Analysis of Measured Isotopic Compositions of High-Burnup BWR MOX Fuel

Analysis of measured isotopic compositions of four high-burnup BWR MOX fuel samples was performed by using a general-purpose neutronic calculation code SRAC and a continuous-energy Monte Carlo burnup code MVP-BURN. The initial Pu fissile content of the samples was 5.52 wt%, and the burnups ranged from 50 to 80 GWd/t. It is confirmed that a geometrical model including the effect of UO₂ assemblies adjacent to the MOX assembly is necessary in the burnup calculations to obtain accurate calculated isotopic compositions. The calculated results of MVP-BURN with JENDL-3.3 taking such effect into account show more accurate results for major actinides (U, Pu, and Am isotopes) and most fission products than those of infinite assembly calculations. The paper also shows the results calculated using SRAC with JENDL-3.3, ENDF/B-VII, and JEFF-3.1.     

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.     

Effect of Pu-Rich Agglomerate in MOX Fuel on a Lattice Calculation

The effect of Pu-rich agglomerates in U-Pu mixed oxide (MOX) fuel on a lattice calculation has been demonstrated. The Pu-rich agglomerate parameters are defined based on the measurement data of MIMAS-MOX and the focus is on the highly enriched MOX fuel in accordance with increased burnup resulting in a higher volume fraction of the Pu-rich agglomerates. The lattice calculations with a heterogeneous fuel model and a homogeneous fuel model are performed simulating the PWR 17 × 17 fuel assembly. The heterogeneous model individually treats the Pu-rich agglomerate and U-Pu matrix, whereas the homogeneous model homogenizes the compositions within the fuel pellet. A continuous-energy Monte Carlo burnup code, MVP-BURN, is used for burnup calculations up to 70 GWd/t. A statistical geometry model is applied in modeling a large number of Pu-rich agglomerates assuming that they are distributed randomly within the MOX fuel pellet. The calculated nuclear characteristics include k-inf, Pu isotopic compositions, power density and burnup of the Pu-rich agglomerates, as well as the pellet-averaged Pu compositions as a function of burnup. It is shown that the effect of Pu-rich agglomerates on the lattice calculation is negligibly small.     

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.     

Lattice physics analysis of measured isotopic compositions of irradiated BWR 9 × 9 UO2 fuel

As part of a validation study of burnup calculations of BWR cores, lattice physics analyses were performed on burnups and isotopic compositions of U, Pu and fission product nuclides measured on five samples taken from 9 × 9 BWR fuel assemblies. Burnup calculations in infinite assembly geometry were carried out using MVP-BURN and SRAC codes coupled with major nuclear data libraries. The burnups determined based on the Nd-148 method were from 27.9 to 64.2 GWd/t. The typical relative differences in isotopic compositions (atom/Total-U) between the burnup calculations and measurements were ?2 ～ 19% for ²³⁴U, ?20 ～ 3% for ²³⁵U, ?1.5 ～ 0.1% for ²³⁶U, ?0.04 ～ 0.02% for ²³⁸U, ?4 ～ 11% for ²³⁸Pu, ?11 ～ ?2% for ²³⁹Pu, ?3 ～ 0% for ²⁴⁰Pu, ?12 ～ ?2% for ²⁴¹Pu and ?2 ～ 3% for ²⁴²Pu. They were ?2 ～ 2% for Nd isotopes, ?15 ～ 7% for Eu isotopes, ?13 ～ 1% for Cs isotopes, ?13 ～ 8% for Sm isotopes, 0 ～ 7% for ¹⁴⁷Pm, ?7 ～ ?2% for ⁹⁵Mo, ?2 ～ ?1% for¹⁰¹Ru and 0 ～ 4% for ¹⁰³Rh.     

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.     

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.     

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.     

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.     

Feedback on neutron capture cross sections of 238Pu and 241Am from analyses of measured isotopic compositions of irradiated LWR fuels and MOX core physics experiments

The atomic fractions of ²³⁸Pu and ²⁴¹Am in MOX fuels recycled in light water reactors are 1% to 2% and not significant compared with those of major Pu isotopes. On the other hand, recent evaluated nuclear data libraries, such as JENDL-4.0 and JEFF-3.2, give noticeably different thermal and epithermal neutron capture cross sections for ²³⁸Pu and ²⁴¹Am. The thermal neutron capture cross sections of ²³⁸Pu and ²⁴¹Am in JEFF-3.2 are 31% and 9% larger than those of JENDL-4.0, respectively. This paper shows the effect of the differences in the neutron cross sections on analysis results of two different integral experiments. The first is the isotopic compositions of ²³⁸Pu on UO₂ and MOX fuels irradiated in BWR and PWR, and the second is the critical experiments of the water moderated cores fully loaded with MOX fuels. The former was analyzed by using the continuous energy Monte Carlo burnup calculation code MVP-BURN and the latter by the continuous energy Monte Carlo calculation code MVP. The comparisons between the calculated and measured results indicate that the most likely thermal and epithermal neutron capture cross sections of ²³⁸Pu and ²⁴¹Am should be around at the middle between those of JEFF-3.2 and JENDL-4.0.     

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.     

Nuclear Design Study on a Super High-burnup Fuel Assembly for Pressurized Water Reactors Using Transuranium

A conceptual design study was carried out on a super high-burnup mixed-oxide (MOX) fuel assembly (SHB FA) for pressurized water reactors (PWRs) using transuranium (TRU). This study aims to avoid the surplus plutonium (Pu) accumulation and to reduce the accumulation of long-lived radioactive minor actinides (MAS) by utilizing the currently existing PWRs under the condition that the Japanese program to develop fast breeder reactors (FBRs) is tend to delay. For this purpose, an SHB FA with discharged burnup of ?80 GWd/t was investigated by utilizing MAS positively as both burnable absorbers and fissile suppliers and loading high-content Pu. It is possible to load the SHB FAs in a current PWR together with UO₂ FAs and to use 2.5 times as much amount of Pu as that in a standard 1/3 MOX core. Moreover, it is found to be possible to reduce the total number of fresh FAs further from that of a high-burnup (55 GWd/t in maximum) UO₂ (4.9 wt%) core and also to reduce the accumulation of MAS in the nuclear fuel cycle significantly.     

Benchmark Problem Suite for Reactor Physics Study of LWR Next Generation Fuels

This paper proposes a benchmark problem suite for studying the physics of next-generation fuels of light water reactors. The target discharge burnup of the next-generation fuel was set to 70GWd/t considering the increasing trend in discharge burnup of light water reactor fuels. The UO₂ and MOX fuels are included in the benchmark specifications. The benchmark problem consists of three different geometries: fuel pin cell, PWR fuel assembly and BWR fuel assembly. In the pin cell problem, detailed nuclear characteristics such as burnup dependence of nuclide-wise reactivity were included in the required calculation results to facilitate the study of reactor physics. In the assembly benchmark problems, important parameters for in-core fuel management such as local peaking factors and reactivity coefficients were included in the required results. The benchmark problems provide comprehensive test problems for next-generation light water reactor fuels with extended high burnup. Furthermore, since the pin cell, the PWR assembly and the BWR assembly problems are independent, analyses of the entire benchmark suite is not necessary: e.g., the set of pin cell and PWR fuel assembly problems will be suitable for those in charge of PWR in-core fuel management, and the set of pin cell and BWR fuel assembly problems for those in charge of BWR in-core fuel management.     

Trend in criticality calculation results of borated-water-moderation experimental cores relating to 10B(n, α) cross section

ABSTRACT

In connection with the accuracy of the ¹⁰B(n, α) cross section in the thermal- and epithermal-neutron energy regions, criticality calculation results were examined for six benchmark sets of light-water-moderation critical experiments of UO₂ and MOX fuel lattice cores with un-borated and borated water. Two of the benchmark sets were those implemented in the Tank-Type Critical Assembly (TCA). The others were taken from the International Handbook of Evaluated Criticality Safety Benchmark Experiments (ICSBEP), and the International Handbook of Evaluated Reactor Physics Benchmark Experiments (IRPhEP). The enrichments of the UO₂ fuel range from 1.9 wt% to 2.6 wt%, and the Pu contents of the MOX fuel do from 2.0 to 6.6 wt%. The boron concentrations in water are up to 1511 ppm. The effective neutron multiplication factors (k_eff ) were taken from the published documents. They were calculated with continuous-energy Monte Carlo calculation codes in combination with JENDL-4.0, and other evaluated nuclear data libraries. It was confirmed that the k_eff values of the critical cores increased with the boron concentrations, which indicates that the ¹⁰B(n, α) cross section in the thermal- and epithermal-neutron energy regions should be larger than those in JENDL-4.0 and other libraries.     

Analysis of Core Physics Experiments on Fresh and Irradiated PWR UO2 Fuels in the REBUS Program

Critical experiments of two cores each loaded with fresh 5 × 5 test PWR-type fuel rods of ²³⁵U enrichment of 3.8 wt% or irradiated 5 × 5 test rods of rod average burnup of 55 GWd/t in the REBUS program were analyzed using diffusion, transport, and continuous-energy Monte Carlo calculation codes coupled with nuclear data libraries based on JENDL-3.2 and JENDL-3.3. Biases in effective multiplication factors k _eff's of the critical cores were about ?1:2%Δk for the diffusion calculations (JENDL-3.2), ?0:5%Δk for the transport calculations (JENDL-3.3), and ?0:5 and 0.1%Δk for the Monte Carlo calculations (JENDL-3.3 and JENDL-3.2, respectively). The measured core fission rate and Sc- or Co-activation rate distributions were generally well reproduced using the three types of calculation. The burnup reactivity determined using the measured water level reactivity coefficients was ?2:35 ± 0:07Δk/kk′. The calculated result of the Monte Carlo calculations agreed with it; however, the diffusion and transport calculations overestimated the absolute value by about 7%, which would be mainly attributed to the errors in the calculation of the reactivity caused by changing the fuel compositions from fresh fuel to irradiated fuel.     

Estimation of Spent Fuel Compositions from Light Water Reactors

The compositions and quantities of minor actinide (MA) and fission product (FP) in spent fuels will be diversified with the use of high discharged burnup fuels and MOX fuels in LWRs which will be a main part of power reactors in future.

In order to investigate above diversities, we have studied on the calculation method to be used in the estimation of spent fuel compositions and adopted the real irradiation calculation in which axial burnup and moderator distribution are considered in the burnup calculation.

On the basis of the calculations, compositions and burnup quantities of various LWR spent fuels (reactor type: PWR and BWR, discharged burnup: 33, 45 and 60 GWd/tHM, fuel type: U0₂ and MOX) are apparently estimated among various forms of fuels. As an example, it is shown that there are considerable discrepancy in MA burnup between PWR and BWR spent fuels.     

MOX Fuel Performance Experiment Specified for Japanese PWR Utilisation in the HBWR

In order to obtain high burn-up MOX fuel irradiation performance data, SBR and MIMAS MOX fuel rods with Pufissile enrichment of about 6 wt% have been irradiated in the HBWR. In-pile performance data of MOX have been obtained, and the peak burn-up of MOX pellet have reached to 66 GWd/tM as of October 2004. MOX fuel temperature is confirmed to have no significant difference compared to UO₂, if taking into account adequately for thermal conductivity degradation due to PuO₂ addition and burn-up development, and measured fuel temperature agrees well with HB-FINE code calculation up to high burn-up region. Fission gas release of MOX is possibly larger than UO₂ based on temperature and pressure assessment. No significant difference is confirmed between SBR and MIMAS MOX on FGR behaviour. MOX fuel swelling rate agrees well with solid swelling rate. Cladding elongation data shows onset of PCMI in high power region. Ramp test data from other experiment programs with various types of MOX fabrication route confirms superior PCI resistance of MOX compared to UO₂, due to enhanced creep rate of MOX. The irradiation is expected to continue until achieving of 70 GWd/tM (MOX pellet peak).     

Determination of fissile fraction in MOX (mixed U + Pu oxides) fuels for different burnup values

When spent Light Water Reactor fuels are processed by the standard Purex method of reprocessing, plutonium (Pu) and uranium (U) in spent fuel are obtained as pure and separate streams. The recovered Pu has a fissile content (consisting of ²³⁹Pu and ²⁴¹Pu) greater than 60% typically (although it mainly depends on discharge burnup of spent fuel). The recovered Pu can be recycled as mixed-oxide (MOX) fuel after being blended with a fertile U makeup in a MOX fabrication plant. The burnup that can be obtained from MOX fuel depends on: (1) isotopic composition of Pu, which is closely related to the discharge burnup of spent fuel from which Pu is recovered; (2) the type of fertile U makeup material used (depleted U, natural U, or recovered U); and (3) fraction of makeup material in the mix (blending ratio), which in turn determines the total fissile fraction of MOX. Using the Non-linear Reactivity Model and the code MONTEBURNS, a step-by-step procedure for computing the total fissile content of MOX is introduced. As was intended, the resulting expression is simple enough for quick/hand calculations of total fissile content of MOX required to reach a desired burnup for a given discharge burnup of spent fuel and for a specified fertile U makeup. In any case, due to non-fissile (parasitic) content of recovered Pu, a greater fissile fraction in MOX than that in fresh U is required to obtain the same burnup as can be obtained by the fresh U fuel.     

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.