Effect of Pu-rich agglomerates in MOX fuel on reactivity analysis of light water reactor MOX core physics experiments

The effect of Pu-rich agglomerates in U-Pu mixed oxide (MOX) on the reactivity analysis of light water reactor MOX core physics experiments was studied with the continuous-energy Monte Carlo calculation code MVP II. First, the following three different models were compared in the analysis of a representative unit cell of a MOX core tested at the KRITZ reactor: a Lattice model where Pu-rich agglomerates were assumed to exist in a fixed pitch, a statistical geometry (STG) model of MVP II, and a Random model where the random distribution of Pu-rich agglomerates was directly modeled. Since the three models gave comparable results, the STG model was used in parametric calculations to systematically understand the reactivity effect depending on the characteristics of Pu-rich agglomerates. In addition, the selected unit cells composing the MOX cores and one representing MOX core tested at the EOLE criticality facility were analyzed with the measured characteristics of Pu-rich agglomerates in MOX fuel. Consequently, the reactivity differences between the calculations assuming the homogeneous Pu distributions and those considering Pu-rich agglomerates were less than 0.0005 Δk/k/k', indicating that the effect of Pu-rich agglomerates was small on the reactivity analysis of the MOX cores tested in the EOLE facility.     

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.     

Study on double heterogeneity effect of Pu-rich agglomerates in mixed oxide fuel using cross section homogenization method for particle-dispersed media

A cross section homogenization method for media containing randomly and uniformly dispersed particles, which was originally developed by Shmakov et al., has been applied to MOX fuels containing Pu-rich agglomerates. This method (Shmakov’s method), which is incorporated into a continuous-energy Monte Carlo code MCNP, has been applied to lattice calculations of an infinite MOX fuel rod array. Shmakov’s method can accurately reproduce the criticality calculation results for an explicit heterogeneous arrangement of Pu-rich agglomerates. A correction factor that Shmakov’s method defines to obtain an effective microscopic cross section provides a proper quantitative indication of the double heterogeneity of MOX fuels containing Pu-rich agglomerates. The correction factors exhibit an obvious double heterogeneity effect of Pu-rich agglomerates dispersed in MOX fuel pellets. The effective microscopic cross sections of plutonium isotopes in MOX fuels containing Pu-rich agglomerates are significantly reduced due to the self-shielding effect as compared to the homogeneous MOX fuel model. However, the double heterogeneity effect of Pu-rich agglomerates on k_eff seems to be unexpectedly minor because the underestimate of the reaction rates in the resonance energy range is offset by the overestimate of the reaction rates in the thermal energy range.     

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 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.     

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.     

超临界水冷堆MOX燃料特性分析

针对超临界水冷堆组件,采用不同Pu含量的MOX燃料进行组件计算,得到不同燃料条件下的燃耗深度、功率分布因子、慢化剂温度反应性系数等结果,并对比分析在超临界水冷堆中应用MOX燃料与应用UO2燃料对组件性能的影响,以及不同Pu含量MOX燃料间的性能区别。分析结果表明,在超临界水冷堆设计中,应用MOX燃料与应用UO2燃料有相似的功率分布,应用MOX燃料可以增加燃耗深度,并有良好的慢化剂温度反应性系数。经过合理设计的MOX燃料可较好应用于超临界水冷堆中,且产生更好的性能。     

A methodology to predict a fission gas release ratio of MOX fuel with heterogeneous microstructure

The objective of this study is to formulate a methodology to predict a fission gas release ratio of MIMAS MOX. An irradiated MIMAS MOX fuel with plutonium rich agglomerates was subjected to elemental analyses by electron probe micro analysis and secondary ion mass spectrometry in order to investigate xenon distribution. The results of the elemental analyses showed that the plutonium rich agglomerates at the periphery of the fuel pellet sample retained a high concentration of xenon as gas bubbles. Then, the results were used as reference data for modification of models in a fuel rod analysis code, FEMAXI-7. Using the modified FEMAXI-7, we applied an approach to prediction of fission gas release ratio of MOX fuel with plutonium rich agglomerates. In the approach, two separated analyses using FEMAXI-7 were performed for the plutonium rich agglomerates and the matrix. Fission gas release ratios obtained from the two analyses were processed through weighted-average with burnup ratios of the plutonium rich agglomerates and the matrix. Finally, the fission gas release ratios were compared with results of rod puncture tests. As a result of the comparison, it was confirmed that the proposed approach could well predict fission gas release ratio of MOX fuel with plutonium rich agglomerates.     

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.     

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.     

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.     

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.     

Helios, current coupling collision probability method, applied for solving the NEA C5G7 MOX benchmark

As part of an effort to test the ability of current transport codes to treat reactor core problems without spatial homogenization, the lattice code HELIOS was employed to perform criticality calculations. The test consists in seven-group calculations of the C5 MOX fuel assembly problem specified by Cavarec et. al. [1]. This problem, known as C5G7 MOX Benchmark, is described in the Benchmark Specification [2] and comprises two cases — two and three-dimensional geometry. There are four fuel assemblies — two with MOX fuel, the other two with UO₂ fuel. Each fuel assembly is made up of a 17×17 lattice of square fuel-pin cells. Fuel pin compositions are specified in the Benchmark Specification, which also provides seven-group transport-corrected isotropic scattering cross-sections for U0₂, the three MOX enrichments, the guide tubes, the fission chamber and the moderator. This paper preset is the methodology employed in solving the C5G7 MOX Fuel Assembly Problem using the transport code HELIOS.     

U－Pu混合氧化物燃料发展状况

文章综述了Ｕ－Ｐｕ混合氧化物（ＭＯＸ）燃料的生产和应用情况，评述了ＭＯＸ燃料制造和后处理工艺过程等有关问题。就我国研制ＭＯＸ燃料问题提出几点看法。     

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.     

百万千瓦级环形MOX燃料堆芯设计

对环形UO2燃料及环形MOX燃料组件参数的计算方法进行了研究。设计了包含193盒环形UO2和MOX燃料组件的混合型长周期(18个月)堆芯方案。对设计的堆芯的重要物理参数进行了分析,并对各循环进行了燃耗计算。结果表明,装载约30%MOX组件的堆芯可在百万千瓦功率下实现长周期换料。堆芯从初装载可安全过渡到平衡循环,各循环的重要物理参数均满足设计要求,说明设计的堆芯及燃料管理方案是安全可行的。     

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.     

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.     

Estimation of the Grain Boundary Gas Inventory in MIMAS/AUC MOX Fuel and Consistency with REP-Na Test Results

In the frame of its research activities on fuel safety, the French “Institut de Radioprotection et de Sûreté Nucléaire” performed the REP-Na program in the CABRI reactor devoted to the study of Reactivity Initiated Accidents. Focused on high burn-up UO2 and MOX fuel behaviour, twelve tests (8 UO2 and 4 MOX) were realized from 1993 to 2000. In all these tests, the influence of grain boundary gas was evidenced and it appeared necessary to perform some estimation of its inventory in irradiated fuel. Such evaluations are presented for the MOX MIMAS/AUC fuel, based on two different approaches: “experimental” and “theoretical.” The fission gas amount located at the grain boundaries increases with burn-up in correlation with the production, but also with the initial Pu enrichment, as soon as the agglomerates have reached the full restructuring threshold for the High Burn-up Structure. The consistency with the REP-Na test results is checked, showing that a significant cladding deformation is needed, clearly higher than for UO2 fuel in order to release all the grain boundary gas in RIA. Furthermore, to the fission gas effect, adds the helium's occluded in the irradiated fuel whose amount increases with burn-up, Pu enrichment and ²⁴¹Pu and ²⁴¹Am initial content.     

球床式高温气冷堆MOX燃料循环优化

与压水堆相比,球床式高温气冷堆能在堆芯结构不做明显改变的情况下采用全堆芯装载混合氧化物（MOX）燃料元件。基于250 MW球床模块式高温气冷堆堆芯结构,设计了4种球床式高温气冷堆下MOX燃料循环方式,包括铀钚混合的燃料球和独立的钚球与铀球混合装载的等效方式,采用高温气冷堆设计程序VSOP进行分析,比较了初装堆的有效增殖因数、燃料元件在堆芯内滞留时间、卸料燃耗、温度系数等主要物理特性。结果表明：采用纯铀和纯钚两种分离燃料球且铀燃料球循环时间更长的方案,平均卸料燃耗较高,总体性能较其他循环方式优越。