Rapid aqueous release of fission products from high burn-up LWR fuel: Experimental results and correlations with fission gas release

Studies of the rapid aqueous release of fission products from UO₂ and MOX fuel are of interest for the assessment of the safety of geological disposal of spent fuel, because of the associated potential contribution to dose in radiological safety assessment. Studies have shown that correlations between fission gas release (FGR) and the fraction rapidly leached of various long-lived fission products can provide a useful method to obtain some of this information. Previously, these studies have been limited largely to fuel with burn-up values below 50 MWd/kg U. Collaborative studies involving SKB, Studsvik, Nagra and PSI have provided new data on short-term release of ¹³⁷Cs and ¹²⁹I for a number of fuels irradiated to burn-ups of 50–75 MWd/kgU. In addition a method for analysis of leaching solutions for ⁷⁹Se was developed. The results of the studies show that the fractional release of ¹³⁷Cs is usually much lower than the FGR covering the entire range of burn-ups studied. Fractional ¹²⁹I releases are somewhat larger, but only in cases in which the fuel was forcibly extracted from the cladding. Despite the expected high degree of segregation of fission gas (and by association ¹³⁷Cs and ¹²⁹I) in the high burn-up rim, no evidence was found for a significant contribution to release from the rim region. The method for ⁷⁹Se analysis developed did not permit its detection. Nonetheless, based on the detection limit, the results suggest that ⁷⁹Se is not preferentially leached from spent fuel.     

On the rate determining step in fission gas release from high burn-up water reactor fuel during power transients

The radial distribution of grain boundary gas in a PWR and a BWR fuel is reported. The measurements were made using a new approach involving X-ray fluorescence analysis and electron probe microanalysis. In both fuels the concentration of grain boundary gas was much higher than hitherto suspected. The gas was mainly contained in the bubble/pore structure. The factors that determined the fraction of gas released from the grains and the level of gas retention on the grain boundaries are identified and discussed. The variables involved are the local fuel stoichiometry, the amount of open porosity, the magnitude of the local compressive hydrostatic stress and the interaction of metallic precipitates with gas bubbles on the grain faces. It is concluded that under transient conditions the interlinkage of gas bubbles on the grain faces and the subsequent formation of grain edge tunnels is the rate determining step for gas release; at least when high burn-up fuel is involved.     

Modeling of fission gas swelling in LWR UO2 fuel under irradiation

An understanding of the behavior of fission gas in uranium dioxide (UO₂) fuel is necessary for the prediction of the performance of fuel rods under irradiation. A mechanistic model for matrix swelling by the fission gas in LWR UO₂ fuel is presented. The model takes into account intragranular and intergranular fission gas bubbles behavior as a function of irradiation time, temperature, fission rate and burn-up. The intragranular bubbles are assumed to be nucleated along the track of fission fragments, which play the dual role of creator and destroyer of intragranular bubbles. The intergranular bubble nuclei is produced until such time that a gas atom is more likely to be captured by an existing nucleus than to meet another gas atom and form a new nucleus. The capability of this model was validated by a comparison with the measured data of fission gas behavior such as intragranular bubble size, bubble density and total fuel swelling. It was found that the calculated intragranular bubble size and density are in reasonable agreement with the measured results in a broad range of average fuel burn-ups 6–83 GW d/tU. Especially, the model correctly predicts the fuel swelling up to a burn-up of about 70 GW d/tU.     

Comments on the threshold porosity for fission gas release in high burn-up fuels

This letter challenges two recent papers in this journal, suggesting that the high burn-up structure of LWR-fuels would evolve towards an open pore system, facilitating gas release. In contrast, recent experimental results and supporting calculations reviewed here as well as new evidence from a 3D pore-reconstruction strongly suggest that the materials in question would show closed porosity conditions and hence reduced probability of gas release, at least up to porosity fractions of about 25%. This value is most likely conservative.     

Change of fuel-to-cladding gap width with the burn-up in FBR MOX fuel irradiated to high burn-up

In order to study the dependence of the gap width change on the burn-up, the fuel-to-cladding gap widths were investigated by ceramography in a large number of FBR MOX fuel pins irradiated to high burn-up. The dependence of gap widths on the burn-up was closely connected with the formations of JOG (joint oxyde-gaine) and rim structure. The gap widths decreased gradually due to the fuel swelling until ∼30 GWd/t, but beyond this burn-up the dependence showed two different tendencies. With the increase of burn-up, the gap widths decreased due to the increase of fuel swelling in the low fuel temperature region where the rim structure was observed, but they increased in the high fuel temperature region where the JOG rich in Cs and Mo formed in the gap.     

大晶粒UO2燃料芯块堆内试验组件的研制

为了开发高性能的压水堆燃料,研制了大晶粒燃料芯块。试验燃料芯块具有高的235U富集度、小直径和大晶粒尺寸的特点。通过堆内辐照试验可以对不同制造工艺的燃料芯块进行评价和筛选,以便确定燃料制造工艺。为了在中国原子能科学研究院池式研究堆中随堆考验,设计了一种试验组件,包含四根双包壳的燃料棒。双包壳燃料棒是在外包壳内装入两根单包壳燃料棒。试验组件直接由反应堆一次循环水冷却,不设专门的冷却回路。试验组件上安装了多种堆芯测量传感器,包括燃料中心温度热电偶、自给能中子探测器和冷却剂出、入口温度热电偶,可以在线监测燃料试验参数。描述了大晶粒UO2燃料芯块的研制、试验燃料组件的研制和检验。     

The spacing of intergranular fission gas bubbles in irradiated UO2

A simple diffusion model is used to demonstrate that irregularly spaced intergranular fission gas bubbles tend to migrate towards regions of unoccupied grain boundary. In consequence it is concluded that coalescence of these bubbles by random migration is unimportant and that, in modelling gas release and swelling, the grain face bubbles may be assumed to remain descrete until they can no longer be accommodated without overlapping.     

A mass spectrometry method for quantitative and kinetic analysis of gas release from nuclear materials and its application to helium desorption from UO2 and fission gas release from irradiated fuel

A new system has been developed to determine absolute quantities of gas (mainly noble gases) released during thermal desorption in the range from 10^?12 to 10^?5 mol with a precision of few percent. The system is actually designed for simultaneous measurement of gaseous elements like He, Xe, Kr, thermally released from nuclear fuel samples and also allows the determination of the release kinetics as a function of time. This system, called Quantitative GAs MEasurement System (Q-GAMES), is based on the principle of collecting, purifying and spiking the sample gas in a “high-pressure” chamber, and continuous sampling of the gas for mass spectrometric analysis without sample depletion during the experiment. It is equipped with its own spike generator and with different gas purification systems. It is shown that this system fulfills the requirement to work with two existing very high-temperature gas desorption facilities for nuclear materials. This paper describes the Q-GAMES principle, the spiking system, its calibration, its operative mode, the different quantification techniques, as well as its technical data, in combination with some examples of typical application.     

Time dependent burn-up and fission products inventory calculations in the discharged fuel of the Syrian MNSR

The Syrian Miniature Neutron Source Reactor (MNSR), a 30 kW, 89.8% HEU fueled (U-Al), went critical in March, 1996. By operating the reactor at nominal power for 2.5 h/day, the estimated core life is 10 years. This paper presents the results of fuel burn-up and depletion analysis of the MNSR fuel lattice using the ORIGEN 2 code. A one-group cross-section data base for the ORIGEN 2 computer code was developed for the Syrian MNSR research reactor. The ORIGEN 2 predicted burn-up dependent actinide compositions of MNSR spent fuel using the newly developed data base show a good agreement with the published results in the literature. In addition, the burn-up characteristics of MNSR spent fuel was analyzed with the new data base. Finally, to study the effect of burn-up on the reactivity, the microscopic cross-sections of the fission products calculated by the WlMS code (using the number densities of fission products generated by the ORIGEN 2 code as a function of burn-up time), were used as an input for the CITATION code calculations. The results contained in this paper could be used in performing criticality safety analysis and shielding calculations for the design of a spent fuel storage cask for the MNSR core.     

Corrosion of high burn-up structured UO2 fuel in presence of dissolved H2

The influence of high burn-up structured material on UO₂ corrosion has been studied in an autoclave experiment. The experiment was conducted on spent fuel fragments with an average burn-up of 67 GWd/tHM. They were corroded in a simplified groundwater containing 33 mM dissolved H₂ for 502 days. All redox sensitive elements were reduced. The reduction continued until a steady-state concentration was reached in the leachate for U at 1.5 × 10⁻¹⁰ M and for Pu at 7 × 10⁻¹¹ M. The instant release of Cs during the first 7 days was determined to 3.4% of the total inventory. However, the Cs release stopped after release of 3.5%. It was shown that the high burn-up structure did not enhance fuel corrosion.     

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.     

Behaviour of fission gas products in single crystal UO2 during intermediate temperature irradiation

A new mathematical interpretation is presented of fission gas release from monocrystalline uranium dioxide fuel during intermediate temperature irradiation in terms of a defect trap model, knock-out process and diffusion of bubbles. In the present model it is assumed that gas in an intermediate state exists side by side with the dissolved fission gas and that trapped in bubbles. It is assumed also that the isolated gas atoms, being re-dissolved, are immobile.The present model gives a satisfactory interpretation of the relative proportions of isotopes in the steady state fission gas release at diffrent temperatures. The dependence of fractional fission gas release on fission rate is also interpreted; regimes either proportional to fission rate or inversely proportional to fission rate are predicted depending on the fission rate interval considered. Both temperature dependent and temperature independent fission gas release can arise.The presented dynamic method of studying the release of fission gases during irradiadion provides a further test beside the static method of the veracity of the assumed mechanisms. Calculations show that fission gas behaviour becomes more complex for oscillated fission rate in the regime where the fractional release is inversely proportional to the fission rate for the steady state.     

Modelling intragranular fission gas release in irradiation of sintered LWR UO2 fuel

A model for the release of stable fission gases by diffusion from sintered LWR UO₂ fuel grains is presented. The model takes into account intragranular gas bubble behaviour as a function of grain radius. The bubbles are assumed to be immobile and the gas migrates to grain boundaries by diffusion of single gas atoms. The intragranular bubble population in the model at low burn-ups or temperatures consists of numerous small bubbles. The presence of the bubbles attenuates the effective gas atom diffusion coefficient. Rapid coarsening of the bubble population in increased burn-up at elevated temperatures weakens significantly the attenuation of the effective diffusion coefficient. The solution method introduced in earlier papers, locally accurate method, is enhanced to allow accurate calculation of the intragranular gas behaviour in time varying conditions without excessive computing time. Qualitatively the detailed model can predict the gas retention in the grain better than a more simple model.     

Experimental study on the effect of fission product gas release into blockage wake region using a simulated LMFBR fuel subassembly

The objective of this study is to evaluate temperature rise due to gas release in the wake region of LMFBR fuel subassemblies. The experiments were conducted in two sets of grid-spacer-type 37-pin bundles simulating LMFBR fuel subassemblies. In Test section 37GC, the central 24 subchannels were blocked by a stainless steel plate and in Test section 37GE one-half edge part (39 subchannels) of the total flow area was blocked by the same material. The experimental results were compared with data obtained in similar tests using a spacer wire-type pin bundle, designated 37WC. The temperature rises in 37GE and 37WC were nearly identical in value and effect of gas release rate. The marked agreement seems to imply that there is a limit in the content of released gas in the wake region. On the other hand, the temperature rise behind the central blockage in the grid-type bundle, where gas might easily flow out to the core flow region, was far less than in the other geometries.     

Using the MCU computer program to analyze the results of critical experiments with HTGR fuel pellets on the Astra testing stand

The Astra testing stand and the critical assemblies simulating on this stand the special physical features of HTGRs are described. The experimental data, obtained using the Astra stand, on the critical parameters of assemblies with HTGR fuel pellets and an analysis of the data using the MCU computer program, which employs the Monte Carlo method, are presented taking account of the requirements of the international program on critical benchmark experiments. It is shown that the experimental data are in good agreement with the computational results.Translated from Atomnaya Ènergiya, Vol. 97, No. 4, pp. 243–252, October, 2004.