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.     

Modeling and parametric studies of the effect of inhomogeneity on fission gas release in LWR MOX fuel

To analyze the effect of an inhomogeneous mixture of an PuO₂ powder on fission gas release in MOX fuel, a model has been developed using the assumption that gas release mechanism in Pu-rich particles is identical with that in UO₂ fuel. A parametric study was performed to see the respective effect of the number density, size and fraction of Pu retained in the Pu-rich particles on gas release in MOX fuel. The model shows that, for the condition of all the other remaining parameters being fixed, more gas is released in a MOX fuel for lower number density of, smaller size of, and larger fraction of Pu retained in, the Pu-rich particles. However, there exists some condition or combination of parameters for which the effect of inhomogeneity on gas release is negligible depending on the characteristics of MOX fuel. Comparison with measured data for OCOM MOX fuel shows that the present model can predict the level of gas release in MOX fuel once the release mechanism in the Pu-rich particles is known.     

Application of fluoride volatility method to the spent fuel reprocessing

ABSTRACT

An advanced reprocessing system has been developed to treat various SF (spent fuels): spent UO₂ and MOX (mixed oxide) fuels from LWR (light water reactor) and MOX fuel from FR (fast reactor). The system consists of SF fluorination to separate most U (uranium) as volatile UF₆, dissolution of solid residue containing Pu (plutonium), FP (fission products), MA (minor actinides) and partial U by nitric acid, and Pu+U separation from FP and MA by conventional solvent extraction. Gaseous UF₆ is purified by the thermal decomposition and the adsorption of volatile PuF₆ and adsorption of other impurities. This system is a hybrid process of fluoride volatility and solvent extraction and called FLUOREX. Fluorination of most U in the early stage of the reprocessing process is aimed at sharply reducing the amount of SF to be treated in the downstream aqueous steps and directly providing purified UF₆ for the enrichment process without conversion. The FLUOREX can flexibly adjust the Pu/U ratio, rapidly separate UF₆ and economically treat aqueous Pu+U. These features are especially suitable for the transition period fuel cycle from LWR to FR. This paper summarizes the feasibility confirmation results of FLUOREX.     

Non destructive determination of PuO2 content in MOX fuel pins for fast reactors using Passive Gamma Scanning

Use of Passive Gamma Scanning for non destructive evaluation of PuO₂ content in mixed oxide (MOX) fuels for fast reactors is demonstrated. Experiments have been carried out on MOX fuel pins for the hybrid core of Fast Breeder Test Reactor having nominal PuO₂ content of 44% and MOX pins having nominal PuO₂ content of 21% for the Prototype Fast Breeder Reactor. A comparison of results obtained using a conventional NaI(Tl) detector and that using a through well shaped detector is also presented.     

Analysis of VIP-BWR reactor core physics experiments on UO2 and MOX mockup fuel assemblies - part 2: analysis with SIMULATE5

Analysis of the three test cores in the VIP-BWR program was performed in a two-dimensional geometrical model with CASMO5 coupled with the JENDL-4.0-based neutron data library, and reported in the previous paper. Following the study, interpretation of the experiments were carried out in a three-dimensional geometrical model with SIMULATE5 for the code validation study. The nuclear libraries for the SIMULATE5 calculations were generated with CASMO5 with the JENDL-4.0-based neutron data library. The effective multiplication factors of the critical cores ranged from 0.9983 to 1.0023 with measurement uncertainties of 0.0003 to 0.0004 (one σ). The root mean squares of (the calculated/the measured-1) for the fission rates at the core-mid plain of all the measured fuel rods were about 3% for the three cores. It was noticed that the calculations underestimated the fission rates of the UO₂ fuel rods and overestimated those of the MOX fuel rods for the test cores loaded with MOX fuel rods, which was consistent with trends in the preceding analysis studies of the VIP-BWR program and other MOX core experiments, and the biases were confirmed in the calculation results of power distributions in MOX-fueled light water reactor cores.     

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.     

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.     

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).     

Analysis of fuel temperature effects on reactivity of light water reactor fuel assemblies by using MVP-2 adopting an exact resonance elastic scattering model

Using the continuous-energy Monte Carlo code MVP-2 adopting a resonance elastic scattering model considering the thermal motion of a target nucleus (the exact model) for major heavy nuclides, analysis of fuel temperature effects on reactivity of mockup UO₂ and MOX fuel assemblies for light water reactors was performed, and the results were compared with those of the conventional asymptotic model. A base condition was a hot operating condition with an in-channel void fraction of 40% and fuel temperature of 520 ℃ for the BWR fuel assemblies and a hot zero-power condition with fuel temperature of 284 ℃ for the PWR fuel assemblies. The fuel temperature of a high-temperature condition was 1500 ℃ for both types of assemblies. The calculated results showed that the exact model made the neutron multiplication factors at the high-temperature condition lower by ?220 to ?440 pcm (10^?5 Δk) and the Doppler reactivity between the base- and high-temperature conditions more negative by 7% to 10% compared with those obtained by the asymptotic model. The energy-dependent reaction rates of capture and ν-fission were also analyzed to study the detail mechanism in the effect of the exact model on the assembly reactivity.     

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 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.     

Removal of Liquid and Solid Impurities from Uranyl Nitrate Hexahydrate Crystalline Particles in Crystal Purification Process

The purification behavior of uranyl nitrate hexahydrate (UNH) was investigated to evaluate the decontamination performance of liquid and solid impurities using a dissolver solution of mixed oxide (MOX) fuel in batch experiments. The UNH crystal recovered from the MOX fuel dissolver solution containing simulated fission products (FPs) was purified by a sweating and melt filtration process. Although the decontamination factors (DFs) of Pu, Cs, and Ba did not change in the sweating process, that of Eu increased with increases in temperature and time. These results indicate that liquid impurities such as Eu were effectively removed by the sweating method, but solid impurities such as Pu, Cs, and Ba were minimally affected in the batch experiments. On the other hand, the DF of Ba increased with 0.45 and 5.0 μ filters in the melt filtration process. Since Pu and Cs formed as Cs₂Pu(NO₃)₆ in the course of U crystallization and was accompanied with the UNH crystal, these behaviors were similar to each other. Although the DFs of Pu and Cs did not change with the 5.0 μ filter, it increased approximately twofold with the 0.45 μ filter. The particle size of Cs₂Pu(NO₃)₆ is relatively small and might pass through the 5.0 μ filter in the melt filtration process. The liquid impurities as Eu remained in the molten UNH crystal with some filters.     

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.     

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.     

Transport Calculations of MOX and UO2 Pin Cells by the Method of Characteristics

A new transport theory code for two-dimensional calculations of both square and hexagonal fuel lattices by the method of characteristics has been developed. The ray tracing procedure is based on the macroband method, which permits more accurate spatial integration in comparison to the equidistant method of tracing. The neutron source within each region is approximated by a linear function and linearly anisotropic scattering can be optionally accounted for. Efficient new techniques for both azimuthal and polar integration are presented. The spatial discretization problem in case of P ₁-scattering has been studied. Detailed analyses show that the P ¹-scattering in case of regular infinite array of fuel cells is significant, especially for MOX fuel, while the transport correction is inadequate in case of real geometry multi-group calculations. Finally, the complicated nature of the angular flux in MOX and UO₂ fuel cells is demonstrated.     

Analysis of the MOX critical experiments BASALA by pin-by-pin core analysis method using three-dimensional direct response matrix

An analysis of the MOX critical experiments BASALA was performed to verify the pin-by-pin core analysis method using a three-dimensional direct response matrix. The BASALA experiments simulate full MOX BWR cores, and they were carried out in the EOLE critical facility of the French Atomic Energy Commission (CEA) by the Nuclear Power Engineering Corporation (NUPEC) in collaboration with CEA. The BASALA experimental cores are very heterogeneous because their size is much smaller than that of commercial power plants. The main features of the pin-by-pin core analysis method using the three-dimensional direct response matrix are that the response matrix can reflect the intra-assembly heterogeneous effect, the diffusion approximation is not involved, and the fuel rod fission rate can be directly evaluated. The maximum difference of the critical k-effective values among all nine cores analyzed was about 0.4% Δk. The root mean square differences between the calculated and measured radial fuel rod fission rate distributions in the test assembly of all cores were within 1.8% and nearly comparable to measurement error. The calculated results of the reactivity worth agreed with the measured results within 9%. These good agreements mean that the pin-by-pin core analysis method using the three-dimensional direct response matrix accurately reflects the effects of the intra- and inter-assembly heterogeneities in heterogeneous systems like the BASALA experimental cores.     

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.     

Applicability of CeO2 as a surrogate for PuO2 in a MOX fuel development

The applicability of cerium oxide, as a surrogate for plutonium oxide, was evaluated for the fabrication process of a MOX (mixed oxide) fuel pellet. Sintering behavior, pore former effect and thermal properties of the Ce–MOX were compared with those of Pu–MOX. Compacting parameters of the Pu–MOX powder were optimized by a simulation using Ce–MOX powder. Sintering behavior of Ce–MOX was very similar to that of Pu–MOX, in particular for the oxidative sintering process. The sintered density of both pellets was decreased with the same slope with an increasing DA (dicarbon amide) content. Both the Ce–MOX and Pu–MOX pellets which were fabricated by an admixing of 0.05 wt% DA and sintering in a CO₂ atmosphere had the same average grain size of 11 μm and a density of 95%T.D. The thermal conductivity of the Pu–MOX was a little higher than that of the Ce–MOX at a lower temperature but both conductivities became closer to each other above 900 K. Cerium oxide was found to be a useful surrogate to simulate the Pu behavior in the MOX fuel fabrication.     

ACP1000中MOX燃料组件管理初步研究

使用SCIENCE程序包对MOX燃料组件进行了初步设计和研究。在此基础上,对采用部分MOX燃料组件的ACP1000堆芯开展燃料管理研究,得到由全堆装载UO₂燃料组件向部分MOX燃料组件堆芯过渡的燃料管理方案,并对MOX燃料组件和部分MOX燃料组件堆芯的安全参数及其他重要参数进行分析和比较。分析结果表明,各种安全参数均满足设计要求,证明在ACP1000堆芯应用MOX燃料是可行的,并为进一步研究提供了参考。     

Investigation and application of hollow anode glow discharge ion source

In the present work, a new shape of a glow discharge ion source has been designed, fabricated and constructed at Accelerators and Ion Sources Department, Nuclear Research Center, Egyptian Atomic Energy Authority, Egypt. The discharge and output beam characteristics of the ion source at different operating gas pressures have been measured at the optimum distance between the anode and the cathode (3.5 mm) using hydrogen and nitrogen gases. Furthermore, mixture of different gases was studied, e.g., addition of H₂ gas to N₂ gas with different ratios has been investigated. Finally, as an application of this new ion source, ion beam modification of insulators (glass) which depends on glass structure has been achieved. It has been found that, the transmission of light is decreased by coating the glass surface with Ar ion beam more than coating with plasma of Ar gas at the same pressure and the same exposure time. So we could use this ion source as a coating tool for borate glass surface. The parameters affected the glow discharge ion source efficiency have been examined carefully using a mixture of gases. Using helium gas, the glow discharge is in a turbulent state due to instabilities. An investigated H₂-N₂ mixture has been used in order to obtain an optimum percentage of the mixture of the two gases to increase the electric field necessary for ionization balance.