Basis for all investigations provided here is the analysis of different potential feed streams
These streams will be fed into the reactor after the start-up to understand the influence of the feed on the long-term evolution of the core. The simulations will be used to get a first understanding of the effects of an increased fission product feeding into a reactor during operation by investigating core criticality and the concentrations of the elements to be transmuted, Pu, Am, and Cm as well as Tc as a representative fission product where the accumulation and the effect of the salt clean-up can be observed. The results will be used to draw conclusions on a potential optimization for a potential future operational scheme.
3.1. The reference case study
The evolution of the system criticality over burnup is given in
Figure 3 for the staggered initiation of the clean-up of different fission product elements as shown in the bottom of the figure. The aim of the scheme is to balance the reactivity of the core for an extended period only through the clean-up initiation without relying on active control measures, like control rods, as well as to assure for the simulation to limit the effect of the k
eff normalization on the results of breeding in a molten salt system [
11]. The idea behind the staggered clean-up approach is to allow studies on the long term behaviour of a potential self-sustained iso-breeding molten salt reactor system with different feed streams as described above (tailings, SNF, SNF+FP) to get a deeper understanding of the effect of feeding very small material amounts over a long time on the long-term changes in composition and criticality.
The feed stream with depleted uranium tailings has been chosen as the reference case for this study (see
Figure 3). Also, it is one of the easiest envisaged operational modes in which U238, already transmuted into fissile Pu239, is replaced after every burnup cycle using the U238 from clean tailings in the feed stream. The feeding stream is optimized to ensure a constant amount of U238 within the core within a reasonable accuracy after each 10 GWd/tHm cycle. This is essential to balance the amount of breeding material available as basis for the iso-breeding. The clean-up of a certain additional element is activated every time when the system criticality falls below 1. In this case 20% of the whole salt amount is cleaned after every 10 GWd/tHM cycle and the choice of the elements to be separated follows the priority list as previously developed [
11]. Applying this staggered approach allows reactor operation until ~900 GWd/tHM is extracted, related to the initial load, compared to ~200 GWd/tHM without clean-up.
For a more detailed analysis of the changes of the isotopic contents of TRU materials, the contents in the core are analysed in the following,
Figure 4,
Figure 5 and
Figure 6. As already described, the initial core is based on enriched Uranium. The initial U-235 content decreases rapidly due to reactor operation, see
Figure 4 and is replaced by Pu-239 as main fissile material at a burnup of ~75 GWd/tHM. The amount of U235 continues to decrease beyond this point and becomes almost negligible at a burnup of ~500 GWd/tHM. At this time, the amount of Pu239 in the system also attains a steady state with an equilibrium between breeding and burning being approached. It is important to highlight here that only a negligible amount of fissile material, besides the U235 required for reactor start-up, has been inserted into the system. All fissile material is produced in-situ through internal breeding within the system. This process is supported by continuous replenishment of U238 through the feed stream to maintain a constant amount of fertile material in the system. The creation of the higher Pu isotopes starts with some time delay, since these isotopes are formed out of material which has to be bred first. At the end of the observation period of ~900 GWd/tHM, the Pu-240 production has slowed down significantly along with the total Pu content, but an asymptotic value has not yet been achieved. The production of Pu-241 and Pu-242 is on a very small level. The final Pu vector is Pu-239, 67%; Pu-240, 28%; Pu-241, 3%; and Pu-242, 2% at 900 GWd/tHM.
The Americium production (see
Figure 5) follows a similar long-term structure as the higher Pu build up, but with even longer time delays since a substantial amount of the precursor isotope has to be bred first. The overall Americium quantity at the end of the observation period is less than 3% of the total Pu content in the fuel salt. Am-241 is mainly formed though the decay of Pu-241 – thus the amount is slightly dependent on reactor power since there is the competition between Pu-241 fission and β
-decay with a half-life of ~14 years. The delay in Am-241 production from the precursor Pu-241 is clearly observed in
Figure 5. The small amount of Am243 is formed mainly through the rapid beta decay of Pu243 (half-life of 5h) which is itself formed through neutron capture in Pu242. Am243 may also be formed due to neutron capture in Am241 and Am242m, but with a significantly lower contribution. Total Am production has reached a point of inflection at ~600 GWd/tHM Indicating that an asymptotic value will be achieved, although this would require a much longer operational time.
The Curium formation in the core is 10 times lower than the Americium formation, see
Figure 6. The leading isotopes are Cm-244 and Cm-242. Cm-242 is mainly formed through neutron capture in Am-241 creating Am-242 (16h half-life), followed by a beta decay to either Cm-242 or through electron capture to Pu-242 (marginal path). Cm-244 is mainly formed through neutron capture in Am-243 and the following decay of Am-244 with a small half-life of only 10h. The delay of the formation of the leading isotope Cm-244 compared to the precursor isotope Am-243 is clearly observable. The Cm-242 production has already reached a clear point of inflection at about 500 GWd/tHM and has got almost asymptotic, while the Cm-244 still accumulates following the trend of Am-243. In general, the Cm-production has not reached a point of inflection during the observation period, mainly due to the still increasing amounts of Cm-244 and Cm-245. To observe the long-term behaviour and to assess a potential asymptotic behaviour a significantly longer observation period would be required.
However, an important fact is that due to the reverse reprocessing all these TRU isotopes will stay in the core and will not require handling like in traditional P&T systems with solid fuel and external reprocessing. This new approach will help to reduce the radiation exposure to workers unlike the multi recycling scheme required in the manufacturing of fuel for conventional solid-fuelled systems [
7].
3.2. Parametric study of different fission product contents
The basis for the simulation is given by the case with SNF feed as calculated, based on light water reactor fuel with an average burnup of 50 GWd/tHM using HELIOS. The use of SNF (black line with squares) instead of tailings (red line with circles) as feed leads to a slightly longer potential operation. The system achieves higher criticality in the first operational period without salt clean-up (see
Figure 7). This effect is due to the higher share of fissile material in the SNF feed (~ 1% Pu and ~1% U-235) as compared to ~0.3% U-235 in tailings. Obviously, this observed difference is mainly important in the first operational stage without salt clean-up, since the following steps do not show major differences anymore. However, it is an interesting outcome that the effect of the fissile material added seems to be stronger than the effect of adding the fission products contained in the SNF. The main reason is that most FPs have significantly higher absorption XS in the thermal neutron spectrum as compared to fast spectrum. Thus, the fission products have a much stronger poisoning effect in light water reactors than in the iMAGINE system.
Next, a higher amount of FPs is inserted into the system while keeping the amount of fertile and fissile materials (uranium and plutonium) in the feed stream as unchanged. The idea is to model two feed streams with different amounts of vitrified waste by only increasing the amount of fission products in the SNF by 2 and 5 times. This model assures a ‘conservative approach’ bringing all fission products and minor actinides into the core. In this way, it is not considered that gaseous and volatile fission products are only contained to a small share in the vitrified waste, while the major share has to be handled in a different way in the reprocessing plant. However, the effect will be limited to the first calculation cycle since all gaseous and volatile fission products will anyway be released at the end of each 10 GWd/tHM cycle.
The insertion of double the amount of fission products (blue line with triangles) has a minor overall effect compared to the case using tailings. However, compared to the case of SNF feed, it becomes clear that the increased amount of fission products has mainly a strong effect in the first stage before the clean-up is activated. The long-term effect is very limited. This can be explained by the overall increase of the amount of fission products in the core as well as with the effect of the clean-up which reduces not only the fission products created through the burnup, but also the fission products which are inserted in addition.
Inserting 5 portions of fission products (green lines with diamonds) has a very strong influence in the first operational period and even does not allow the reactor to get critical in the averaged criticality analysis per cycle. In general, the insertion of such a large amount of fission products significantly penalizes the operation reducing the total burnup by ~20% from 910 GWd/tHM to 720 GWd/tHM compared to the SNF case. However, it is clear that the reactor could still be operated with such a high fission product load, which confirms that the insertion of larger amounts of fission products, eg through the feeding of dissolved vitrified waste would be possible as waste management method. On the one hand this offers the opportunity to burn minor actinides which have not been separated previously in reprocessing; on the other hand, the approach will allow the use of reverse reprocessing method with the opportunity of the elementwise separation of fission products leading to new possibilities for conditioning of the waste streams.
The comparative analysis of the plutonium accumulation,
Figure 8, shows that the Pu concentration in the core depends only weakly on the different feed scenarios. The Pu content in the scenario with the tailings feed is slightly lower, while feeding the largest amount of fission products will deliver a marginally higher Pu content. However, there is no real effect on the overall tendency of the increase in the Pu amount and the formation of an almost asymptotic concentration at the end of the observation period. The amount of Pu fed (dashed lines) is identical in all SNF cases, which verifies the correct implementation of the model for the fission product feed.
The analysis of the Pu management shows that the amount resident in the system is in all cases slightly higher than in the reference case. However, in all SNF feeding cases the overall Pu amount is slightly reduced compared to the reference case with tailings feed. The inserted Pu amount consists of the Pu fed into the system and the Pu bred in the system. The Pu reduction is calculated using Eq. (1). Obviously, the difference between the slightly higher Pu concentration at the end of the observation period is lower than the amount of Pu fed into the system through the SNF feed. The results indicate that some small amount of Pu burning is achieved in the SNF fed scenarios. The different amounts of fission products have only a very marginal effect.
Table 1.
Detailed analysis of the Pu management based on feeding and the amount resident at the end of the observation period.
Table 1.
Detailed analysis of the Pu management based on feeding and the amount resident at the end of the observation period.
| |
Pu-tail [atoms/barn*cm] |
Pu-SNF [atoms/barn*cm] |
Pu-SNF1.1 [atoms/barn*cm] |
Pu-SNF1.4 [atoms/barn*cm] |
| Amount fed |
0.00E+00 |
5.56E-05 |
5.26E-05 |
4.40E-05 |
| Amount resident |
6.79E-04 |
6.94E-04 |
6.90E-04 |
6.81E-04 |
| Pu reduction |
|
-6% |
-6% |
-6% |
The comparative analysis of the Americium content in the core,
Figure 9, shows that the general tendency of the accumulation of Am is only slightly influenced through the feed. This indicates that the Am concentration in the core is mainly driven by the operation of the reactor and the breeding processes. Increasing the Am amount in the core through the feed leads to a slightly higher concentration, but the effect is smaller than the increase due to operation. The Am feed is indicated through the dashed lines. It is already apparent from these lines that the inserted amount of Am is larger than the difference the concentration appearing in the core over the observations period.
A more detailed analysis of the Am management,
Table 2, confirms this observation for the cases with higher fission product feed, but this is not the case for the unmodified SNF feed. The amount resident at the end of the observation period depends on the operational time and the amount of Am fed into the system leading to the lowest resident amount for the SNF 1.4 case.
Figure 9 supports here the understanding, the lowest amount is obviously a result of the shorter observation period, while the concentration is highest through the whole period. The overall Am change is calculated using Eq. (1). The higher Am content is because the increased Pu content in the SNF feed case leads to a higher breeding of Am, since the SNF contains greater amounts of higher Pu isotopes as precursor. Especially in the beginning since a fully developed LWR Pu vector at 50 GWd/tHM is inserted while the clean configuration based on enriched Uranium will initially be Pu free. In the tailings-based system the breeding will start at a lower average mass of the Pu isotopes (see the delay in the Am concentration for the tailings fed case). The breeding process creates only Pu-239 in the first time period of operation, the formation of higher Pu isotopes requires a longer irradiation time, see
Figure 4. In the cases of higher loads of Am through the feeding stream, Am reduction takes place and the reduction efficiency increases with increased Am concentration which coincides with the observation that have been made in a large number of P&T studies delivered in the past [
30,
31,
32].
The Cm content over the observation period is rising for all cases, see
Figure 10. No saturation level is achieved and the concentration of Cm in the salt is still growing almost linearly at the end of the observation period. However, there is a clear difference between the base case where no Cm is fed into the core and all other cases. In all cases, Cm is bred inside the core from neutron capture reactions in Am - this means the production is strongly dependent on the Am content in the core and thus delayed in a clean core where the Am has to be bred first. However, the delay in the increase of the Cm concentration is much more pronounced than for Am, compare
Figure 9 and
Figure 10. It gets obvious in the other cases, that the rapid increase in the Cm concentration at the beginning is caused by the feed through the SNF and additionally through the ‘vitrified’ waste, see the identical gradient of the concentration (solid lines) and the content inserted through the feed (dashed lines) up to 100 GWd/tHM. The massive insertion of Cm in the SNF 1.4 scenario and the almost identical slope of the feed and the content indicates that efficient burning takes place when the concentration is high enough.
A more detailed analysis of the Cm management and the concentrations as well as the feed is given in
Table 3. The overall Cm change is calculated using Eq. (1). The concentration of Cm in the system (amount resident) at the end of the observation period increases by 27%, 28% and 31%, respectively for the scenarios with increased Cm feed. Obviously, the feeding amount is more influential in the case of Cm on the amount resident than the breeding process. However, the higher the feed, the greater is the amount of Cm which is transmuted during the operation of the reactor. In the scenario with the highest Cm feed, almost all material added through the feeding process is already burnt at the end of the observation period, which indicates a successful transmutation process, even if the concentration is still increasing. The cases with the lower feed support some transmutation, but the process is not yet efficient enough due to the low amount of Cm added.
In the final step, the effect of the different scenarios on fission product accumulation and salt clean-up is evaluated using technetium as representative fission product, see
Figure 11. The initial analysis indicates that the amount of all fission products inserted through the feeding stream is small compared to the accumulation of Tc which is created due to reactor operation One of the main reasons is that the LWR fuel which is inserted through the feed stream has a limited burnup of ~50GWd/tHM, much lower than the overall burnup in the fuel over the observation period. A more important observation for the long-term operation is that the asymptotic value of Tc after activation of the salt clean-up seems to be only marginally influenced by the feed. This confirms the expectation that the effect of the higher amount of fission products in the feed stream will be almost completely balanced through the clean-up system. This effect is interesting since it could lead to the conclusion that it would promising to start with a comparably high fission product load while initiating the clean-up system earlier and using the fission products as a removable poison. These could be siphoned off when the reactor physics demands the removal of a specific fission product to reduce the number of different fission products to be tackled in the clean-up system in early operation stage.