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Nuclear Engineering and Design 330 (2018) 241–249

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Nuclear Engineering and Design


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

Transmutation considerations of LWR and RBMK spent nuclear fuel by the T


fusion–fission hybrid system
R. Plukienėa,⁎, A. Plukisa, L. Juodisa, V. Remeikisa, O. Šalkauskasa, D. Ridikasb, W. Gudowskic
a
Center for Physical Sciences and Technology, Savanoriu 231, LT-02300 Vilnius, Lithuania
b
International Atomic Energy Agency, Vienna International Centre, PO Box 100, 1400 Vienna, Austria
c
KTH (Royal Institute of Technology), AlbaNova University Centre, 106 91 Stockholm, Sweden

A R T I C L E I N F O A B S T R A C T

Keywords: The performance of the fusion–fission hybrid system based on the molten salt (flibe) blanket, driven by a plasma
Fusion–fission hybrid system based fusion device, was analyzed by comparing transmutation scenarios of actinides extracted from the LWR
Incineration of trans-uranium elements (Sweden) and RBMK (Lithuania) spent nuclear fuel in the scope of the EURATOM project BRILLIANT. The IAEA
LWR and RBMK spent nuclear fuel nuclear fuel cycle simulation system (NFCSS) has been applied for the estimation of the approximate amount of
heavy metals of the spent nuclear fuel in Sweden reactors and the SCALE 6 code package has been used for the
determination of the RBMK-1500 spent nuclear fuel composition. The total amount of trans-uranium elements
has been estimated in both countries by 2015. Major parameters of the hybrid system performance (e.g., kscr, keff,
Φn(E), equilibrium conditions, etc.) have been investigated for LWR and RBMK trans-uranium transmutation
cases. Detailed burn-up calculations with continuous feeding to replenish the incinerated trans-uranium material
and partial treatment of fission products were done using the Monteburns (MCNP + ORIGEN) code system.
About 1.1 tons of spent fuel trans-uranium elements could be burned annually with an output of the 3 GWth
fission power, but the equilibrium stage is reached differently depending on the initial trans-uranium compo-
sition. The radiotoxicity of the remaining LWR and RBMK transmuted waste after the hybrid system operation
time has been estimated.

1. Introduction (Salvatores, 2002). The fast reactor technology is one of the most
promising when compared with others at present. Some commercially
When trans-uranium elements (TRU) are removed from the dis- available examples such as BN-600, BN-800 in Russia or FBTR (Fast
charged fuel destined for disposal, the radiotoxic nature of the re- Breeder Test Reactor) in India could be mentioned. Other FBRs (mostly
maining materials drops below that of natural uranium ore within a research) have been built and operated in the United States, the United
period of 500 years (Ewing, 1999). Hence the possibilities of parti- Kingdom, France, the former USSR, India and Japan (Waltar and
tioning and transmutation of the long-lived radioactive waste into Reynolds, 1981). It is true that light-water reactors dominate nuclear
stable or short-lived isotopes, which could then be surface-stored with power today due to nowadays relatively low uranium prices and
the little/no proliferation value, are now under investigation. In addi- availability, lower capital costs (by 25%) compared with fast neutron
tion, TRU elements could serve as fuel for transmutation systems. The reactors, but still in Generation IV reactor initiative three from six GEN
transmutation steps include the reprocessing process, fuel fabrication, IV reactors are of the Fast Reactor (FR) type: Gas-cooled Fast Reactor
management of secondary wastes, etc. and it is likely to be the most (GFR), Sodium-cooled Fast Reactor (SFR), Lead-cooled Fast Reactor
challenging issue to be solved in the sustainable nuclear fuel cycle. (LFR) and Supercritical Water-cooled Reactor (SCWR) (GEN IV, 2016).
These problems are comparable for all types of transmutation systems The latest system has an option for the actinide management based on
since they are related to the specific TRU content of the transmutation the particular core design with the fast neutron spectrum (Oka, 2010).
dedicated fuels (Salvatores, 2009; Yurov and Prikhod’ko, 2014). The The MSFR concept is also recognized as one of Gen IV options because
idea of the “closed” fuel cycle of plutonium/higher actinides and TRU of the compact size and relatively low costs to both build and operate
recycling could be implemented in the future fast neutron systems (less metal is needed to fabricate/maintain and no initial fuel

Abbreviations: ADS, Accelerator Driven System; Flibe, LiF-BeF2-(HN)F4 molten-salt blanket; FP, Fission Products; LWR, Light Water Reactor; MA, Minor Actinides; SNF, Spent Nuclear
Fuel; RBMK, High Power Channel-type Reactor (in Russian abbreviation); TBR, Tritium Breeding Rate; TRU, Trans-Uranium Elements

Corresponding author.
E-mail address: rita.plukiene@ftmc.lt (R. Plukienė).

https://doi.org/10.1016/j.nucengdes.2018.01.046
Received 25 September 2017; Received in revised form 20 January 2018; Accepted 27 January 2018
Available online 20 February 2018
0029-5493/ © 2018 The Authors. Published by Elsevier B.V. This is an open access article under the CC BY-NC-ND license (http://creativecommons.org/licenses/BY-NC-ND/4.0/).
R. Plukienė et al. Nuclear Engineering and Design 330 (2018) 241–249

fabrication, handling, durability, shuffling, transport, reprocessing, or power, a 250 MW power fusion device operating with a deuterium–-
fuel refabrication and radioactive waste management costs), and the tritium fuel cycle is sufficient to provide an external 14 MeV neutron
lesser environmental impact (mine tailings, etc.) (Siemer, 2015). One of source of 9 × 1019 n/s.
the reasons, among others, why GEN IV reactors are considered is the In (Ridikas et al., 2006) we have shown that in spite of very pro-
fact that they are expected to “close” the fuel cycle by significantly mising results on the efficient TRU destruction a significant quantity of
reducing high level waste. The same applies to Accelerator Driven curium isotopes is accumulated, while for the rest of actinides fully
Systems (ADS) and fusion–fission hybrid systems, which are considered equilibrated concentrations are reached. In the parallel paper (Plukiene
by many research organizations. ADS for radioactive waste transmu- et al., 2006) an optimization procedure has been developed in order to
tation and energy production for the first time were proposed by Rubbia determine the optimal fission-blanket composition corresponding to the
(1997)) and Bowman (1992). For implementation of ADS, the spalla- fast incineration rate of all actinides. For this purpose a different fission-
tion target (neutron production) and proton beam optimization are blanket composition (based on Be + F-salt: 14.29% – 6Li + 7Li,
needed together with the development of new spent fuel partitioning 57.14% – Be, 28.57% – F (Be salt)) corresponding to the fast incinera-
technique and materials technology (Henderson, 2011). tion rate of actinides including minor actinides (also Cm isotopes) was
The plasma-based fusion device could provide as intense neutron investigated. In both F-salt and Be + F-salt cases the same incineration
source as a high power accelerator up to 1019 n/s (Cheng, 1998), and rate (1.1 tons/year) of minor actinides was obtained, but Be + F-salt
this does not require very high fusion based reactors (∼200–300 MW showed better hybrid-system performance characteristics and a smaller
thermal would be sufficient for our purposes). One of the attractive actinide mass in the blanket: kscr at 0.82 ± 0.002 and lower fusion
criteria and advantages of the fusion–fission hybrid system is that, the power of 260 MW at equilibrium, which is reached after about 700 d.
same as ADS, it is designed to be always sub-critical. It is still too early However, in the present study we have analyzed feasibility of different
to talk about the self-sustained fusion–fission hybrid system feasibility spent nuclear fuel transmutation options in the fusion–fission hybrid
from the industrial point of view, but we believe that as soon as the system with conventional LiF-BeF2-(HN)F4: 28.57% – 6Li + 7Li,
fusion International Thermonuclear Experimental Reactor (ITER) pro- 14.29% – Be, 57.13% – F (F salt), which is also usually employed in ADS
ject is completed, the demonstration of a molten-salt blanket as a systems analysis (Henderson, 2011). All calculations of the flibe-based
medium for trans-uranium actinides (TRU) for nuclear waste trans- actinide transmutation blanket were made employing the Monteburns
mutation could be possible as one of the applications of the fusion code system (Trellue and Poston, 1999). MCNP (Briesmeister, 2000)
system – the next step for closed the fuel cycle accomplishment. The was used to obtain neutron multiplication factors keff and kscr (com-
progress in the plasma-based fusion device technologies is tangible: the prising the external source neutron input to the total neutron multi-
plasma fusion driver can be designed based on latest progress in the plication factor of the system) of the TRU blanket and also to estimate
construction and operation of the (ITER) (Merola et al., 2014) and EAST the neutron flux.kscr is defined as:
(Experimental Advanced Superconducting Tokamak) (Wu et al., 2011).
There is a growing interest within the fusion community in US re- kscr = (Mn−1)/(Mn−1/ ν ) (1)
visiting the concept of the fusion–fission hybrid reactor (Freidberg and
Kadak, 2009; Kotschenreuthera et al., 2009). Ambitious plans have where ν – is the average number of neutrons per fission and Mn is a total
been set up to generate more than 200 GWe of nuclear power in China neutron multiplication factor of the system.
in 2050 and a fusion-driven subcritical system concept based on viable In the scope of the EURATOM project BRILLIANT, which has been
technologies has been proposed (Wu et al., 2009, 2011). This system is initiated to identify the barriers for developing nuclear power in the
expected to recycle nuclear waste making the energy production more Baltic region countries and to prepare the basis for overcoming them,
environmentally friendly. the alternative of closed fuel cycle technologies instead of the open
The main parameters defining the transmutation process are the cycle with the spent nuclear fuel (SNF) disposal has been analyzed. One
neutron energy spectrum and neutron fluxes of the system. In principle, of the project objectives is to identify the milestones for the develop-
any intensive neutron source can be used for waste transmutation ment of the sustainable nuclear fuel cycle using the transmutation
(Slessarev and Bolov, 2003). The more intensive neutron flux de- technology. The main aim of the work is considerations of the feasi-
termines a shorter lifetime of a certain nucleus in the system flux. On bility study of waste transmutation in the epithermal-fast neutron flux
the other hand, transmutation depends on the neutron capture and the of this hybrid system by comparing transmutation scenarios of actinides
neutron-induced fission cross sections. A unique solution is impossible extracted from the LWR (Sweden) and RBMK (Lithuania) spent nuclear
because the capture and fission cross sections vary considerably from fuel in the scope of the EURATOM project BRILLIANT. This research
one isotope to another. Looking for a new efficient and economically was done from the point of view of the reactor core physics and of the
viable transmutation system the main consideration is given to the isotopic composition of the fuels which would ensure at least the the-
neutron flux and spectrum characteristics of a particular system oretical part of the transmutation feasibility. In particular, the trans-
(Salvatores, 2002) as well as the interaction of this neutron flux with mutation scenario of TRU elements has been simulated by using the
the given composition of transmutable material. model of the fusion–fission hybrid system for different spent nuclear
For the fusion–fission hybrid system both the materials and tech- fuels accumulated in the Baltic countries: RBMK-1500 (Lithuania), BWR
nology development is still needed. However, the neutronic char- and PWR (Sweden) reactors. In the framework of the EURATOM BRI-
acteristics in the transmutation blanket have been studied in (Cheng LLIANT project the results of this study provide valuable data for
and Wong, 2000; Cheng, 2001; Ridikas et al., 2006). An inertial con- analysis and optimization of nuclear fuel cycle options in the Baltic
finement fusion (ICF) device (based on the D + T → 4He+n nuclear region in case of the further development of nuclear power.
reaction) could provide a powerful neutron source. The 1 MW fusion In order to investigate the transmutation efficiency of the fu-
power corresponds to ∼4 × 1017 n/s. A molten-salt blanket (LiF-BeF2- sion–fission hybrid system for different spent nuclear fuel TRU, the
(HN)F4 – “flibe”), surrounding this neutron source, then could serve as actinides extracted from the light water reactor (LWR) (averaged
a medium for trans-uranium actinides (TRU) to be burned. Flibe also composition of SNF TRU) and RBMK spent fuel (different cases) were
has a function of both the coolant and the carrier of tritium breeding analyzed. Major performance parameters of the transmutation system
material (6Li in this case). A well known advantage of the molten salt is (e.g., kscr, keff, Φn(E), equilibrium conditions, etc.) for different TRU
its possibility of both refueling of burned TRU and extraction of fission cases have been investigated. Detailed burn-up calculations with con-
products (FP) on-line. The averaged neutron flux is very high (of the tinuous feeding of TRU material to refresh the burned one and partial
order of ∼1.5·1015 n s−1 m−2) and it corresponds to the flux typical treatment of fission products have been performed in the modeling.
only of high-flux reactors. In order to produce 3000 MWth fission

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R. Plukienė et al. Nuclear Engineering and Design 330 (2018) 241–249

Table 1
Existing PWR and BWR type nuclear reactors in Sweden and RBMK-type reactors in Lithuania. The average parameters of LWR and RBMK reactors are marked in bold.

Name Type Fuel enrich-ment Power (MW) Loading factor (%) Operation time, y. (until 2015 y.) Partial input to SNF Burn-up MWd/kg
(PRIS) (U.S DOE/EIS, 2008)

Forsmark 1 BWR 2.5 984 82.2 31.91 0.094 33.75


Forsmark 2 BWR 2.1 1120 80.2 30.9 0.104 34.5
Forsmark 3 BWR 2.8 1167 84.8 27.4 0.096 34.25
Oskarshamn 1 BWR 2.3 473 60.4 28.33 0.046 33.75
Oskarshamn 2 BWR 2.5 638 73.3 31.98 0.071 29
Oskarshamn 3 BWR 2.6 1400 77.4 26.01 0.114 34.25
Ringhals 1 BWR 2.8 881 67.2 30.75 0.098 29
Ringhals 2 PWR 3.2 807 67.4 30.75 0.09 33.5
Ringhals 3 PWR 2.8 1063 76.1 29.72 0.101 39.5
Ringhals 4 PWR 4.0 1118 80.1 21.82 0.1 39.5
Barsebäck 1 BWR 2.9 600 74.5 19.93 0.039 26.25
Barsebäck 2 BWR 3.2 600 74.9 22.96 0.046 29
Sweden LWR 2.1–4 1000 76 28 1 34
Ignalina-1 RBMK 2–2.6 1500 53.9 21 0.488 18*
Ignalina-2 RBMK 2–2.8 1500 64.4 22 0.512 20*
Lithuania RBMK 2–2.8 1500 59.3 21.5 1 19

*
(Shevaldin et al., 1998; Krivoshein, 2002).

2. Initial conditions of the hybrid system and tru composition in Table 2


the blanket Initial TRU compositions (%) in the molten salt blanket for different SNF cases. The main
TRU elements are marked in bold.

For the investigation of the possibilities to incinerate the actinides Isotope LWR RBMK 1 RBMK 2 RBMK 3
separated from SNF of different power plants in the fusion–fission hy-
237
brid system we performed an evaluation of an inventory of the spent Np,% 3.78 2.07 3.32 3.82
238
Pu,% 1.81 0.19 0.51 0.67
nuclear fuel generated in Sweden and Lithuania nuclear reactors (PWR, 239
Pu,% 51.64 61.18 49.62 46.08
BWR and RBMK) up to 2015. Collected data on parameters of existing 240
Pu,% 24.61 27.56 31.09 31.86
PWR, BWR and RBMK-type nuclear reactors in Lithuania and Sweden 241
Pu,% 8.22 0.64 0.94 0.98
242
are presented in Table 1. Averaged data of the discharged fuel burn-up Pu,% 4.61 1.92 4.70 6.06
depending on the fuel enrichment and the discharge year in BWR and Total Pu,% 90.89 91.49 86.86 85.64
241
Am,% 4.21 6.32 9.30 9.74
PWR reactors are taken from (U.S DOE/EIS, 2008); power and the 243
Am,% 0.83 0.12 0.51 0.78
loading factor of the reactor are taken from (PRIS website (2016)). We Total Am,% 5.04 6.44 9.81 10.52
have used the IAEA nuclear fuel cycle simulation system (NFCSS 244
Cm,% 0.19 0.005 0.01 0.02
(2012)) and a generalized reactor model assumption for the country:
those different types of reactors of the same power and the same initial
fuel flow will produce approximately the same amount of SNF. That 2001, Plukienė et al., 2009). Three representative RBMK-1500 SNF of
means that the assumption of generalized reactor model for Sweden the Ignalina NPP RBMK TRU vectors after the 50 years cooling time
takes into account the averaged power, the average operation time, the have been evaluated: “RBMK 1” – 2% 235U enrichment and 14 MWd/kg
averaged fuel enrichment and the averaged fuel burn-up of all existing burn-up; “RBMK 2” – 2.4% 235U enrichment, 22 MWd/kg; “RBMK 3” –
BWR and PWR nuclear reactors in the country as listed in Table 1. 2.6% 235U enrichment, 26 MWd/kg. These RBMK TRU cases have been
According to (Plan 2013, 2014) there was 7520 tons of SNF in Sweden chosen taking into account the SNF composition of the Ignalina NPP
in 2013. According to this model the total amount of heavy metals of (Lithuania). The different RBMK SNF cases have been modelled using
SNF is approximately 7630 tons including 77.5 tons of TRU at the end of ORIGEN-ARP with prepared one-group burn-up dependent cross-sec-
2015. During operation of the Ignalina NPP (Lithuania) about 22,000 tion libraries, which are comprehensively explained in publication
assemblies of SNF (UO2 fuel with 2.0, 2.4, 2.6 and 2.8% initial 235U (Barkauskas et al., 2017). Depletion calculations for generation of the
enrichment (Barkauskaset al., 2016; Shevaldin et al., 1998; Krivoshein, cross-section libraries were performed using the SCALE 6.1 code
2002) from the two RBMK-1500 reactors were accumulated. The ap- package with the TRITON control module, which employs a NEWT
proximate amount of TRU is 24 tons. deterministic 2D transport code with the 238-group energy library
The TRU composition in the LWR SNF significantly depends on the based on ENDF-B VII library and the ORIGEN-S nuclide composition
initial fuel enrichment and the fuel burn-up in the reactor; these calculation code. The calculated composition of actinides has been
parameters have changed a lot from 1974 to 2015. There exists a wide validated by comparing the evaluation against experimental data. The
variety of fuel assembly designs used in BWR (8 × 8, 9 × 9, SVEA-64, similar isotopic composition has been obtained in benchmark calcula-
SVEA-100) and in PWR (15 × 15, 17 × 17) with different fuel enrich- tions of the RBMK spent nuclear fuel isotopic composition using MCNP
ments (2.1%–4% of 235U), which also influences the TRU composition and ORIGEN codes where modeling results of 2% enrichment 235U fuel
(Favalli et al., 2016). We have used the average spent nuclear fuel were compared with the same experimentally measured data of the
composition of the LWR reactor (3% enrichment 235U) after the 5 years RBMK-1000 fuel isotopic composition (Burlakov et al., 2003). One
cooling time. The isotopic composition of the average LWR reactor SNF should note that if the RBMK-1500 SNF cooling time is 50 years the
composition was calculated by using ORIGEN-ARP (SCALE module) larger part of 241Pu decays to 241Am. And, if the cooling time is shorter,
with specially prepared CE 14 × 14 (Westinghouse) ORIGEN-S multi- the 241Pu amount in RBMK-1500 SNF would be closer to the LWR 241Pu
burn-up libraries, which have been validated (Bowman et al., 2011, amount. Historically, uranium fuel with the 2% enrichment was used
Bowman and Leal, 2000). The considered TRU isotopic compositions in from the very beginning of the Ignalina NPP operation. It is the same
the molten salt are presented in Table 2. type of fuel loaded in RBMK-1000 reactors in Chernobyl (Ukraine). We
The RBMK-1500 SNF composition strongly depends on the initial have chosen two SNF burn-up cases with this enrichment: 1) 14 MWd/
RBMK reactor fuel enrichment and the burn-up rate (Kimtys et al., kg – assemblies of low burn-up and 2) 20 MWd/kg – assemblies of high

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continuous TRU and 6Li feeding as well as continuous FP removal have


been used in all simulated cases during the irradiation. A mechanism to
remove the fission products is needed in the molten salt transmutation
system not only due to the better neutron balance of the system – if not
removed solidification of fission products will occur in the molten salt
quite soon after the operation. The hybrid system transmutation blanket
parameters, kscr, Φn(E), equilibrium conditions and the tritium breeding
ratio, have been calculated for each analyzed SNF TRU case. Further,
the comparative analysis of the LWR and RBMK SNF TRU incineration
rate has been performed.

3. Modeling results of SNF TRU transmutation and main


performance parameters of the hybrid system

Here we present the results of the modeling of LWR and RBMK SNF
TRU transmutation process by the previously described hybrid fu-
sion–fission system. From Table 2 one can notice that 240Pu part is
considerably larger in all RBMK TRU composition cases compared with
the LWR SNF case (especially for RBMK 2 and RBMK 3 cases), besides
the concentration of 241Am is higher and that of 244Cm is lower. This is
due to the lower initial RBMK fuel enrichment and higher Pu trans-
Fig. 1. A simplified geometry model of the fusion–fission hybrid. FD stands for a Fusion
mutation in the RBMK type reactor. The strong neutron absorption by
Device. 240
Pu and a relatively smaller amount of the fissile element con-
centration determine the smaller kscr values in RBMK TRU as compared
burn-up, both representatives of a typical burn-up fuel before 1996. with the LWR TRU case (Fig. 2(a)). Therefore, a larger fusion power is
From 1996 up to 2004 the 2.4% 235U enrichment fuel with 0.41% needed at the beginning of irradiation as it is presented in Fig. 2(b) to
burnable poison (erbium) was the most frequently used nuclear fuel in sustain the 3 GW thermal power of the system. The fusion power is
RBMK-1500; here the average fuel burn-up was 22 MWd/kg. The last proportional to kscr: Pfus ∼ (1-kscr)/kscr.
RBMK 3 case was selected to test the SNF originated from later op- By comparing LWR and RBMK TRU transmutation cases in terms of
erational campaigns (from 2002) with the 2.6% 235U enrichment and the main performance parameters of the hybrid system, a number of
0.5% of burnable poison – erbium, which was first tested in the Ignalina important advantages have been obtained in favor of the LWR isotopic
NPP in ∼2001. This initial fuel load characteristic was used until the composition: the values of kscr (0.83) and Pfus (180 MW) are almost
final shutdown of the Ignalina NPP (Unit I in 2004 and Unit II in 2009). stable comparing the beginning and equilibrium stages, the equilibrium
The simplified spherical geometry setup described in Ridikas et al., is reached after ∼3 years of the system operation, and the tritium
2006 was used in our calculations (see Fig. 1 for details). The diameter breeding rate (TBR) is sufficient to supply tritium for the fusion device
of the cavity with the fusion device is 400 cm, surrounded by the 1 cm (TBR = 1.25). In the case of RBMK 1, the equilibrium is reached after
thick liquid flibe (6Li 0.1% in Li) wall, the 0.3 cm – metallic wall ∼3.3 years, kscr (0.77) is lesser at the beginning but later it approaches
(corrosion resistant SS316 50%), and the 1 cm thick graphite. A 60 cm that of the LWR TRU case. In equilibrium kscr = 0.814, Pfus = 190 MW,
thick transmutation blanket (divided into 4 regions for calculation) TBR = 1.25. In case of RBMK 2 and RBMK 3 transmutation in the
with TRU inside a flibe is placed between the graphite and the metallic molten salt kscr at the beginning of irradiation is 0.69 and 0.67, re-
wall. All the structure was surrounded by a 20 cm thick graphite re- spectively, and the 370 MW and 440 MW fusion power is needed for
flector and a 5 cm thick stainless-steel shell (Cheng, 2001; Ridikas et al., corresponding cases, and the TBR is not sufficient for such fusion power
2006). Initial conditions of the hybrid system were the same for all TRU (TBR < 1, 0.73 and 0.67, respectively). When the equilibrium for main
isotopic vectors considered: Ptherm 3 GW, initial TRU mass – 3.04 t. The isotope concentrations is reached, in both cases the situation is

Fig. 2. (a) kscr as a function of irradiation time in the molten salt blanket for different TRU cases, (kscr calculated with <1 σ ≥ 0.004). (b) Corresponding Pfus is needed to compensate the
neutron balance and sustain the 3 GW thermal power for different TRU cases.

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R. Plukienė et al. Nuclear Engineering and Design 330 (2018) 241–249

Fig. 3. (a) The macroscopic fission cross-sections for 239Pu, 241Pu, all MA and all TRU in the molten salt blanket for different TRU composition cases; (b) the macroscopic neutron capture
cross-sections for TRU, 240Pu, 239Pu and all MA (TRU cross-sections are on Y-axis on the right).

improved: kscr – 0.795 and 0.797, Pfus – 220 MW and 230 MW, TBR is equilibrium of fissile TRU in LWR, RBMK 2 and RBMK 3 cases is reached
1.11 and 1.04 for corresponding cases. In the latter cases a large part of faster as compared with the RBMK 1 case. This is determined by a
TRU are composed of 240Pu i.e., the 241Pu isotope is produced more higher concentration of 239Pu at the beginning and also by the feeding
intensively, and therefore the kscr rise gradient is larger than in the LWR concentration of the same TRU isotopic composition. Despite the higher
case. fissile isotope concentration in RBMK1 compared with the LWR case,
The neutron spectrum in the molten salt blanket is independent of the kscr begins at a lower value and approaches LWR kscr value at
the TRU isotopic composition and is stable during the irradiation time equilibrium. This can be explained by the macroscopic neutron capture
as it was shown in the paper (Ridikas et al., 2006). Most of the neutrons and fission cross-sections in Fig. 3: it is clearly seen that a higher 241Pu
are epithermal (about 80%) and when the equilibrium is reached the macroscopic fission cross-section determines a higher kscr at the be-
values of actinide macroscopic cross-sections also equilibrate. The value ginning in the LWR case, while the macroscopic neutron capture cross-
of kscr of the hybrid system with the molten salt blanket depends on the section of 240Pu equilibrates the neutron balance for the RBMK 1 case,
neutron capture and fission macroscopic cross-sections of corre- and, as a result the neutron absorption is similar in both LWR and
sponding TRU. The fission and neutron capture macroscopic cross- RBMK 1 cases.
sections of Pu isotopes, all TRU isotopes and MA (Minor Actinides) are The kscr behavior depends on the fission product accumulation in
presented in Fig. 3(a) and (b), respectively. One can observe a sharp the molten salt blanket as it was discussed in (Ridikas et al., 2006), but
increase of macroscopic fission cross-sections of TRU in all RBMK cases, it is also influenced by accumulating volatile materials such as 3H and
3
and it results in a sharp rise of kscr at the beginning of the system He. 3H (T-tritium) is produced from 6L, which is continuously re-
performance. The fertile nuclide part is the largest in RBMK 2 and plenished with TRU fuel, the other isotope – 3He – is produced by β−
RBMK 3 TRU cases (see Fig. 4), and this determines the larger macro- reaction from 3H. 3He is a strong neutron absorber (neutron capture
scopic neutron capture cross-sections for TRU in these cases. ∼1000 b). The presence of 3H and 3He deteriorates the neutron balance
The mass evolution of fissile and fertile isotopes in the system for in the system as it is seen in Fig. 5. Here kscr decreases by 6% after
different TRU transmutation cases is presented in Fig. 4. The 3000 days due to 3H and 3He in the molten salt. In a real situation both

Fig. 4. The fissile and fertile isotope mass evolution for different TRU transmutation Fig. 5. kscr behavior in the molten salt blanket of a hybrid system in the RBMK 1 TRU
cases. transmutation case performing 3H and 3He separation and without 3H and 3He separation.

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R. Plukienė et al. Nuclear Engineering and Design 330 (2018) 241–249

Fig. 6. The variation of Pu (a) and MA (b) isotope mass against time in the molten salt blanket/RBMK 2 case.

elements should be separated from the molten salt blanket and this Table 3
should be taken into account when performing the modeling calcula- Actinide concentrations (%) at the equilibrium stages for different TRU cases. The main
TRU elements are marked in bold.
tion.
For the establishment of LWR and RBMK TRU equilibrium condi- LWR RBMK 1 RBMK 2 RBMK 3
tions in the molten salt blanket the analogous procedure as described in
237
(Ridikas et al., 2006) has been performed. It has been determined that Np,% 1.6 0.8 1.3 1.4
238
the system reaches equilibrium when the variation of the Pu isotope Pu,% 6.5 4.5 6.6 7.1
239
Pu,% 22.6 25.1 20.1 18.5
mass is less than 4% (this variation have been chosen to include the 240
Pu,% 30.9 34.9 32.9 31.8
statistical uncertainties of calculations) in respect of the actual pluto- 241
Pu,% 15.2 14.9 14.3 13.9
242
nium mass in the blanket. The physical effect of saturation for each Pu,% 9.8 7.7 9.4 10.4
nuclide for a certain nuclide composition is achieved in the molten salt Total Pu,% 85.0 87.1 83.3 81.7
in equilibrium. The variation of the Pu and MA isotope mass against
241
time in the molten salt blanket in the RBMK 2 case is presented in Fig. 6 Am,% 1.5 1.9 2.6 2.6
242m
Am,% 0.3 0.4 0.5 0.5
a and b). The time needed to reach the equilibrium state of the system is 243
Am,% 1.7 1.4 1.6 1.8
determined by the fissile and fertile actinide concentrations and their
macroscopic cross-sections of interaction with neutrons for different Total Am,% 3.5 3.7 4.7 4.9

TRU compositions. The equilibrium for Pu transmutation is reached 242


Cm,% 0.7 0.9 1.2 1.2
after 1000 days for LWR, RBMK 2 and RBMK 3 TRU cases and after 243
Cm,% 0.2 0.3 0.5 0.5
244
1200 days for the RBMK 1 case. Meanwhile the equilibrium for MA is Cm,% 6.0 4.7 5.9 6.7
245
reached in ∼2500 days for all considered cases. The latest equilibrium 246
Cm,% 2.6 2.1 2.6 3.0
Cm,% 0.4 0.4 0.5 0.6
stage is reached for 246Cm, 245Cm and 244Cm isotopes.
The actinide composition is different for considered SNF cases at the Total Cm,% 9.9 8.4 10.7 12.0
equilibrium stage, however, as compared with the initial composition,
the fissile and fertile isotope concentration ratio becomes comparable
Table 4
for all cases (at the beginning this ratio is 0.9 ÷ 1.62, in equilibrium –
Neutron fluence (MW·y/m2) to the first wall of the fusion–fission hybrid system for dif-
0.6 ÷ 0.77). ferent TRU cases.
In all the analyzed TRU cases the hybrid system incinerates about
1.1 tons per year of TRU with the 3 GW thermal power output. The Stage LWR RBMK 1 RBMK 2 RBMK 3
initial TRU vector influences the composition of actinides at the equi-
kscr peak 1.3 2.0 2.9 4.2
librium stage. The actinide isotopic composition at the equilibrium Equilibrium 6.5 7.7 6.7 6.7
stage is presented in Table 3. 237Np, 239Pu, and 241Am are incinerated 3000 days 21.1 21.0 21.3 21.3
most effectively: – the transmuted part is 30–51% for 237Np, 28–50%
for 239Pu and ∼26–54% for 243Am for RBMK2-LWR cases, while the
lowest transmutation rate was obtained for RBMK3 case: 17% for to the first molten salt wall (see Table 4). Evaluation shows that, in-
237
Np, 14% for 239Pu and 11% for 243Am. The smallest amount of Cm is dependently of the initial TRU composition, the first molten salt wall is
accumulated in the RBMK1 case (smaller amount of 244Cm is re- crossed by ∼2.1 × 1027 neutrons during 8 years (∼21 MW·y/m2). The
plenished). The minor actinides are accumulating in the molten salt application of a different molten salt composition (Be salt) as in
(minimum ∼200 kg in the RBMK 1 case, maximum ∼300 kg in the (Plukiene et al., 2006) could improve these fusion–fission system per-
RBMK 3 case). formance parameters.
The critical parameter for the hybrid system is the neutron fluence

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R. Plukienė et al. Nuclear Engineering and Design 330 (2018) 241–249

Fig. 7. Inhalation radiotoxicity of Pu and Np from RBMK 2 (a) and LWR (b) SNF at the beginning and at the end of transmutation in fusion–fission hybrid system.

4. Radiotoxicity analysis of the final TRU waste decay. 241Pu accumulation from 240Pu is larger in the RBMK 2 case as
compared with the LWR case, but it decreases to natural U radiotoxicity
The efficiency of transmutation has been investigated in detail for after 200 years.
LWR and RBMK 2 cases by evaluating the inhalation radiotoxicity of At the end of transmutation the isotopic composition in both cases
TRU before and after transmutation in the hybrid system (after 10 years becomes more or less similar and the same happens with the radio-
cooling time). toxicity. In both considered cases the radiotoxicity of 239Pu, 240Pu,
237
The inhalation pathway of the actinide intake is much more dan- Np and 241Am is considerably decreased. In the molten salt trans-
gerous than the ingestion and it was used as a more conservative re- mutation blanket a larger amount of Cm isotopes is accumulated, but
ference (Plukiene et al., 2004, 2014). The inhalation radiotoxicity (In- the contribution of this isotope to the total waste radiotoxicity is minor.
hTox) was calculated as follows: InhTox = A × 3,7 × 1010 × EInh , where The total transmutation time in the system is 8.2 years. During this
A is the nuclide activity (Bq), EInh are committed effective dose coeffi- operation time about 9 tons of TRU can be incinerated and the radio-
cients (SvBq−1) for each nuclide taken from International Commission toxicity of the remaining final waste decreases approximately by 4–6
on Radiological Protection (ICRP) publication 119 (ICRP, 2012). times in the period from 1 thousand to 100 thousand years.
The radiotoxicity of RBMK 2 at the beginning was considerably
smaller compared with that of LWR. This was determined by the
smaller quantity of 241Pu (T1/2 = 14.2 y) and 238Pu (T1/2 = 87.7 y) due 5. Conclusions
to the longer RBMK SNF cooling time (50 years) in the RBMK 2 case.
The inhalation radiotoxicity of Pu and MA at the beginning and at The closed fuel cycle scenario of LWR and RBMK SNF has been
the end of transmutation is demonstrated in Fig. 7(a and b) and in analyzed in the framework of the EURATOM project BRILLIANT. The
Fig. 8(a and b) for RBMK 2 and LWR, respectively. The radiotoxicity transmutation of TRU elements has been simulated by using the model
increases by a factor of 2 in the first 10 years after transmutation (due to of the fusion–fission hybrid system for different spent nuclear fuels
238
Pu) in the RBMK 2 case, but it decreases afterwards due to 238Pu accumulated in the Baltic countries: RBMK-1500 (Lithuania) and LWR
(Sweden). According to the IAEA nuclear fuel cycle simulation system

Fig. 8. Inhalation radiotoxicity of MA from RBMK 2 (a) and LWR (b) SNF at the beginning and at the end of transmutation in the fusion–fission system.

247
R. Plukienė et al. Nuclear Engineering and Design 330 (2018) 241–249

(NFCSS) and the generalized reactor model assumption for the country Lithuanian state budget and partially accomplished within the frame of
about 71% of SNF is produced in BWR and 29% in PWR type reactors in the European Commission project “Brilliant” (EURATOM program, No.
Sweden as well as the total amount of heavy metals of SNF is ap- 662167).
proximately 7630 tons, including 77.5 tons of TRU at the end of 2015.
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