Microstructure and elemental distribution of americium-containing uranium plutonium mixed oxide fuel under a short-term irradiation test in a fast reactor

In order to investigate the effect of americium addition in MOX fuel on the irradiation behavior, the ‘Am-1’ program is being conducted in the experimental fast reactor Joyo. The Am-1 program consists of two short-term irradiation tests of 10 min and 24 h irradiations and a steady-state irradiation test. The short-term irradiation tests were successfully completed and the post irradiation examinations (PIEs) are in progress. This paper reports on the results of PIEs for Am-containing MOX fuel irradiated for 10 min. MOX fuel pellets containing 3% or 5% Am were fabricated in a shielded air-tight hot cell using a remote handling technique. The oxygen to metal ratio (O/M) of these fuel pellets was 1.98. They were irradiated at peak linear heating rate of about 43 kW m⁻¹. Focus was being placed on migration behavior of Am during the irradiation. The ceramography results showed that structural changes such as lenticular pores and a central void occurred early, within the brief 10 min of irradiation. The results of electron probe microanalysis revealed that the concentration of Am increased in the vicinity of the central void.     

Behavior of Si impurity in Np-Am-MOX fuel irradiated in the experimental fast reactor Joyo

The irradiation behavior of uranium-plutonium mixed oxide fuels containing a large amount of silicon impurity was examined by post-irradiation examination. Influences of Si impurity on fuel restructuring and cladding attack were investigated in detail. Si impurity, along with Am, Pu and O were transported by spherical pores and cylindrical tubular pores to the fuel center during fuel restructuring of the Np-Am-MOX fuel, where a eutectic reaction of fuel and Si-rich inclusions occurred. After fuel restructuring of the Np-Am-MOX fuel, Si-rich inclusions without fuel constituents were agglomerated at fuel crack openings where shallow attacks on the inner wall of the cladding were seen. Such shallow attacks on the inner wall of the cladding were likewise observed near the location of fuel cracks in long-term steady-state irradiated MOX fuels. Evidence of these shallow attacks on the inner wall of the cladding remained after fuel restructuring in normal MOX fuel. However, grain boundary corrosion of the cladding inner wall at the opening of the fuel cracks was selective and was marked in MOX fuel at higher oxygen potential by the release of reactive fission products such as Cs and Te in comparison with other regions of cladding wall.     

Oxygen potentials of mixed oxide fuels for fast reactors

Oxygen potentials of homogenous (Pu_0.2U_0.8)O_2−x and (Am_0.02Pu_0.30Np_0.02U_0.66)O_2−x which have been developed as fuels for fast breeder reactors were measured at temperatures of 1473-1623 K by a gas equilibrium method using an (Ar, H₂, H₂O) gas mixture. The measured oxygen potentials of (Pu_0.2U_0.8)O_2−x were about 25 kJ mol⁻¹ lower than those of (Pu_0.3U_0.7)O_2−x measured previously and were consistent with the values calculated by Besmann and Lindemer’s model. The measured oxygen potentials of (Am_0.02Pu_0.30Np_0.02U_0.66)O_2−x were slightly higher than those of MOX without minor actinides. No fuel-cladding chemical interaction is affected significantly by adding their minor actinides.     

Radial redistribution of actinides in irradiated FR-MOX fuels

The redistributions of neptunium, plutonium and americium during two kinds of short-term irradiation tests for 10 min and 24 h at high linear heating rate around 430 W cm⁻¹ were studied in the uranium and plutonium mixed oxide fuel containing Am and/or Np. It was found in the irradiation test for 24 h that the concentrations of Pu and Am increased toward the central void, but there was no change in the concentration of Np. The obtained experimental redistributions of Am and Pu were analyzed, based on both pore migration and thermal diffusion models. As a result, the calculated redistributions of Pu and Am showed good agreements with the experimentally obtained ones.     

Equilibrium and nonequilibrium molecular dynamics simulations of heat conduction in uranium oxide and mixed uranium-plutonium oxide

The thermal conductivity of nuclear fuels such as UO_2+x and (U,Pu)O_2−x has been calculated by the molecular dynamics (MD) simulation in terms of oxygen stoichiometric parameter x, temperature and Pu content. In the present study, the MD calculations were carried out in both equilibrium (EMD) and nonequilibrium (NEMD) systems. In the EMD simulation, the thermal conductivity was defined as the time-integral of the correlation function of heat fluxes according to the Green-Kubo relationship. Meanwhile, in the homogeneous NEMD, it was given by the ratio of the time-averaged heat flux to the perturbed external force subjected to each particle in the simulated cell. NEMD, as compared with EMD, gave somewhat precise results efficiently. Furthermore, both MD calculations showed that the thermal conductivity of these oxide fuels decreased with increase of temperature and defects, i.e. excess oxygen or vacancy, and was rather insensitive to Pu content for the stoichiometric fuel.     

Design of a fuel element for a lead-cooled fast reactor

The options of a lead-cooled fast reactor (LFR) of the fourth generation (GEN-IV) reactor with the electric power of 600 MW are investigated in the ELSY Project. The fuel selection, design and optimization are important steps of the project. Three types of fuel are considered as candidates: highly enriched Pu-U mixed oxide (MOX) fuel for the first core, the MOX containing between 2.5% and 5.0% of the minor actinides (MA) for next core and Pu-U-MA nitride fuel as an advanced option. Reference fuel rods with claddings made of T91 ferrite-martensitic steel and two alternative fuel assembly designs (one uses a closed hexagonal wrapper and the other is an open square variant without wrapper) have been assessed. This study focuses on the core variant with the closed hexagonal fuel assemblies. Based on the neutronic parameters provided by Monte-Carlo modeling with MCNP5 and ALEPH codes, simulations have been carried out to assess the long-term thermal-mechanical behaviour of the hottest fuel rods. A modified version of the fuel performance code FEMAXI-SCK-1, adapted for fast neutron spectrum, new fuels, cladding materials and coolant, was utilized for these calculations. The obtained results show that the fuel rods can withstand more than four effective full power years under the normal operation conditions without pellet-cladding mechanical interaction (PCMI). In a variant with solid fuel pellets, a mild PCMI can appear during the fifth year, however, it remains at an acceptable level up to the end of operation when the peak fuel pellet burnup ∼80 MW d kg⁻¹ of heavy metal (HM) and the maximum clad damage of about 82 displacements per atom (dpa) are reached. Annular pellets permit to delay PCMI for about 1 year. Based on the results of this simulation, further steps are envisioned for the optimization of the fuel rod design, aiming at achieving the fuel burnup of 100 MW d kg⁻¹ of HM.     

A method for the quantification of total xenon concentration in irradiated nuclear fuel with SIMS and EPMA

A new method for the quantitative determination of the total xenon concentration in irradiated nuclear fuel is presented. The SIMS measurement of xenon enables the detection of the gas filling bubbles which are not detected with EPMA. The quantification is achieved using the EPMA data as reference at position where no or nearly no bubbles are detected. A new approach using the complementary information given by EPMA, SEM and SIMS is proposed, it opens new horizons for the characterisation of fission gases in irradiated nuclear fuel.     

The irradiation test of inert-matrix fuel in comparison to uranium plutonium mixed oxide fuel at the halden reactor

Conservative modelling for pin layout shows that the relatively low thermal conductivity of Inert-Matrix Fuel (IMF) causes higher temperatures and therefore higher fission gas release than in uranium plutonium mixed oxide (MOX). According to neutronic calculations, performance differences will also arise from different evolutions of the respective radial power and burnup distributions. Modelling of these effects as well as a 10% greater production of Xe in the thermal spectrum of the Halden reactor is well within the capabilities of appropriate codes. Some of the data and models used for the pre-calculations are preliminary and will be revised after the first experimental data have become available.     

Minor actinide transmutation in fast reactor metal fuels irradiated for 120 and 360 equivalent full-power days

An irradiation experiment on uranium–plutonium–zirconium (U–Pu–Zr) alloys containing 5 wt% or less minor actinides (MAs) and rare earths was carried out in the Phénix fast reactor. The isotope compositions of the fuel alloys irradiated for 120 and 360 equivalent full-power days (EFPDs) were chemically analyzed by inductively coupled plasma–mass spectrometry after 3.3–5.3 years of cooling. The results of chemical analysis indicated that the discharged burnups of the fuel alloys irradiated for 120 and 360 EFPDs were 2.1–2.5 and 5.3–6.4 at%, respectively. The changes in the isotopic abundances of plutonium, americium, and curium during the irradiation experiment were assessed to discuss the transmutation performance of MA nuclides added to U–Pu–Zr alloy fuel. Multigroup three-dimensional diffusion and burnup calculations accurately predicted the changes in these isotopic abundances after fuel fabrication. An evaluation of the MA transmutation ratio based on the results of chemical analysis revealed that the quantity of MA elements in the U–19Pu–10Zr–5MA (wt%) alloy decreased by about 20% during the irradiation experiment for 360 EFPDs.     

Dissolution behavior of irradiated mixed oxide fuel with short stroke shearing for fast reactor reprocessing

An efficient dissolution process was established for future reprocessing in which mixed-oxide (MOX) fuels with high plutonium contents and dissolver solution with high heavy-metal (HM) concentrations (more than 500 g dm^?3) will be treated. This dissolution process involves short stroke shearing of fuels (～10 mm in length). The dissolution kinetics of irradiated MOX fuels and the effects of the Pu content, HM concentration, and fuel form on the dissolution rate were investigated. Irradiated fuel was found to dissolve as 10²–10³ times fast as non-irradiated fuel, but the rate decreased with increasing Pu content. Kinetic analysis based on the fragmentation model, which considers the penetration and diffusion of nitric acid through fuel matrices prior to chemical reaction, indicated that the dissolution rate of irradiated fuel was affected not only by the volume ratio of liquid to solid (L/S ratio) but also by the exposed surface area per unit mole of nitric acid (A/m ratio). The penetration rate of nitric acid is expected to be decreased at high HM concentrations by a reduction in the L/S ratio, but enhanced by shearing the fuel pieces with short strokes and thus enlarging the A/m ratio.     

Comparative study of minor actinide transmutation in sodium and lead-cooled fast reactor cores

This paper shows that lead-cooled and sodium-cooled fast reactors (LFRs and SFRs) can preferentially consume minor actinides without burning plutonium, both in homogeneous and in heterogeneous mode. The former approach consists of admixing about 5% of minor actinides (MAs) into uranium–plutonium fuels in the core and using a limited number of thermalising pins consisting of UZrH_1.6. These are needed to keep the negative Doppler feedback larger than the positive coolant reactivity coefficient. Our Monte Carlo burn-up calculations showed that a 600 MW_e LFR self-breeder without blankets can burn an average of around 67 kg annually of MAs with a reactivity swing of only about −0.7$ per year. The reactivity swing of a corresponding 600 MW_e SFR is more than three times larger due to the poorer breeding and half the critical mass in comparison to the LFR. However, when axial and radial blankets loaded with 10% MAs are added, the SFR burns 25% more MAs (131 kg/yr) and breeds 30% more Pu (150 kg/yr) than an equally sized LFR. When only the blankets are loaded with MAs, the SFR breeds 30% more Pu (198 kg/yr) and still burns about 60 kg a year of MAs. However, in terms of severe accident behaviour, the LFR, with its superior natural coolant circulation and larger heat capacity, has definite advantages.     

Irradiation analysis of U, Am samples irradiated in experimental fast reactor “Joyo” for protected plutonium production in fast breeder reactor blanket

Americium is a key element to design the FBR based nuclear fuel cycle, because of its long-term high radiological toxicity as well as a resource of even-mass-number plutonium by its transmutation in reactors, which contributes the enhancement of proliferation resistance. The present paper summarizes analysis of the individual Am and U samples irradiation in Joyo to re-evaluate the results of Pu isotopes in the measure of proliferation resistance, and to combine the results for the prediction of DU-Am irradiation especially in the production of Pu isotopes. By the prediction of DU-Am oxide fuel in fast reactor environment with detail fuel irradiation analysis, it was confirmed that neutron moderation and fuel size affects the produced Pu isotope and its vector due to the very high sensitivity of ²³⁸U resonance capture reaction, the larger diameter fuel is more preferable in the case of moderated neutron spectrum environment for denaturing Pu in fast reactor blanket. Finally proliferation resistance of all the Pu produced in U, Am sample irradiation and DU-Am fuel irradiation prediction were evaluated based on decay heat and spontaneous fission neutron rate, and it was confirmed ²⁴¹Am produces un-attractive Pu to abuse from the beginning to the end of irradiation, and more than 2% of ²⁴¹Am doping is required to enhance the proliferation resistance of Pu to MOX grade and Kessler’s proposal in moderated neutron spectrum environment in fast reactor.     

Fracture behavior of austenitic stainless steels irradiated in PWR

Fracture behavior of cold-worked 316 stainless steels irradiated up to 73 dpa in a pressurized water reactor was investigated by impact testing at −196, 30 and 150 °C, and by conventional tensile and slow tensile testing at 30 and 320 °C. In impact tests, brittle IG mode was dominant at −196 °C at doses higher than 11 dpa accompanying significant decrease in absorbed energy. The mixed IG mode, which was characterized by isolated grain facets in ductile dimples, appeared at 30 and 150 °C whereas the fracture occurred macroscopically in a ductile manner. The sensitivity to IG or mixed IG mode was more pronounced for higher dose and lower test temperature. In uniaxial tensile tests, IG mode at a slow strain rate appeared only at 320 °C whereas mixed IG mode appeared at both 30 and 320 °C at a fast strain rate. A compilation of the results and literature data suggested that IG fracture exists in two different conditions, low-temperature high-strain-rate (LTHR) and high-temperature low-strain-rate (HTLR) conditions. These two conditions for IG fracture likely correspond to two different deformation modes, twining and channeling.     

Study of atomic clusters in neutron irradiated reactor pressure vessel surveillance samples by extended X-ray absorption fine structure spectroscopy

Copper and nickel impurities in nuclear reactor pressure vessel (RPV) steel can form nano-clusters, which have a strong impact on the ductile-brittle transition temperature of the material. Thus, for control purposes and simulation of long irradiation times, surveillance samples are submitted to enhanced neutron irradiation. In this work, surveillance samples from a Swiss nuclear power plant were investigated by extended X-ray absorption fine structure spectroscopy (EXAFS). The density of Cu and Ni atoms determined in the first and second shells around the absorber is affected by the irradiation and temperature. The comparison of the EXAFS data at Cu and Ni K-edges shows that these elements reside in arrangements similar to bcc Fe. However, the EXAFS analysis reveals local irradiation damage in the form of vacancy fractions, which can be determined with a precision of ∼5%. There are indications that the formation of Cu and Ni clusters differs significantly.     

Ion beam analysis of materials in the PBMR reactor

South Africa is developing a new type of high temperature nuclear reactor, the so-called pebble bed modular reactor (PBMR). The planned reactor outlet temperature of this gas-cooled reactor is approximately 900 °C. This high temperature places some severe restrictions on materials, which can be used. The name of the reactor is derived from the form of the fuel elements, which are in the form of pebbles, each with a diameter of 60 mm. Each pebble is composed of several thousands of coated fuel particles. The coated particle consists of a nucleus of UO₂ surrounded by several layers of different carbons and SiC. The diameter of the fuel particles is 0.92 mm. A brief review will be given of the advantages of this nuclear reactor, of the materials in the fuel elements and their analysis using ion beam techniques.     

Some aspects of risk reduction strategy by multiple recycling in fast burner reactors of the plutonium and minor actinide inventories

This paper shows the impact of recycling light water reactor (LWR) mixed oxide (MOX) fuel in a fast burner reactor on the plutonium (Pu) and minor actinide (MA) inventories and on the related radioactivities. Reprocessing of the targets for multiple recycling will become increasingly difficult as the burnup increases. Multiple recycling of Pu + MA in fast reactors is a feasible option which has to be studied very carefully: the Pu (except the isotopes Pu-238 and Pu-240), Am and Np levels decrease as a function of the recycle number, while the Cm-244 level accumulates and gradually transforms into Cm-245. Long cooling times (10 + 2 years) are necessary with aqueous processing. The paper discusses the problems associated with multiple reprocessing of highly active fuel types and particularly the impact of Pu-238, Am-241 and Cm-244 on the fuel cycle operations. The calculations were performed with the zero-dimensional ORIGEN-2 code. The validity of the results depends on that of the code and its cross-section library. The time span to reduce the initial inventory of Pu + MA by a factor of 10 amounts to 255 years when average burnups are limited to 150 GW · d t⁻¹ (tonne).