Thermal conductivity of homogeneous and heterogeneous MOX fuel with up to 44 MWd/kgHM burn-up

New thermal diffusivity data for homogeneous SBR and heterogeneous MIMAS and OCOM MOX fuels are reported. No significant difference between the thermal diffusivity of the homogeneous and heterogeneous fuels was found at the burn-up up to 44 MWd/kgHM. These measurements, combined with previously published results or correlation functions for irradiated UO₂ and MOX were compared and it was found that separate correlations for these two fuels are not justified. A correlation for the thermal conductivity of irradiated UO₂ and MOX as a function of burn-up and irradiation temperature is proposed.     

Thermal diffusivity of homogeneous SBR MOX fuel with a burn-up of 35 MWd/kgHM

The effect of burn-up on the thermal conductivity of homogeneous SBR MOX fuel is investigated and compared with standard UO₂ LWR fuel. New thermal diffusivity results obtained on SBR MOX fuel with a pellet burn-up of 35 MWd/kgHM are reported. The thermal diffusivity measurements were carried out at three radial positions using a shielded “laser-flash” device and show that the thermal diffusivity increases from the pellet periphery to the centre. The fuel thermal conductivity was found to be in the same range as for UO₂ of similar burn-up. The annealing behaviour was characterized in order to identify the degradation due to the out-of-pile auto-irradiation.     

Thermal conductivity degradation analyses of LWR MOX fuel by the quasi-two phase material model

The temperature measurements of mixed oxide (MOX) and UO₂ fuels during irradiation suggested that the thermal conductivity degradation rate of the MOX fuel with burnup should be slower than that of the UO₂ fuel. In order to explain the difference of the degradation rates, the quasi-two phase material model is proposed to assess the thermal conductivity degradation of the MIMAS MOX fuel, which takes into account the Pu agglomerate distributions in the MOX fuel matrix as fabricated. As a result, the quasi-two phase model calculation shows the gradual increase of the difference with burnup and may expect more than 10% higher thermal conductivity values around 75 GWd/t. While these results are not fully suitable for thermal conductivity degradation models implemented by some industrial fuel manufacturers, they are consistent with the results from the irradiation tests and indicate that the inhomogeneity of Pu content in the MOX fuel can be one of the major reasons for the moderation of the thermal conductivity degradation of the MOX fuel.     

Analysis of MOX fuel behavior in reduced-moderation water reactor by fuel performance code FEMAXI-RM

To assess the feasibility of the 31% Pu-MOX fuel rod design of reduced-moderation water reactor (RMWR) in terms of thermal and mechanical behaviors, a single rod assumed to be irradiated in the core of RMWR up to 106 GWd/tHM has been analyzed by a fuel performance code FEMAXI-RM which is an extended version of FEMAXI-6 code. In the analysis, design specifications of fuel rod and irradiation conditions have been input, and available models of both MOX fuel and UO₂ fuel have been used as appropriate. The results are: fission gas release is several tens of percent, rod internal pressure does not exceed the coolant pressure, and the highest fuel center temperature is 2400 K, while cladding diameter increase caused by pellet swelling is within 1% strain. These predictions suggest that the MOX fuel rod integrity will be held during irradiation in RMWR, though actual behavior of MOX pellet swelling and cladding oxidation require to be investigated in detail.     

An Apparatus for Continuously Measuring Radon-222 Exhalation from Ground

High burnup MOX and UO₂ test rods were prepared from the fuel rods irradiated in commercial BWRs. Each test rod was equipped with a fuel center thermocouple and reirradiated in the Halden boiling water reactor (HBWR) in Norway. The burnups of MOX and UO₂ test rods reached about 84GWd/tHM and 72GWd/t, respectively. Fuel temperature was measured continuously during the re-irradiation tests. Thermal conductivity change in high burnup fuel was evaluated from the results of comparison between the measured fuel temperature and the data calculated by using the fuel analysis code FEMAXI-6. The comparison results suggested that the thermal conductivity of MOX fuel pellets is comparable to that of UO₂ fuel pellets in the high burnup region around 80 GWd/t. It is probable that the impurity effect of Pu atoms gradually diminishes with increasing burnup because other factors that affect pellet thermal conductivity, such as the accumulation effect of soluble fission products and irradiation-induced defects in crystal lattice, become dominant in a high burnup region.     

Oxygen stoichiometry shift of irradiated LWR-fuels at high burn-ups: Review of data and alternative interpretation of recently published results

The available oxygen potential data of LWR-fuels by the EFM-method have been reviewed and compared with thermodynamic data of equivalent simulated fuels and mixed oxide systems, combined with the analysis of lattice parameter data. Up to burn-ups of 70-80 GWd/tM the comparison confirmed traditional predictions anticipating the fuels to remain quasi stoichiometric along irradiation. However, recent predictions of a fuel with average burn-up around 100 GWd/tM becoming definitely hypostoichiometric were not confirmed. At average burn-ups around 80 GWd/tM and above, it is shown that the fuels tend to acquire progressively slightly hyperstoichiometric O/M ratios. The maximum derived O/M ratio for an average burn-up of 100 GWd/tM lies around 2.001 and 2.002. Though slight, the stoichiometry shift may have a measurable accelerating impact on fission gas diffusion and release.     

Change of fuel-to-cladding gap width with the burn-up in FBR MOX fuel irradiated to high burn-up

In order to study the dependence of the gap width change on the burn-up, the fuel-to-cladding gap widths were investigated by ceramography in a large number of FBR MOX fuel pins irradiated to high burn-up. The dependence of gap widths on the burn-up was closely connected with the formations of JOG (joint oxyde-gaine) and rim structure. The gap widths decreased gradually due to the fuel swelling until ∼30 GWd/t, but beyond this burn-up the dependence showed two different tendencies. With the increase of burn-up, the gap widths decreased due to the increase of fuel swelling in the low fuel temperature region where the rim structure was observed, but they increased in the high fuel temperature region where the JOG rich in Cs and Mo formed in the gap.     

Burning of MOX fuels in LWRs; fuel history effects on thermal properties of hull and end piece wastes and the repository performance

The thermal impacts of hull and end piece wastes from the reprocessing of MOX spent fuels burned in LWRs on repository performance were investigated. The heat generation rates in MOX spent fuels and the resulting heat generation rates in hull and end piece wastes change depending on the history of MOX fuels. This history includes the burn-up of UO₂ spent fuels from which the Pu is obtained, the cooling period before reprocessing, the storage period of fresh MOX fuels before being loaded into an LWR, as well as the burn-up of the MOX fuels. The heat generation rates in hull and end piece wastes from the reprocessing of MOX spent fuels with any of those histories are significantly larger than those from UO₂ spent fuels with burn-ups of 45 GWd/THM. If a temperature below 80°C is specified for cement-based materials used in waste packages after disposal, the allowable number of canisters containing compacted hull and end pieces in a package for 45 and 70 GWd-MOX needs to be limited to a value of 0.4–1.6, which is significantly lower than 4.0 for 45 GWd-UO₂.     

Modeling of WWER-440 fuel pin behavior at extended burn-up

Currently, there is an ongoing effort to increase fuel discharge burn-up of all LWRs fuel including WWERs as much as possible in order to decrease power production cost. Therefore, burn-up is expected to be increased from 60 to 70 MWd/kg U. The change in the fuel radial power distribution as a function of fuel burn-up can affect the radial fuel temperature distribution as well as the fuel microstructure in the fuel pellet rim. Both of these features, commonly termed the “rim effect.” High burn-up phenomena in WWER-440 UO₂ fuel pin, which are important for fission gas release (FGR) were modeled. The radial burn-up as a function of the pellet radius and enrichment has to be known to determine the local thermal conductivity.In this paper, the radial burn-up and fissile products distributions of WWER-440 UO₂ fuel pin were evaluated using MCNP4B and ORIGEN2 codes. The impact of the thermal conductivity on predicted FGR calculations is needed. For the analysis, a typical WWER-440 fuel pin and surrounding water moderator are considered in a hexagonal pin well. The thermal release and the athermal release from the pellet rim were modeled separately. The fraction of the rim structure and the excessive porosity in the rim structure in isothermal irradiation as a function of the fuel burn-up was predicted. A computer program; RIMSC-01, is developed to perform the required FGR calculations. Finally, the relevant phenomena and the corresponding models together with their validation are presented.     

Analysis of MOX Fuel Behavior in Halden Reactor by FEMAXI-6 Code

Capabilities of the FEMAXI-6 code to analyze the behavior of high burnup MOX fuels in LWRs have been evaluated. Coolant conditions, detailed power histories and specifications of the MIMAS-MOX fuel rods, rod 10 and rod 11, of IFA-597.4–7 irradiated in the Halden reactor were input, and calculated rod internal pressures and pellet center temperatures were compared with the measured data for the range of 0-31 MWd/kgUO₂. Some sensitivity studies were conducted mainly with respect to pellet thermal conductivity and swelling rate to investigate the changes in thermal behavior and their effects on fission gas release.

In the irradiation period up to about 23 MWd/kgUO₂, the calculated pellet center temperatures sufficiently agreed with the measured data and also the calculated rod internal pressures reproduced the tendency of an increase in the measured rod internal pressures. These results suggest that fission gas release from MOX fuels can be reasonably predicted by a diffusion process that is modeled in UO₂ pellet grains. On the other hand, the steep increase in the measured rod internal pressures observed at the power ramp around 23 MWd/kgUO₂ cannot be reproduced by FEMAXI-6 and can be regarded as the result of a relatively large amount of gas release, which possibly caused a pellet-cladding-gap closure through pellet gas-bubble swelling.     

Diametral strain of fast reactor MOX fuel pins with austenitic stainless steel cladding irradiated to high burnup

The C3M irradiation test, which was conducted in the experimental fast reactor, “Joyo”, demonstrated that mixed oxide (MOX) fuel pins with austenitic steel cladding could attain a peak pellet burnup of about 130 GWd/t safely. The test fuel assembly consisted of 61 fuel pins, whose design specifications were similar to those of driver fuel pins of a prototype fast breeder reactor, “Monju”. The irradiated fuel pins exhibited diametral strain due to cladding void swelling and irradiation creep. The cladding irradiation creep strain were due to the pellet-cladding mechanical interaction (PCMI) as well as the internal gas pressure. From the fuel pin ceramographs and ¹³⁷Cs gamma scanning, it was found that the PCMI was associated with the pellet swelling which was enhanced by the rim structure formation or by cesium uranate formation. The PCMI due to cesium uranate, which occurred near the top of the MOX fuel column, significantly affected cladding hoop stress and thermal creep, and the latter effect tended to increase the cumulative damage fraction (CDF) of the cladding though the CDF indicated that the cladding still had some margin to failure due to the creep damage.     

Corrosion of irradiated MOX fuel in presence of dissolved H2

The corrosion behaviour of irradiated MOX fuel (47 GWd/tHM) has been studied in an autoclave experiment simulating repository conditions. Fuel fragments were corroded at room temperature in a 10 mM NaCl/2 mM NaHCO₃ solution in presence of dissolved H₂ for 2100 days. The results show that dissolved H₂ in concentration 1 mM and higher inhibits oxidation and dissolution of the fragments. Stable U and Pu concentrations were measured at 7 × 10⁻¹⁰ and 5 × 10⁻¹¹ M, respectively. Caesium was only released during the first two years of the experiment. The results indicate that the UO₂ matrix of a spent MOX fuel is the main contributor to the measured dissolution, while the corrosion of the high burn-up Pu-rich islands appears negligible.     

Oxidizing dissolution of spent MOX47 fuel subjected to water radiolysis: Solution chemistry and surface characterization by Raman spectroscopy

The mechanisms of oxidizing dissolution of spent MOX fuel (MIMAS TU2®) subjected to water radiolysis were investigated experimentally by leaching spent MOX47 fuel samples in pure water at 25 °C under different oxidizing conditions (with and without external gamma irradiation); the leached surfaces were characterized by Raman spectroscopy. The highly oxidizing conditions resulting from external gamma irradiation significantly increased the concentration of plutonium (Pu(V)) and uranium (U(VI)) compared with a benchmark experiment (without external irradiation). The oxidation behavior of the plutonium-enriched aggregates differed significantly from that of the UO₂ matrix after several months of leaching in water under gamma irradiation. The plutonium in the aggregates appears to limit fuel oxidation. The only secondary phases formed and identified to date by Raman spectroscopy are uranium peroxides that generally precipitate on the surface of the UO₂ grains. Concerning the behavior of plutonium, solution analysis results appear to be compatible with a conventional explanation based on an equilibrium with a Pu(OH)_4(am) phase. The fission product release - considered as a general indicator of matrix alteration - from MOX47 fuel also increases under external gamma irradiation and a change in the leaching mode is observed. Diffusive leaching was clearly identified, coinciding with the rapid onset of steady-state actinide concentrations in the bulk solution.     

Modeling of fission gas swelling in LWR UO2 fuel under irradiation

An understanding of the behavior of fission gas in uranium dioxide (UO₂) fuel is necessary for the prediction of the performance of fuel rods under irradiation. A mechanistic model for matrix swelling by the fission gas in LWR UO₂ fuel is presented. The model takes into account intragranular and intergranular fission gas bubbles behavior as a function of irradiation time, temperature, fission rate and burn-up. The intragranular bubbles are assumed to be nucleated along the track of fission fragments, which play the dual role of creator and destroyer of intragranular bubbles. The intergranular bubble nuclei is produced until such time that a gas atom is more likely to be captured by an existing nucleus than to meet another gas atom and form a new nucleus. The capability of this model was validated by a comparison with the measured data of fission gas behavior such as intragranular bubble size, bubble density and total fuel swelling. It was found that the calculated intragranular bubble size and density are in reasonable agreement with the measured results in a broad range of average fuel burn-ups 6–83 GW d/tU. Especially, the model correctly predicts the fuel swelling up to a burn-up of about 70 GW d/tU.     

Behaviour of fission gas in the rim region of high burn-up UO2 fuel pellets with particular reference to results from an XRF investigation

XRF and EPMA results for retained xenon from Battelle's high burn-up effects program are re-evaluated. The data reviewed are from commercial low enriched BWR fuel with burn-ups of 44.8–54.9 GWd/tU and high enriched PWR fuel with burn-ups from 62.5 to 83.1 GWd/tU. It is found that the high burn-up structure penetrated much deeper than initially reported. The local burn-up threshold for the formation of the high burn-up structure in those fuels with grain sizes in the normal range lay between 60 and 75 GWd/tU. The high burn-up structure was not detected by EPMA in a fuel that had a grain size of 78 μm although the local burn-up at the pellet rim had exceeded 80 GWd/tU. It is concluded that fission gas had been released from the high burn-up structure in three PWR fuel sections with burn-ups of 70.4, 72.2 and 83.1 GWd/tU. In the rim region of the last two sections at the locations where XRF indicated gas release the local burn-up was higher than 75 GWd/tU.     

Preparation and characterization of the simulated burnup americium-containing uranium–plutonium mixed oxide fuel

In order to investigate the effect on fuel thermophysical properties when adding americium and selected fission products to uranium–plutonium mixed oxide (MOX) fuel, simulated low decontamination MOX fuel with high burn-ups to 250 GWd/t, has been prepared and subjected to characterization tests, elastic moduli measurements and melting temperature measurement. Elastic moduli for the simulated low decontamination MOX fuel were almost the same level as fuel without americium and fission products and decrease in the moduli was slight with increasing simulated burn-up. The melting temperature of high burn-up, low decontamination MOX fuel may be estimated by using the findings on the effect of americium, plutonium addition and fission products accumulation.     

High burn-up operation and MOX burning in LWR; Effects of burn-up and extended cooling period of spent fuel on vitrification and disposal

Looking ahead to final disposal of high-level radioactive waste arising from further utilization of nuclear energy, the effects of high burn-up of light-water reactors (LWR) with UO₂ and MOX fuel and extended cooling period of spent fuel on waste management and disposal were discussed. It was assumed that the waste loading of waste glass is restricted by three factors: heat generation rate, MoO₃ content, and platinum group metal content. As a result of evaluation for effects of extended cooling period, the waste loading of waste glass from both UO₂ and MOX spent fuel could be increased in the current vitrification technology. For the storage of waste glass from MOX spent fuel with higher waste loading, however, those waste glass require long storage period prior to geological disposal because decay heat of ²⁴¹Am contributes significantly. Therefore, the evaluation of effects of Am separation on the storage period was performed. Furthermore, heat transfer calculation was carried out in order to evaluate the temperature of buffer material in a geological repository. The results showed, 70 to 90% of Am separation is sufficiently effective in terms of thermal feasibility of a repository.     

Irradiation performance of fast reactor MOX fuel pins with ferritic/martensitic cladding irradiated to high burnups

The ACO-3 irradiation test, which attained extremely high burnups of about 232 GWd/t and resisted a high neutron fluence (E > 0.1 MeV) of about 39 × 10²⁶ n/m² as one of the lead tests of the Core Demonstration Experiment in the Fast Flux Test Facility, demonstrated that the fuel pin cladding made of ferritic/martensitic HT-9 alloy had superior void swelling resistance. The measured diameter profiles of the irradiated ACO-3 fuel pins showed axially extensive incremental strain in the MOX fuel column region and localized incremental strain near the interfaces between the MOX fuel and upper blanket columns. These incremental strains were as low as 1.5% despite the extremely high level of the fast neutron fluence. Evaluation of the pin diametral strain indicated that the incremental strain in the MOX fuel column region was substantially due to cladding void swelling and irradiation creep caused by internal fission gas pressure, while the localized strain near the MOX fuel/upper blanket interface was likely the result of the pellet/cladding mechanical interaction (PCMI) caused by cesium/fuel reactions. The evaluation also suggested that the PCMI was effectively mitigated by a large gap size between the cladding and blanket column.     

Thermal conductivity evaluation of high burnup mixed-oxide (MOX) fuel pellet

The thermal conductivity formula of fuel pellet which contains the effects of burnup and plutonium (Pu) addition was proposed based on the Klemens’ theory and reported thermal conductivities of unirradiated (U, Pu) O₂ and irradiated UO₂ pellets. The thermal conductivity of high burnup MOX pellet was formulated by applying a summation rule between phonon scattering parameters which show the effects of plutonium addition and burnup. Temperature of high burnup MOX fuel was evaluated based on the thermal conductivity integral which was calculated from the above-mentioned thermal conductivity formula. Calculated fuel temperatures were plotted against the linear heat rates of the fuel rods, and were compared with the fuel temperatures measured in a test reactor. Since both values agreed well, it was confirmed that the proposed thermal conductivity formula of MOX pellets is adequate.     

ADAGIO technique: From UO2 fuels to MOX fuels

The amount of gas at the grain boundaries plays an important role in the fuel transient behaviour during accident conditions, such as a loss-of-coolant accident (LOCA) or a reactivity-initiated accident (RIA). Direct experimental determination of the grain boundary gas inventory has been performed for MOX fuel irradiated in an EDF pressurised water reactor (PWR) using the ADAGIO technique (ADAGIO is a French acronym meaning ‘Discriminatory Analysis of Accumulated Inter-granular and Occluded Gas’). The ADAGIO protocol applied to a MOX MIMAS fuel produced inter-granular gas fraction results that were consistent with those reached with other methods of evaluation i.e. electron probe microanalysis (EPMA). Furthermore, a new methodology for the numerical treatment of ⁸⁵Kr release kinetics which was developed for UO₂ was applied to MOX fuels. The corresponding results evidenced two types of release kinetics. These kinetics were attributed to the inter-granular bubbles of the UO₂ matrix and the bubbles located in the restructured zones, i.e. Pu agglomerates.