studied the minor actinide transmutation charac-
2002; Wakabayashi, 2002). Up to present, very few research works teristics in the pressurized water reactors (Liu et al., 2014). They
about the transmutation of MA and LLFPs come right down to the calculated the effects to keff after adding the MA nuclides to PWR
specific loading pattern of MA and LLFPs in the in different types of core in uniform distribution with fuel and in the transmutation
reactors. However, finding an optimal MA and LLFP loading pattern rod form. Their calculation results denote that, except to reducing
in a reactor is a successful starting point of whole research works the initial reactivity significantly, the uniform distribution of MA
of MA and LLFP transmutation in a specific reactor. A popular say- nuclides in the uranium dioxide fuel may also affect the lifetime
ing is that the MA and LLFPs transmutation rate in thermal reactors of a fuel cycle. Their calculation results also denote the uniform
is far less than that of in the fast reactors and the subcritical reac- distribution of MA nuclides in the uranium dioxide nuclear fuel
tors, so to study the transmutation characteristics of MA and LLFPs results in a reactivity mismatch and control difficulties in PWRs.
in thermal reactors is meaningless, this conclusion is based on the Although MA nuclides uniform distribution with fuel in PWR core
argument that the neutron flux in the thermal reactors is much less may transmute the MA nuclides effectively, the unfavorable effects
than the neutron flux in the fast reactors and the subcritical reac- to PWR core after adding MA nuclides uniform to the fuel are the
tors. However, the majority of commercial reactors in operation in significant disadvantages. Obviously adding the MA nuclides uni-
the world are pressurized water reactor, i.e., the thermal reactors. form with fuel in PWR core is not a right choice to transmute the
Subcritical reactor is a future reactor; we are uncertain whether its MA nuclides in PWR. Their calculation result also denotes that
destiny is similar to fusion reactors or fast reactors. At present, we the spatial self-shielding effects of the heterogeneous distributions
are certain that subcritical reactor will not operate commercially to of MA nuclides in the PWR core can avoid the initial reactivity to
provide us power within at least a couple of decades, it is unneces- drop significantly after adding MA nuclide transmutation materials
sary to mention that the subcritical reactor can transmute nuclear to the PWR core, in this way, the reactivity mismatch and control
wastes for us. Although the first electric power generating nuclear difficulties in the PWRs can be also overcome. But the total trans-
reactor was fast reactor (Walters, 1999) and several countries built mutation rate on transmutation rod average is very low due to the
19 fast reactors (most of the fast reactors are experimental fast spatial self-shielding effects, only the MA nuclides on the surface of
reactor) for the past several decades, there are almost no commer- transmutation rod are transmuted, so to introduce the MA nuclides
cial fast reactors operation in the world in a long period of time, in PWR core in this heterogeneous distribution, that is in transmu-
this may come from fact that people worry about the safety of fast tation rod form, is also unfeasible.
reactor operation and the extravagant fuel cost. Before fast reactor Yang et al. proposed to transmute the minor actinides and LLFP
can generate the power commercially in large scale as the thermal in the film coating on fuel rods or annular transmutation target to
reactor does, there are still a lot of technologies to break through reduce the self-shielding effects and improve the minor actinides
for fast reactors. So up to now, the thermal reactors, especially and LLFP transmutation rate (Yang et al., 2004). Although Yang’s
the pressurized water reactor, still dominates the power reactor approaches can reduce the self-shielding effects of transmutation
in the world, see Fig. 1 for details (IAEA, 2013). Only the technology rods and improve the transmutation rate greatly, coating a thin
of thermal reactors is mature, the majority of commercial reactors layer of MA or LLFP on the PWR fuel rods will change the structure
in operation in the world are pressurized water reactor, so to study of PWR fuel rods, this needs to completely to upgrade all the PWR
the minor actinide transmutation characteristics in the pressurized fuel rod manufacture technique which has been a pretty mature
water reactors are very important. Probably, at the present time technique for past several decades. So Yang’s approach to trans-
the commercial PWR reactors are the only choice to transmute mute the MA and LLFP in the film coating on fuel rods or annular
the nuclear wastes in large scale. transmutation target still lacks of feasibility in the transmutation
76 W. Hu et al. / Annals of Nuclear Energy 77 (2015) 74–82

Fig. 1. Total nuclear reactor number and type in the World (2013).

of minor actinides in the reactors in the large scale and China Guangdong Daya Bay 900 MW PWR core which includes the
economically. distribution pattern of the fuel assemblies. Table 1 lists the key
No matter which ways to introduce the MA to PWR reactor parameters of the fuel assemblies of this 900 MW PWR. All the fuel
cores, MA uniform distribution with fuel, heterogeneous distribu- assemblies are the typical 17  17 PWR fuel assemblies, every fuel
tions in the reactor core or film coating MA on fuel rods, all these assembly has 264 fuel rods, 24 control rod guide tubes and 1 neu-
approaches need either to change the composition of the fuel, con- tron detector guide tube. For easy calculation, all the fuel assemblies
figuration of the reactor core or the structure of the fuel rods. All have the same U-235 enrichment 2.1%.
these modifications to the reactor core will change the physical The reactor with the first fuel loading has very large excess
characteristics of the reactor, and all these changes need to make reactivity, to ensure the moderator temperature coefficient is neg-
modifications on the well proven thermal reactor core design tech- ative during PWR operation, the boron concentration is not
nology. So the cost to rebuild a thermal reactor core to transmute allowed too high, therefore some burnable poison rods with strong
the MA or LLFP may be tremendously and impractically. To avoid neutron absorption ability are arranged in 66 fuel assemblies to
the above problems in transmutation of the MA in the thermal balance reactivity. 48 fuel assemblies with 12 burnable poison rods
reactors, in this paper we study the minor actinide transmutation and 18 fuel assemblies with 16 burnable poison rods are included
characteristics in the pressurized water reactors by loading the in the PWR core, specific arrangement of the MCNP4C simulated
MA transmutation materials in the PWR burnable poison rods. In PWR core is shown in Fig. 2. The distribution patterns of burnable
doing so, people do not need to change the composition of the fuel, poison rods in the different fuel assemblies are shown in Fig. 3. The
configuration of the reactor core or the structure of the fuel rods at cutaway view of a typical burnable poison rod is shown in Fig. 4.
all. We combine the conventionally well developed thermal reactor Based on the parameters in Table 1, we use MCNP code to sim-
design technology with MA transmutation technology to simulate ulate a PWR core to study the transmutation characteristics of the
the MA transmutation characteristics in the pressurized water China Daya Bay 900 MW PWR after minor actinide transmutation
reactor by MCNP code. We concentrate on studying the effects to materials loaded to the burnable poison rods of PWR. We assume
PWR reactor keff after adding minor actinides to PWR burnable poi- all the control rods are completely withdrawal from the PWR core
son rods and try to find an optimal minor actinide transmutation in MCNP simulation calculation. The initial reactivity is 1.0108
material loading pattern within PWRs. which means the PWR core is in criticality. The initial concentra-
tion of the boric acid in the coolant is 1074 ppm. The abundance
of boron-10 in boric acid is 20%.
2. The minor actinide transmutation on PWR burnable poison
rods
3. Coating a layer of minor actinides in the water gap of
We establish a PWR MA transmutation core by using MCNP4C burnable poison rods
code (Briesmeister, 2000). MCNP code has criticality calculation
feature for critical systems (Liu et al., 2010). We use MCNP4C code 3.1. Design of minor actinide transmutation rods
to study MA transmutation characteristics in the pressurized water
reactors after minor actinide transmutation materials are loaded In MCNP4C simulation calculation, all MA nuclides in the ratio
on PWR burnable poison rods. that is the same as MA nuclides ratio in the thermal reactor
depleted fuel, see Table 2 for details. The ratio of each MA nuclide
2.1. The configuration of PWR transmutation core in Table 2 is based on a 3 GW thermal power from which an annual
33 tons of fuel with a burnup of 33,000 MWd/t, cooling for 10 years
We simulate reactor core of China Guangdong Daya Bay 900 MW (Broeders et al., 2000).
pressurized water reactor (Su and Yang, 2005) to study the MA As the PWR has been operated for several decades, its technol-
transmutation characteristics. Fig. 2 depicts the configuration of ogy has been demonstrated and verified is mature and reliable. We
W. Hu et al. / Annals of Nuclear Energy 77 (2015) 74–82 77

Fig. 2. The arrangement of burnable poison rod assemblies in PWR core.

cladding and the stainless steel which is filled with water (water
Table 1
The key parameters of fuel assembly.
gap), we let MA transmutation materials fill part of this water
gap as shown in the Fig. 5. In the Fig. 5, the outer diameter of
Fuel assembly type 17 * 17 MA transmutation materials is 0.5525 cm and inner diameter is
Number of fuel rods 264
Number of guide tubes 25
0.49 cm, the space between the zircaloy cladding and MA transmu-
Outer diameter of clad (mm) 9.5 tation materials still filled with water.
Thickness of clad (mm) 0.57 This PWR transmutation core contains 41,488 fuel rods, and the
Fuel pellet diameter (mm) 8.19 diameter of fuel rod is 0.819 cm, the density of UO2 is 10.2 g/cm3. A
Material of clad Zircaloy
PWR can load about 81.55 tons UO2 nuclear fuel based on our
Fuel pellet pitch (mm) 13
Outer diameter of guide tubes (mm) 12.2 MCNP calculation. To reduce the complexity of the simulation cal-
Inner diameter of guide tubes (mm) 11.2 culations, the MA transmutation materials are loaded in all the fuel
assemblies with burnable poison rods. 8 Burnable poison rods with
MA transmutation materials substitute for 8 burnable poison rods
without MA transmutation materials in all the fuel assemblies with
load the MA nuclides in the burnable poison rods to study the MA 12 burnable poison rods and 16 burnable poison rods, as shown in
transmutation characteristics in the PWR, in this way we can avoid Figs. 3 and 6. We use MCNP code to model this MA transmutation
to alter the PWR core configuration, fuel rod structure or the com- PWR core and to calculate the MA loading capacity and PWR keff. To
position of the fuel rods which have been well proven for several study the effects to the PWR core, we fix inner radius of the MA
decade PWR operation experience. In comparison with the other transmutation materials in 0.49 cm, and calculate the PWR keff as
MA or LLFP transmutation material loading pattern to the PWR the outer radii are 0.495 cm, 0.5 cm, 0.51 cm, 0.52 cm, 0.53 cm,
core (Liu et al., 2014, 2013; Yang et al., 2004), we believe loading 0.54 cm, 0.55 cm, respectively, the calculation results are listed in
MA transmutation materials in the PWR burnable poison rods is Table 3.
more feasible and is a promising minor actinide transmutation The calculation results listed in Table 3 indicate that as the coat-
material loading pattern. ing thickness increases, the total loading amount of MA transmuta-
In the investigation on loading MA transmutation materials in tion materials also increases, the PWR initial reactivity drops
the PWR burnable poison rods, we just need to modify the struc- correspondingly, we need to increase the enrichment of the reactor
ture of burnable poison rod slightly, in this way we can minimize fuel, reduce the boric acid concentration in the coolant or remove
changes of PWR structure and maximize the transmutation rate some burnable poison rods from PWR core to let the PWR return
when loading the MA transmutation materials in PWRs. From Fig criticality. Therefore we can conclude, after adding MA nuclides
4 we can see, there is an empty space between the zircaloy to the core of the PWR reactor, MA nuclides consume a lot of
78 W. Hu et al. / Annals of Nuclear Energy 77 (2015) 74–82

Fig. 3. The distribution of 12 and 16 burnable poison rods in fuel assembly.

MA nuclide transmutation materials can be used to partially


substitute for the burnable poisons in the PWRs, reduce the con-
centration of the boric acid in the coolant of the PWRs and increase
the negative temperature coefficient of the PWRs, all these mea-
sures can dramatically reduce the possibility of the critical accident
in a fuel cycle. This is a distinct advantage to transmute MA nuc-
lides in the PWRs.

3.2. Minor actinide partial substitution for boric acid

In a PWR reactor, very slow but ultimately very large changes in


reactivity is made by adjusting the boric acid concentration which
dissolved in the coolant. This is so called chemical shim control.
Since the boric acid distribution is uniform in the coolant and is
independent of the amount of reactivity being controlled, the fuel
Fig. 4. The cutaway view of a burnable poison rod.
loading can be more easily distributed to yield a uniform power
distribution. Chemical shim control reduces the mechanical con-
trol rod requirement quite considerably. However, chemical shim
control has a major effect on the moderator temperature coeffi-
Table 2
The ratio of MA nuclides in MCNP simulation calculation. cient of reactivity. In PWR, this effect on the moderator tempera-
237 241 243 244 245
ture coefficient of reactivity is usually quite negative, since the
Nuclides Np Am Am Cm Cm
injection of the boric acid to the coolant means that the decrease
Percentage (%) 41.8 47.86 8.62 1.63 0.09 in coolant density, this further leads to a decrease in neutron mod-
eration and hence reactivity. However if a soluble poison is pres-
ent, a decrease in coolant density will also lead to a decrease in
poison concentration, a positive reactivity effect. Therefore, our
desire for a negative temperature coefficient will limit the amount
of boric acid allowed in the primary coolant.
As minor actinides behave as control poisons in some ways in
the thermal reactors (Liu et al., 2014), after loading minor actinide
transmutation material to PWR, we definitely need to reduce the
boric acid concentration in the coolant to compensate some the
reactivity decrease induced by minor actinide nuclides. To study
the actually amount of the boric acid concentration in the coolant
can be reduced after coating a different thickness of minor actini-
des on PWR burnable poison rod water gap, we readjust the boric
acid concentration in the PWR coolant to let the reactor to return
criticality and calculate reduced boric acid concentration in the
coolant. The calculated results are listed in the Table 4.
From the results listed in the Table 4 we can conclude, under the
initial boric acid concentration 1074 ppm, as the minor actinide
Fig. 5. The cutaway view of MA transmutation rod.
coating thickness increases the system keff decreases correspond-
ingly, this indicates that the total minor actinide coating amount
on the PWR burnable poison rods also increases. Likewise, we can
neutrons, MA nuclides actually can act as the burnable poisons in let the PWR keff return criticality by readjusting the boric acid con-
the thermal reactors. In other words, loading minor actinide trans- centration in the coolant of PWR. The more minor actinide is loaded
mutation material to PWR does not consume extra neutron, minor to the PWR, the more boric acid concentration need to be reduced
actinide transmutation material just consumes the neutrons which from the coolant. For instance, when the coating thickness of minor
absorbed by the removed control poisons. actinide is 0.03 cm, i.e. the outer radius of MA transmutation
W. Hu et al. / Annals of Nuclear Energy 77 (2015) 74–82 79

Table 3
The calculation results after coating MA transmutation materials in water gap of burnable poison rods.

Inner radius of MA Outer radius of MA Total MA loading Equivalence to the annual keff Standard deviation
transmutation materials/cm transmutation materials/cm amount/kg MA yield of a PWR 
0.49 0.49 0 0 1.01083 0.00054
0.49 0.495 30.48 0.8 0.98628 0.00053
0.49 0.50 61.27 1.7 0.98436 0.00052
0.49 0.51 123.78 3.4 0.97710 0.00053
0.49 0.52 187.53 5.1 0.97298 0.00053
0.49 0.53 252.52 6.9 0.96986 0.00052
0.49 0.54 318.74 8.7 0.96590 0.00054
0.49 0.55 386.20 10.5 0.96327 0.00053
 
Note: The annual MA yield of a PWR is based on A typical 1000 MW (e) PWR generates 20 to 30 tons of spent fuel per year (Moyer, 2010).

Table 4
Partial Substitution of Minor Actinides for Boric Acid.

Inner radius of MA Outer radius of MA The keff after coating MA on PWR The boric acid concentration after The reduced boric acid
transmutation materials/cm transmutation materials/cm burnable poison rods readjusting keff to criticality concentration (CB)
0.49 0.495 1074 ppm/0.98628 976 ppm/1.01000 98 ppm
0.49 0.50 1074 ppm/0.98436 950 ppm/1.00905 118 ppm
0.49 0.51 1074 ppm/0.97710 885 ppm/1.00983 189 ppm
0.49 0.52 1074 ppm/0.97298 850 ppm/1.00958 224 ppm
0.49 0.53 1074 ppm/0.96986 813 ppm/1.01059 261 ppm
0.49 0.54 1074 ppm/0.96590 790 ppm/1.01059 284 ppm
0.49 0.55 1074 ppm/0.96327 765 ppm/1.01002 309 ppm

materials is 0.52 cm; 224 ppm boric acid concentration must be After introducing minor actinides into PWR core, it can behave
reduced from the PWR primary coolant to let the PWR return as control poisons in some senses in the PWR reactors. Except par-
criticality. From Table 3 we can see that in this situation the total tially substitute for boric acid in the PWR primary coolant to
coating amount of minor actinides on the PWR burnable poison increase the negative temperature coefficient of the PWR, we are
rods is approximately equivalent to 5–6 PWR annual minor actinide confident to believe that minor actinides can also be used to sub-
yields. We can expect that even we just coat minor actinide trans- stitute for burnable poison rods to control the excess reactivity of
mutation materials on the burnable poison rod to outer radius pressurized water reactors.
0.52 cm on all the operation PWRs, this will reduce the worldwide In China Guangdong Daya Bay 900 MW pressurized water reac-
minor actinide inventory dramatically. tor, there are total 66 fuel assemblies with burnable poison rods.
As a result, we may say that loading the minor actinide to the 48 fuel assemblies with 12 burnable poison rods and 18 fuel
PWR is equivalent to introducing extra poisons to PWR system to assemblies with 16 burnable poison rods are included in this
control excess reactivity; we need to remove some control poisons PWR core, see Fig. 2 for detail. The inner radius of the burnable poi-
like boric acid concentration from primary coolant to keep the son rod is 0.2413 cm; the outer radius of the burnable poison rod is
reactor in criticality. This once again indicates that minor actinide 0.4267 cm. To study the possibility of minor actinide transmuta-
can partially substitute for boric acid in the PWR primary coolant tion material substitution for the burnable poison rods, based on
to increase the negative temperature coefficient of the PWR; the the calculation results listed in the Table 3, all the burnable poison
reduction of the boric acid concentration in the primary coolant rods without coating the minor actinide transmutation material
can reduce the possibility of the critical accident in a fuel cycle are removed from the fuel assemblies with 12 burnable poison
of PWR. This is definitely one of distinct advantages to transmute rods and from the fuel assemblies with 16 burnable poison rods,
the minor actinides in the PWR reactors. then we calculate the system keff again. This means that all the fuel
assemblies with burnable poison rods only has 8 burnable poison
3.3. Minor actinide partial substitution for burnable poison rods rods coated with certain thickness minor actinide in the water
gap, see Fig. 6 for detail. The system keff calculation results with
The lifetime of a given PWR core fuel loading is generally 8 burnable poison rods coated with certain thickness minor acti-
determined by sufficient excess reactivity to permit startup and nide transmutation material are listed in the Table 5.
full power operation. The amount of nuclear fuel loaded into the From the calculation results listed in the Table 5 we can clearly
PWR reactor will depend in part on the excess reactivity that can see that when the outer radius of minor actinide transmutation
be compensated for by the reactor control elements. In order to material less than 0.5 cm, the system keff can return criticality after
increase the allowable initial core fuel loading, it is common to removing the burnable poison rods without coating the minor acti-
load into PWR core burnable poisons with high neutron absorption nide transmutation material from the fuel assemblies. If the outer
cross sections that compensate for excess reactivity during the radius of minor actinide transmutation material goes to 0.51 or
early stages of the PWR core lifetime. People choose such burnable 0.52 cm, the system keff slightly below criticality after removing
poisons used in the PWR because they burn out somewhat faster the burnable poison rods without coating the minor actinide trans-
than the fuel burnup, so that later in PWR core life they contribute mutation material from the fuel assemblies, we may reduce a little
negligible negative reactivity. Burnable poisons thus possess bit of boric acid concentration from primary coolant to keep the
several advantages. They increase PWR core lifetime without any reactor in criticality again. Base on above analyses, we once again
decrease in control safety, reduce the amount of control rods conclude that the optimal coating thickness for minor actinide
requirement, and can improve PWR core power distribution if transmutation material in the PWR burnable poison rods is to coat
distributed in PWR core in a proper way. minor actinide to outer radius 0.52 cm. The minor actinide
80 W. Hu et al. / Annals of Nuclear Energy 77 (2015) 74–82

Table 6
The effect on PWR keff of burnable poison.

Inner radius of burnable Outer radius of burnable keff


poison/cm poison/cm
0.2413 0.4267 1.01083
0.2413 0.40 1.01734
0.2413 0.38 1.02152
0.2413 0.36 1.02483
0.2413 0.34 1.03051
0.2413 0.32 1.03609
0.2413 0.30 1.04295
0.2413 0.28 1.04927
0.2413 0.26 1.05595
0.2413 0.2413 1.06565

Fig. 6. Layout of MA transmutation rods in a fuel assembly.


Table 7
The effect on PWR keff of minor actinide.
Table 5
Inner radius of minor actinide/ Outer radius of minor actinide/ keff
Minor actinides substitution for some burnable poison rods.
cm cm
Inner radius of MA Outer radius of MA keff keff after removing 0.2413 0.4267 0.97378
transmutation transmutation some burnable 0.2413 0.40 0.97954
materials/cm materials/cm poison rods 0.2413 0.38 0.98565
0.49 0.495 0.98628 1.00687 0.2413 0.36 0.99211
0.49 0.50 0.98436 1.00287 0.2413 0.34 0.99848
0.49 0.51 0.97710 0.99716 0.2413 0.32 1.00694
0.49 0.52 0.97298 0.99257 0.2413 0.30 1.01431
0.49 0.53 0.96986 0.98811 0.2413 0.28 1.02460
0.49 0.54 0.96590 0.98599 0.2413 0.26 1.03969
0.49 0.55 0.96327 0.98104 0.2413 0.2413 1.06565

transmutation material does not disturb the PWR keff too much in radius of two different materials, the keff of PWR core with burnable
this coating thickness, and the minor actinide coating amount can poison rods filled with minor actinide transmutation material is
reach 5–6 PWR annual minor actinide yields, see Table 3 for detail. always less than that of the PWR core with burnable poison rods
Chemical skim control and the burnable poison control are as filled with burnable poison. This result explicitly indicates that
two most important PWR control mechanisms, they have quite dif- minor actinide can be used in the PWR as control poison in some
ferent control characteristics on the reactor core. To change the sense, and their excess reactivity control ability is stronger than
concentration of boric acid in PWR coolant, we can adjust PWR keff that of the convectional burnable poison. This exhibits that, if the
gradually and continuously. The burnable poison rods symmetri- fissions of minor actinides do not alter the physical characteristics
cally distribute in the fuel assemblies of PWR, therefore just chang- of PWRs dramatically, minor actinide nuclides can be used in the
ing the number of the burnable poison rods in the PWR we are burnable poison rods as the control poisons and can be also trans-
unable to adjust the PWR keff gradually and continuously. We muted in the PWR burnable poison rods simultaneously.
believe that to control PWR keff after coating minor actinide trans- Based on the calculation results listed in Tables 6 and 7, we
mutation materials on PWR burnable poison rods, we need to investigate the feasibility of minor actinide direct substitution for
remove some burnable poison rods without coating minor actinide the burnable poison in the burnable poison rods and try to find
transmutation materials from the PWR core, then change the con- an optimal minor actinide thickness in the burnable poison rods.
centration of boric acid in the PWR coolant to let keff gradually and In this way we also can minimize the modification to the PWR core
continuously to return criticality. configuration and the structure of the PWR burnable poison rods
when loading the minor actinide transmutation material to PWR
for transmutation. We reduce outer radius of the burnable poison
4. The MA direct substitution for burnable poison within (also the inner radius of minor actinide) in the burnable poison rods
burnable poison rods and fill in the gap between stainless steel and burnable poison with
minor actinide transmutation material for all the fuel assemblies
In different to the minor actinide transmutation material fill the which have 12 burnable poison rods or 16 burnable poison rods,
water gap between the zircaloy cladding and the stainless steel as see Figs. 3 and 7 for detail. We calculate PWR keff for different outer
shown in Fig. 5, we further investigate another approach of minor radius of the burnable poison with minor actinide transmutation
actinide transmutation material direct substitution for the burn- material fills the gap between stainless steel and burnable poison
able poison in PWR burnable poison rods. We let the minor actinide step by step, the MCNP code simulation calculation results are
transmutation material direct substitution for the burnable poison listed in the Table 8.
in the burnable poison rods. First we compare the neutron absorp- From Table 8 we can see that as the outer radius of the burnable
tion ability between burnable poison and minor actinide, this abil- poison (also the inner radius of minor actinide) in the burnable poi-
ity also denotes the excess reactivity control ability of two different son rods decreases, this indicates the minor actinide loading
materials. By fixing the inner radius and changing the outer radius amount increases and the burnable poison decreases in the burn-
of burnable poison and minor actinide in burnable poison rod, we able poison rods, the PWR keff drops continuously. Until all the burn-
use MCNP code to calculate the effects of two different materials able poisons in the burnable poison rods are substituted by minor
to PWR keff, the calculation results are listed in Tables 6 and 7. In actinide transmutation materials, the PWR keff becomes 0.97378;
comparison Table 6 with Table 7 we can see that for the same outer we can slightly reduce the boric acid concentration in the coolant
W. Hu et al. / Annals of Nuclear Energy 77 (2015) 74–82 81

are the fissile nuclides, thus after loading minor actinide nuclides
to the PWR they may change the physical characteristics of the
PWR. This is quite different to the transmutation characteristics
of the fission products in the PWRs, because the fission products
do not fission in the PWRs at all.
Because the small delayed neutron fraction of the minor actin-
ides, loading a large amount of MA nuclides into the core of PWRs
may alter the physics characteristics in several ways and threaten
the safety of the reactor. In the transmutation of MA nuclides, the
PWR reactor must remain in criticality condition. This indicates
that the transmutation of minor actinides in PWR reactors would
ultimately be limited by criticality and safety constraints.
There are some similarities between loading plutonium (MOX)
and MA nuclides in a PWR reactor. The delayed neutron fraction
is smaller in Pu-239 than in U-235, the subprompt-critical reactiv-
Fig. 7. The cutaway view of MA transmutation rod of MA direct substitution for the ity range is much less for plutonium-fueled reactors than for only
burnable poison. uranium-fueled reactors; and because the delayed neutron fraction
is much smaller in minor actinides than in plutonium nuclides,
reactors fueled with minor actinides will have an even smaller sub-
Table 8
MA direct substitution for the burnable poison in the burnable poison rods of PWRs.
prompt-critical reactivity range than reactors fueled with pluto-
nium and uranium. From Tables 3 and 8 we can see that the
Inner radius keff after filling minor Total minor Equivalence to the ratio of total weight of MA nuclides to the weight of the fuel of
of minor actinide in burnable actinide annual MA yield
actinide/cm poison rods loading of a PWR 
the PWR will be much less than 1.0% in all the MA loading patterns,
amount/kg this is much less the Pu-239 and Pu-241 ratio in the PWR reactor
0.4267 1.01083 0 0
fueled with MOX fuel, so we predicate that loading less than
0.40 0.99535 223.5 6.2 1.0% minor actinides of total uranium nuclear fuel to PWR core will
0.38 0.98852 381.5 10.6 not dramatically alter the physics characteristics and threaten the
0.36 0.98508 531.4 14.8 safety of the PWR reactor.
0.34 0.98234 673.2 18.7
In despite of loading small fractions of minor actinide nuclides
0.32 0.97998 806.8 22.4
0.30 0.97729 932.4 25.9 to PWRs will not threaten the safe operation of PWR reactors;
0.28 0.97629 1049.9 29.2 we still need to study the effects to PWR power distribution, bur-
0.26 0.97486 1159.3 32.2 nup, fuel cycle length and the moderator reactivity temperature
0.2413 0.97378 1254.2 34.8 coefficient after loading a certain amount of minor actinide trans-
 
Note: The annual MA yield of a PWR is based on A typical 1000 MW (e) PWR mutation materials in PWR burnable poison rods. Especially, we
generates 20 to 30 tons of spent fuel per year (Moyer, 2010). need to know whether minor actinide transmutation materials
can burn out somewhat faster than the fuel burnup as the burnable
poison does in the PWR, so that later in PWR core life they contrib-
to let the reactor return criticality again. From Table 8 we can see ute negligible negative reactivity. All these research works consti-
that even just coating 0.0267 cm thickness minor actinide outside tute crucial part of whole research works of minor actinide
the burnable poison, this denotes that both the inner radius of minor transmutation in PWRs.
actinide and outer radius of burnable poison are 0.4 cm, the PWR keff At this stage, we concentrate on finding an optimal minor acti-
is 0.99535 which is just slightly below the criticality. The minor acti- nide transmutation loading pattern in PWR. Based on the reactivity
nide loading amount can reach 223.5 kg, this is approximately balance at the beginning of cycle calculations, we believe minor
equivalent to 6.2 PWR annual minor actinide yields. actinide transmutation materials fill the water gap of burnable poi-
In summary, we have studied two different minor actinide son rods and minor actinide transmutation material direct substi-
transmutation materials loading patterns on the PWR burnable tution for burnable poison within burnable poison rods are the
poison rods, one is to coat a thin layer of minor actinide in the ideal minor actinide transmutation loading patterns in PWRs.
water gap between the zircaloy cladding and the stainless steel, These two minor actinide loading patterns do not need to modify
the other one is direct substitution for burnable poison within configuration of PWR core, fuel composition and fuel structure,
burnable poison rods. Both loading patterns are technically feasi- we believe these two minor actinide loading patterns are superior
ble; most importantly do not need to modify the configuration of to the other minor actinide loading patterns which they need to
the PWR and composition of nuclear fuel, just need to slightly modify configuration of PWR core, fuel composition or fuel struc-
change the structure of the PWR burnable poison rods. In these ture, etc (Liu et al., 2014, 2013; Yang et al., 2004). As PWR manu-
two different loading patterns the minor actinide transmutation facture technology is a pretty mature technology for past several
materials are completely isolated from nuclear fuel, so it also facil- decades, any modification to the configuration of PWR core, fuel
itates fuel reprocessing after discharged from PWR. No matter composition and fuel structure may ruin its mature technology.
which minor actinide loading pattern in the PWR burnable poison Finding an optimal minor actinide loading patterns in PWRs
rods, it can get a considerable amount of minor actinide loading to constitutes crucial part of whole research works of minor actinide
PWR for transmutation without affecting PWR keff markedly. We transmutation in PWRs, this establishes a successful starting point
believe that loading minor actinides to PWR burnable poison rods and choose a right track of the whole research works of minor acti-
for transmutation is an optimal minor actinide loading pattern. nide transmutation in PWRs.
We would like to reiterate here, although minor actinide nuc-
lides can behave as control poisons in some senses in the PWR 5. Conclusions
reactors, the minor actinide nuclides have large thermal neutron
absorption cross section and after minor actinide nuclides absorb The intension of minor actinide transmutation is to converse
neutrons they may become the new minor actinide nuclides which minor actinides to some useful materials or short lived radioactive
82 W. Hu et al. / Annals of Nuclear Energy 77 (2015) 74–82

materials, at the same time people may make use of the energy can burn out somewhat faster than the fuel burnup as the burnable
released from the minor actinide transmutation to generate power. poison does in the PWR, so that later in PWR core life they
The majority of commercial reactors in operation in the world are contribute negligible negative reactivity. All these research works
pressurized water reactors, so to study the minor actinide trans- constitute crucial part of whole research work of minor actinide
mutation characteristics in the pressurized water reactors are cru- transmutation in PWRs.
cial problem in the area of the nuclear waste disposal. The low
neutron flux is perplexing the PWRs as a perfect neutron source Acknowledgements
to transmute the minor actinide; the key issues associated with
the minor actinide transmutation in PWRs are finding an appropri- This work is supported by China National 863 Project entitled
ate loading pattern to overcome the low neutron flux when intro- Thermal Reactor Transmutation Technology under contract
ducing minor actinides to the PWR core. People can realize number 2013AA051402. This work is also supported by Beijing
transmuting minor actinide in large scale and generating power Higher Education Young Elite Teacher Project.
in PWRs simultaneously.
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