Analysis of measured isotopic compositions by CASMO5 coupled with a JENDL-4.0 base library for irradiated fuel of light water reactors

Measured isotopic compositions of UO₂ and MOX fuel samples taken from irradiated light water reactor fuel assemblies were analyzed by CASMO5 coupled with a JENDL-4.0 base library to assess the uncertainties in the calculated isotopic compositions on heavy and fission product nuclides. The burnup calculations for the analysis were performed based on a single-assembly model taking into account the detail fuel assembly specifications and irradiation histories. For the MOX fuel samples, a multiple-assembly model was also adopted taking into account the effect of the surrounding UO₂ fuel assemblies. The average and standard deviation of the biases (C/E ? 1's (here C and E are calculated and measured results, respectively)) were calculated for each nuclide separately on the PWR and BWR UO₂ fuel samples. The averaged biases for ²³⁵U, ²³⁶U, ²³⁹Pu, ²⁴⁰Pu, ²⁴¹Pu and ²⁴²Pu were 2.7%, ?0.9%, 0.3%, 0.7%, ?2.4% and ?1.7% for PWR UO₂ samples, and 6.7%, ?1.5%, 2.5%, ?0.6%, 0.4% and ?0.1% for BWR UO₂ samples, respectively. The biases with the single-assembly model on the MOX fuel samples showed large positive values of ²³⁹Pu, and application of the multiple-assembly model reduced the biases as reported in our previous studies.     

Analysis of measured isotopic compositions of high-burnup PWR MOX and UO2 fuels in the MALIBU program

The measured isotopic compositions of fuel samples taken from high-burnup spent PWR MOX and UO₂ assemblies in the MALIBU program has been analyzed by lattice physics codes. The measured isotopes were U, Np, Pu, Am, and Cm isotopes and about 30 major fission product nuclides. The codes used in the present study were a continuous-energy Monte Carlo burnup calculation code (MVP-BURN) and a deterministic burnup calculation code (SRAC) based on the collision probability method. A two-dimensional multi-assembly geometrical model (2 × 2 model) was mainly adopted in the analysis in order to include the fuel assemblies adjoining the relevant fuel assembly, from which the samples were taken. For the MOX sample, the 2 × 2 model significantly reduces the deviations of the calculated results from the measurements compared with a single assembly model. The calculation results of MVP-BURN in the 2 × 2 model reproduce the measurements of U, Np, and Pu isotopes within 5% for the MOX sample of 67 GWd/t. The deviations of their calculated results of U, Np, and Pu isotopes from the measurements are less than 7% for the UO₂ sample of 72 GWd/t.     

Prospective Power-Reactor Fuel Cycles Based on Water-Free Reprocessing of Spent Fuel

A pyroelectrochemical process for reprocessing spent fuel and fabricating granular oxides UO₂, PuO₂ or (U, Pu)O₂ from chloride melts has been developed at the Scientific-Research Institute of Nuclear Reactors for a prospective nuclear fuel cycle. The basic equipment has been developed. The basic results of a comprehensive study of fuel elements with vibrationally compacted (U, Pu)O₂ fuel for fast reactors are presented. The performance of the reactors remains high up to 30% burnup in standard BOR-60 reactor fuel assemblies and 32% burnup in experimental fuel elements. An assessment is made of the effectiveness of the pyroelectrochemical methods and vibrational compaction technology for plutonium utilization.     

Application of Multiband Method to Pin Cell Calculations

Abstract

In order to accurately calculate effective neutron cross sections in the resonance energy region, the multiband method has been applied to cell calculations. Cell calculations for UO² and MOX fuels of light water reactors have been performed and the results were compared with those of a continuous energy Monte Carlo code VIM and the conventional self-shielding method using the Dancoff factor.

The k∞values calculated by the multiband method agreed with those of the VIM calculations within 0.20% Δk for the UO² fuel cell and within 0.30% Δk for the MOX fuel cell, respectively, whereas the Dancoff factor method yielded about l.l%Δk errors for the two cells. The element- wise contribution to this error was investigated, and it was found that the effective microscopic cross sections, particularly those for the giant resonances of ²³⁸U, calculated by the multiband method were in good agreement with those of VIM. It was also found that interference effect between ²³⁸U and ²³⁵U resonances in the UO² fuel and that between ²³⁸U and ²³⁹Pu resonances in the MOX fuel made about 0.20%Δk contributions to k∞ in both fuel cells.     

Analyses of used BWR fuel assay data with the integrated burnup code system SWAT4.0

Criticality safety of the fuel debris from the Fukushima Daiichi Nuclear Power Plant is one of the most important issues, and the adoption of burnup credit is desired for criticality safety evaluation. To adopt the burnup credit, validation of the burnup calculation codes is required. Assay data of the used nuclear fuel irradiated by the Fukushima Daini Nuclear Power Plant Unit 2 are evaluated to validate the SWAT4.0 code for solving the BWR fuel burnup problem. The calculation results revealed that the number densities of many heavy nuclides and fission products show good agreement with the experimental data, except for those of ²³⁷Np, ²³⁸Pu, and samarium isotopes. These differences were considered to originate from inappropriate assumption of void fraction. Our results implied overestimation of the (n, γ) cross-section of ²³⁷Np in JENDL-4.0. The Calculation/Experiment – 1 (C/E–1) value did not depend on the type of fuel rod (UO₂ or UO₂–Gd₂O₃), which was similar to the case of PWR fuel. The differences in the number densities of ²³⁵U, ²³⁹Pu, ²⁴⁰Pu, ²⁴¹Pu, ¹⁴⁹Sm, and ¹⁵¹Sm have a large impact on k_eff. However, the reactivity uncertainty related to the burnup analysis was less than 3%. These results indicate that SWAT4.0 appropriately analyzes the isotopic composition of BWR fuel, and it has sufficient accuracy to be adopted in the burnup credit evaluation of fuel debris.     

Comparative study of actinide and fission product inventory of HEU and potential LEU fuels for MNSRs

A comparative study of fuel burnup and buildup of actinides and fission products for potential LEU fuels (UO₂ and U–9Mo) with existing HEU fuel (UAl₄–Al, 90% enriched) for a typical Miniature Neutron Source Reactor (MNSR) has been carried-out using the WIMSD4 computer program. For the complete burnup, the UAl₄–Al, UO₂ and U–9Mo based systems show a total consumption of 6.89, 6.83 and 6.88 g of ²³⁵U, respectively. Relative to 0.042 g ²³⁹Pu produced in case of UAl₄–Al HEU core, UO₂ and U–9Mo based cores have been found to yield 0.793 and 0.799 g, respectively, indicating much larger values of conversion ratios and correspondingly high values of fuel utilization factor. The end-of-cycle activity of the HEU core has been found 2284 Ci which agrees well with value found by Khattab where as for UO₂ based and U–9Mo based LEU cores show 1.8 and 4.8% increase with values 2326 and 2394 Ci, respectively.     

Helium behavior in oxide nuclear fuels: First principles modeling

UO₂ and (U, Pu)O₂ solid solutions (the so-called MOX) nowadays are used as commercial nuclear fuels in many countries. One of the safety issues during the storage of these fuels is related to their self-irradiation that produces and accumulates point defects and helium therein.We present density functional theory (DFT) calculations for UO₂, PuO₂ and MOX containing He atoms in octahedral interstitial positions. In particular, we calculated basic MOX properties and He incorporation energies as functions of Pu concentration within the spin-polarized, generalized gradient approximation (GGA) DFT calculations. We also included the on-site electron correlation corrections using the Hubbard model (in the framework of the so-called DFT + U approach). We found that PuO₂ remains semiconducting with He in the octahedral position while UO₂ requires a specific lattice distortion. Both materials reveal a positive energy for He incorporation, which, therefore, is an exothermic process. The He incorporation energy increases with the Pu concentration in the MOX fuel.     

Determination of Li-6/Li-7 Isotopic Ratio by Means of Thermogravimetric Analysis for Lithium Sulphate Monohydrate

Plutonium concentrations and burnup at Pu spots were calculated in U-Pu mixed oxide (MOX) fuel pellets for light water reactors with the neutron transport and burnup calculation code VIMBURN. The calculation models were suggested for Pu spots and U matrices in a heterogeneous MOX fuel pellet. The calculated Pu concentrations and burnup at Pu spots were compared with the PIEs data in a MOX pellet (38.8 MWd/kgHM). The calculated Pu concentrations agreed by 5–18% with the measured ones, and the calculated burnup did by less than 10% with the estimated one with the measured Nd concentrations. Commercial PWR types of MOX fuels were also analyzed with the calculation code and the models. Burnup at Pu spot increased as the distance was greater from the radial center of a MOX fuel pellet. Burnup at Pu spots in the peripheral region became 3–5 times higher than pellet average burnup of 40 MWd/kgHM. The diameters (20–100 μm) of Pu spots were not found a significant factor for burnup at Pu spots. In the outer half volume region (outer than r/r _o=0.7) of a MOX fuel pellet, burnup at Pu spots exceeded 70MWd/kgHM (the threshold burnup of microstructure change in UO₂ fuel pellet) at pellet average burnup of 1430 MWd/kgHM.     

Nuclear Analysis of PIE Data of Irradiated BWR 8×8-2 and 8×8-4 UO2 Fuel Assemblies

The measured pellet average inventories of actinides and fission product nuclides on the fifteen samples taken from a three-cycle irradiation BWR 8×8-2 UO₂ assembly were compared with those of assembly burnup calculations using a collision probability method (SRAC) with the JENDL-3.2 nuclear data library. The present calculations overestimate the inventories of ²³⁵U, well reproduce those of ²³⁹Pu and ²⁴⁰Pu, yet underestimate those of ²³⁶U, ²³⁷Nd, ²³⁸Pu, ²⁴¹Pu, and ²⁴²Pu. The inventories of minor actinides are underestimated by the present analysis except for ²⁴¹Am. The major FP nuclides contributing to neutron absorption such as Nd, Cs, Eu, and Sm are almost well reproduced by the present calculations. The measured pellet average burnups and major actinide inventories on the twenty samples taken from four BWR 8×8-4 UO₂ assemblies were also compared with those of the burnup calculations using SRAC and a continuous energy Monte Carlo burnup analysis code (MVP-BURN). Most of the calculated pellet average burnups of both codes agree with the measurements within the range of ±10%. The general trends of the measured pellet radial distributions of actinide and FP nuclides on six samples of the 8×8-4 UO₂ assemblies were well reproduced by the burnup calculations of MVP-BURN.     

Releases of Cesium and Poorly Volatile Elements from UO2 and MOX Fuels under Severe Accident Conditions

Radionuclide release from fuel under severe accident conditions has been investigated in the VEGA program at the Japan Atomic Energy Agency. In this program, three types of fuel, two UO₂ fuels irradiated at PWR and BWR and a MOX fuel irradiated at the ATR Fugen, were heated up to about 3130K in helium atmosphere at 0.1 MPa. Comparison of experimental data and evaluation with computer code analyses showed that Cs release is essentially identical among the three fuels. The Cs release from fuel may differ below about 1770K due to a difference in migration to grain boundaries during irradiation. The difference was not also observed for releases of poorly volatile elements, namely, U, Pu, Sr and Mo between UO₂ and MOX fuels. The release rate of Pu became slightly higher than that of U at 3130 K. The release rate of Sr increased at 3130 K, while that of Mo was quite low at temperatures above 2310 K.     

Fast Reactor Operating on Uranium–Plutonium Oxide Fuel in a Self-Regulatable Regime

Mathematical simulation is used to show that it is possible to develop a fast reactor operating on uranium–plutonium oxide fuel (UO₂)_1–x (PuO₂) _x , the same for all fuel elements in the core, and with uranium carbide in breeding elements with heavy coolant (PbBi eutectic). A self-regulatable regime is obtained in the reactor. This enhances safety while minimizing control. Tailings uranium with 0.1% ²³⁵U and a mixture of plutonium isotopes, which is obtained from spent fuel, making it possible to conduct operation in an actinide-closed fuel cycle, is used in the fuel and uranium carbide. ²³⁸U is actually consumed in the reactor, but most fission products are produced from ²³⁹Pu.     

Compression and Decompression Waves in Steam-Water System

The ratio of the γactivities per fission from fission products of ²³⁹Pu and ²³⁵U, and its time dependence were measured by double fission chamber technique. The γ-activity from the fission products of ²³⁹Pu fission was lower than the corresponding activity relevant to ²³⁵U fissions. The ratio varied with the cooling time allowed after irradition.

This ratio was applied to power distribution measurements by γ-scanning method in multi-region cores composed of PuO₂-UO₂ and UO₂ fuels. To obtain the relative power, the measured γ-activities from the fission products in the fuel rods were corrected for the difference between the γ-activities per fission from the fission products.     

Fundamental Study of the Sulfide Reprocessing Process for Oxide Fuel (I) Study on the Pu,MA and FP Tracer-Doped U3O8

For the recovery of fuel materials from spent nuclear fuel, a novel reprocessing process based on the selective sulfurization of fission products (FP) has been proposed, where FP and minor actinides (MA) are first sulfurized by CS₂ gas, and then, dissolved by a dilute nitric acid solution. Consequently, the fuel elements are recovered as UO₂ and PuO₂. As a basic research of this new concept, the sulfurization and dissolution behaviors of U, Pu, Np, Am, Eu, Cs, and Sr were investigated by γ-ray and α spectrometries in this paper using ²³⁶Pu-, ²³⁷Np-, ²⁴¹Am-, ¹⁵²Eu-, ¹³⁷Cs-, and ⁸⁵Sr-doped U₃O₈ samples. The dependence of the dissolution ratio of each element on the sulfurization temperature was studied and reasonably explained by combining the information of the sulfide phase analysis and the chemical thermodynamics of the dissolution reaction. The sulfurization temperature ranging from 350 to 450°C seems to be promising for the separation of FP and MA from U and Pu, since a clear difference in the dissolution ratio between FP and U was derived by the sulfurization treatment in this temperature range.     

MgO-pyrochlore composite as an inert matrix fuel: Neutronic and thermal characteristics

Inert matrix fuels are an important component of advanced nuclear fuel cycles, as they provide a means of utilizing plutonium and reducing the inventory of ‘minor’ actinides. We examine the neutronic and thermal characteristics of MgO-pyrochlore (A₂B₂O₇: La₂Zr₂O₇, Nd₂Zr₂O₇ and Y₂Sn₂O₇) composites as inert matrix fuels in boiling water reactors. By incorporating plutonium with resonance nuclides, such as Am, Np and Er, in the A-site of pyrochlore, the k_infvs. burn-up curves are shown to be similar to those of UO₂, although the Doppler coefficients are less negative than UO₂. The Pu depletion rates are 88-90% (²³⁹Pu) and 54-58% (total Pu) when the inert matrix fuels experience a burn-up equivalent of 45 GWd/tHM UO₂. Because of the high thermal conductivity of MgO, the center-line temperatures of the MgO-pyrochlore composites at 44.0 kW/m are lower than those of UO₂ pellets. After burn-up, the A-site cation composition is 15-35 at.% lower than that of the B-site cations in pyrochlore (e.g., A_1.84B_2.17O_7.00) due to the fission of Pu in the A-site and the presence of fission product elements in the A- and B-sites of the pyrochlore structure.     

The corrosion of spent UO2 fuel in synthetic groundwater

Leaching of high burnup BWR fuel for up to 3 years showed that both U and Pu attain saturation rapidly at pH 8.1, giving values of 1–2 mg/l and 1 μg/l respectively. The leaching rate for Sr-90 decreased from about 10⁻⁵/d to 10⁻⁷/d but was always higher than the rates for U, Pu, Cm, Ce, Eu and Ru. Congruent dissolution was only attained at pH values of about 4. When reducing conditions were inposed on the pH 8.1 groundwater by means of H₂/Ar in the presence of a Pd catalyst, significantly lower leach rates were attained.The hypothesis that alpha radiolytic decomposition of water is a driving force for UO₂ corrosion even under reducing conditions has been examined in leaching tests on low burn-up (low alpha dose-rate) fuel. No significant effect of alpha radiolysis under the experimental conditions was detected. Thermodynamically the calculated uranium solubilities in the pH range 4–8.2 generally agreed well with the measured ones, although assumptions made for certain parameters in the calculations limit the validity of the results.     

Leaching of actinide elements from simulated fuel debris into seawater

For the prediction of the leaching behavior of actinide elements contained in the fuel debris that has arisen from the severe accident in Fukushima Daiichi Nuclear Power Station (NPS), a simulated fuel debris consisting of UO₂–ZrO₂ solid solution doped with ¹³⁷Cs, ²³⁷Np, ²³⁶Pu and ²⁴¹Am tracers was synthesized, and agitated leaching tests were conducted for the simulated fuel debris in seawater. The synthesized simulated fuel debris was immersed and shaken in natural seawater collected at a coast 11 km away from Fukushima Daiichi NPS. The brief leaching test conditions were T = 25 °C and solid–liquid ratio = 4 g/l, and the test duration was up to 31 days. The ratio of tracers leached into seawater from the simulated fuel debris by the agitated leaching test for 4 days was evaluated to be 0.09% for U, 0.01% for Np, 0.01% for Pu, 0.01% for Am and 35.39% for Cs by the α or γ spectrometry of the soluble fraction. The leaching of actinides from the real fuel debris in reactor units 1–3 in Fukushima Daiichi NPS is expected to be suppressed in comparison with that from normal light water reactor spent fuel.     

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.     

Neutron Behavior in Cluster-Type Fuel Lattices, (I)

Lattice parameters φ²⁸, φρ²⁵, ρ²⁸ and C^* were measured on cluster-type fuel lattices of the ATR (Advanced Thermal Reactor) by using a two region critical facility (D₂0-cluster test and H₂O-rod driver regions). Their dependence on lattice pitch, coolant-void ratio and fuel composition (whether UO₂ or PuO₂-UO₂) have been made clear by this experiment.

A foil handling technique has been developed for determining the lattice parameters of the Pu0₂- UO₂ fuel pins, and the resulting measurement errors are almost as small as those obtained on the U0₂ fuel pins.

The effects of the Cd-filter and of the presence of UO₂ buttons in the measurement of ρ²⁸ and χ²⁵ were studied experimentally and correction factors have been determined.

A method of observing the spatial distribution of the γ-ray source in an activated foil has been developed, and the relation between the spatial distribution and the coincidence counting efficiency of the foil has been examined.     

Low cost, proliferation resistant, uranium–thorium dioxide fuels for light water reactors

Our objective is to develop a fuel for the existing light water reactors (LWRs) that, (a) is less expensive to fabricate than the current uranium-dioxide (UO₂) fuel; (b) allows longer refueling cycles and higher sustainable plant capacity factors; (c) is very resistant to nuclear weapon-material proliferation; (d) results in a more stable and insoluble waste form; and (e) generates less high level waste. This paper presents the results of our initial investigation of a LWR fuel consisting of mixed thorium dioxide and uranium dioxide (ThO₂–UO₂). Our calculations using the SCALE 4.4 and MOCUP code systems indicate that the mixed ThO₂–UO₂ fuel, with about 6 wt.% of the total heavy metal U-235, could be burned to 72 MW day kg⁻¹ (megawatt thermal days per kilogram) using 30 wt.% UO₂ and the balance ThO₂. The ThO₂–UO₂ cores can also be burned to about 87 MW day kg⁻¹ using 35 wt.% UO₂ and 65% ThO₂with an initial enrichment of about 7 wt.% of the total heavy metal fissile material. Economic analyses indicate that the ThO₂–UO₂ fuel will require less separative work and less total heavy metal (thorium and uranium) feedstock. At reasonable future costs for raw materials and separative work, the cost of the ThO₂–UO₂ fuel is about 9% less than uranium fuel burned to 72 MW day kg⁻¹. Because ThO₂–UO₂ fuel will operate somewhat cooler, and retain within the fuel more of the fission products, especially the gasses, ThO₂–UO₂ fuel can probably be operated successfully to higher burnups than UO₂ fuel. This will allow for longer refueling cycles and better plant capacity factors. The uranium in our calculations remained below 20 wt.% total fissile fraction throughout the cycle, making it unusable for weapons. Total plutonium production per MW day was a factor of 3.2 less in the ThO₂–UO₂ fuel than in the conventional UO₂ fuel burned to 45 MW day kg⁻¹. Pu-239 production per MW day was a factor of about 4 less in the ThO₂–UO₂ fuel than in the conventional fuel. The plutonium produced was high in Pu-238, leading to a decay heat about three times greater than that from plutonium derived from conventional fuel burned to 45 MW day kg⁻¹ and 20 times greater than weapons grade plutonium. This will make fabrication of a weapon more difficult. Spontaneous neutron production from the plutonium in the ThO₂–UO₂ fuel was about 50% greater than that from conventional fuel and ten times greater than that from weapons grade plutonium. High spontaneous neutron production drastically limits the probable yield of a crude weapon. Because ThO₂ is the highest oxide of thorium while UO₂ can be oxidized further to U₃O₈ or UO₃, ThO₂–UO₂ fuel appears to be a superior waste form if the spent fuel is to be exposed ever to air or oxygenated water. And, finally, use of higher burnup fuel will result in proportionally fewer spent fuel bundles to handle, store, ship, and permanently dispose of.     

Comparison of Calculated Values with Measured Values on the Amount of TRU and FP Nuclides Accumulated in Gadolinium Bearing PWR Spent Fuels

Destructive analyses for five spent fuel samples taken from a Gd bearing fuel assembly were done. The measured amounts of actinides of ^234-238U, ²³⁷Np, ^238-242p_u 241,242m,243Am ^242,244Cm, and fission products of ¹³⁴Cs and ¹⁵⁴Eu were used for evaluating the accuracy of calculation made by CASMO-MICBURN and ORIGEN-2 codes. The effect of Gd on the neutron spectrum was taken into account in the CASMO-MICBURN calculation.

The amounts of ²³⁵U, ²³⁹Pu and ²⁴¹Pu calculated by CASMO-MICBURN agreed well with the observed values within about 3%. On the other hand, the amounts obtained from ORIGEN-2 calculation showed lower values than those observed, especially by —12% in average in ²³⁵U for Gd₂0₃U0₂ fuel. The main cause of this large difference may be attributed to the effect of Gd on the neutron spectrum. The amounts of the other actinides by both calculation codes revealed no significant difference in nearly 10% except for ^242mAm, in which a large fluctuation among the samples was observed. About 10% difference between the measured values and the calculated values was also observed for ¹³⁴Cs, but the calculated values for ¹⁵⁴Eu showed a significant difference from measured values.