Spent fuel dissolution in Belgian Supercontainer conditions: source term and compatibility

2012 ◽  
Vol 1475 ◽  
Author(s):  
K. Lemmens ◽  
Th. Mennecart ◽  
C. Cachoir

ABSTRACTIn the frame of the Safety and Feasibility Case 1 development, the Belgian agency for radioactive waste (ONDRAF/NIRAS) has to demonstrate that the geological disposal of spent nuclear fuel in the Boom Clay host rock following the Supercontainer design provides sufficient radiological safety in the long term. This safety relies on the containment of the radionuclides by the overpack, the limitation of radionuclide release from the waste matrix, the diffusion controlled transport of the radionuclides, and their low solubility and sorption on the Boom Clay host rock. This paper presents an evaluation of the main processes considered for the limitation of radionuclide release by the Spent Fuel in Supercontainer conditions, characterized by the presence of a concrete buffer and hyperalkaline pore water. We present a description of the main expected processes with their potential impact on the fuel alteration mechanisms, and potential reference fuel matrix alteration rates and effective fuel surface areas for use in safety and performance assessment models.

2021 ◽  
Vol 11 (18) ◽  
pp. 8566
Author(s):  
Barbara Pastina ◽  
Jay A. LaVerne

For the long-term safety assessment of direct disposal of spent nuclear fuel in deep geologic repositories, knowledge on the radionuclide release rate from the UO2 matrix is essential. This work provides a conceptual model to explain the results of leaching experiments involving used nuclear fuel or simulant materials in confirmed reducing conditions. Key elements of this model are: direct effect of radiation from radiolytic species (including defects and excited states) in the solid and in the first water layers in contact with its surface; and excess H2 may be produced due to processes occurring at the surface of the spent fuel and in confined water volumes, which may also play a role in keeping the spent fuel surface in a reduced state. The implication is that the fractional radionuclide release rate used in most long-term safety assessments (10−7 year−1) is over estimated because it assumes that there is net UO2 oxidation caused by radiolysis, in contrast with the alternative conceptual model presented here. Furthermore, conventional water radiolysis models and radiation chemical yields published in the literature are not directly applicable to a heterogeneous system such as the spent fuel–water interface. Suggestions are provided for future work to develop more reliable models for the long-term safety assessment of spent nuclear fuel disposal.


Author(s):  
Xavier Sillen ◽  
Jan Marivoet ◽  
Wim Cool ◽  
Peter de Preter

The classical numerical output, or indicator, from assessments of the long-term safety of geological disposal systems for high-level radioactive waste is the individual effective dose rate. This indicator is an estimate of the possible individual health detriment and it is commonly compared to regulatory limits for assessing the safety of other nuclear activities as well, such as medical and industrial activities. As a safety indicator, the individual dose rate provides an estimate of the overall safety of the disposal system. However, because of the time frames involved in safety assessments of geological disposal systems, the need arises of complementary safety indicators that could be less affected by uncertainties like those associated with future human behaviour or the effects of climate change on the biosphere and the aquifers. Such alternative safety indicators can be, for example, radionuclide concentrations in the groundwater or fluxes to the biosphere due to a repository. Safety indicators only tell how globally safe a disposal system is. For confidence building, performance indicators can be used in addition to tell how the system works. In particular, performance indicators such as fluxes, activities or activity concentrations of selected radionuclides can show how the different components of the system fulfil their safety functions and contribute to the overall safety. The SPIN project of the European Commission assessed the usefulness of seven safety indicators and fourteen performance indicators by testing them in four actual assessments of disposal systems in granite formations. In this paper, indicators calculated from an assessment of the disposal of spent fuel in the poorly indurated Boom Clay formation are presented. Conclusions from the SPIN project that hold for repositories in clays are highlighted, as well as results that illustrate differences between the granite and clay disposal options. Finally, various performance and safety indicators are combined into a logical sequence to comprehensively present, and explain, the results of a safety assessment.


1989 ◽  
Vol 176 ◽  
Author(s):  
Bernd Grambow ◽  
L.O. Werme ◽  
R.S. Forsyth ◽  
J. Bruno

ABSTRACTComparison of spent fuel corrosion data from nuclear waste management projects in Canada, Sweden and the USA strongly suggests that the release of 90Sr to the leachant can be used as a measure of the degradation (oxidation/dissolution) of the fuel matrix. A surprisingly quantitative similarity in the 90 Sr release data for fuel of various types (BWR, PWR, Candu), linear power ratings and burnups leached under oxic conditions was observed in the comparison. After 1000 days of leachant contact, static or sequential, the fractional release rates for 90Sr (and for cesium nuclides) were of the order of 10−7/d.The rate of spent fuel degradation (alteration) under oxic conditions can be considered to be controlled either by the growth rates of secondary alteration products, by oxygen diffusion through a product layer, by the rate of formation of radiolytic oxidants or by solubility-controlled dissolution of the matrix. These processes are discussed. Methods for determining upper limits for long-term 90Sr release, and hence fuel degradation, have been derived from the experimental data and consideration of radiolytic oxidant production.


2006 ◽  
Vol 932 ◽  
Author(s):  
Andreas Loida ◽  
Manfred Kelm ◽  
Bernhard Kienzler ◽  
Horst Geckeis ◽  
Andreas Bauer

ABSTRACTThe long-term immobilization for individual radioelements released from the waste form “spent fuel” in solid phases upon groundwater contact depends strongly on the (geo)chemical constraints prevailing in the repository. Related experimental studies comprise effects induced by the presence of Fe based container material, and near field materials other than Fe for a rock salt environment. The effect of the presence of an argillaceous host rock containing organic matter and pyrite on fuel alteration was studied in addition. The results have shown that oxidative radio-lysis products were found to be consumed at a significant extent by the metallic Fe and by the argillaceous host rock. Under these conditions a decrease at a factor of ca.100 for both the matrix dissolution rates and the solution concentrations of U and Pu was found. There is mutual support between the matrix dissolution rates, the solution concentrations and the amounts of oxygen encountered during the experiments under various conditions controlled by the presence of near field materials under study.


2012 ◽  
Vol 1475 ◽  
Author(s):  
Aku Itälä ◽  
Arto Muurinen

ABSTRACTThe Finnish spent nuclear fuel disposal is based on the Swedish KBS-3 concept in crystalline bedrock. The concept aims at long-term isolation and containment of spent fuel in copper canisters surrounded by bentonite buffer which mostly consists of montmorillonite. For the long-term modelling of the chemical processes in the buffer, the cation-exchange selectivity coefficients have to be known at different temperatures. In this work, the cation-exchange selectivity coefficients and cation-exchange isotherms were determined in batch experiments for montmorillonite at three different temperatures (25 °C, 50 °C and 75 °C). Five different ratios of NaClO4/Ca(ClO4)2 were used in the experimental solutions. After equilibration the solution and montmorillonite were separated and the solution analysed to get the desired exchange parameters. The experiments were modelled with a computational model capable of taking into account the physicochemical processes that take place in the experiment.


2004 ◽  
Vol 824 ◽  
Author(s):  
A. B. Kolyadin ◽  
V. Ya. Mishin ◽  
K. Ya. Mishin ◽  
A. S. Aloy ◽  
T. I. Koltsova

AbstractThe oxidation of UO2–type spent nuclear fuel (SNF) in gaseousmedia was studied at different temperatures and oxygen contents using gravimetric and powder X-ray diffraction (XRD) techniques. The aim of the study was to determine the mechanism(s) of thermal-oxidation alteration of SNF during long-term dry storage. The samples used in the experiments were chips of RBMK-1000 fuel rods.Oxidation of UO2with a mean burn-up of 10.7 and 19.73 MW d/kg in humid air was observed at a temperature as low as 150°C. At 200°C nearly all of the UO2was transformed into U3O8 between 3500-4000 hours. In a humid nitrogen environment containing of 0.05-1.3 vol. % oxygen at 300°C, the UO2 completely transformed to U3O8 between 2500-3000 hours. Oxidation of UO2in samples with small amounts of jacket damage (e.g., <0.04 MM2)ll progresses more slowly and after â3000 hours the oxygen-to-uranium ratio was 2.56.Stabilization of the oxidation process was not observed in the fuel samples upto an O/U ratio of 2.4, which may be attributed to the smallburn-up of the fuel under investigation.


MRS Advances ◽  
2016 ◽  
Vol 1 (62) ◽  
pp. 4147-4156 ◽  
Author(s):  
C. Ferry ◽  
J. Radwan ◽  
H. Palancher

ABSTRACTHelium is produced in spent nuclear fuel by α-decays of actinides. After 10,000 years, the concentration of He accumulated in UO2 spent fuel is about 0.23 at.%. For direct disposal of spent nuclear fuel, consequences of helium build-up on the fuel matrix microstructure must be evaluated since it can modify the radionuclide release when water comes into contact with the spent fuel surface, after breaching of the disposal canister. An operational model has been proposed in order to evaluate the effect of helium on the microstructure of spent fuel in a repository. Based on conservative assumptions and different scenarios of bubble population, the calculated helium critical concentration, that could lead to a partial loss of integrity of the spent fuel pellet, is 0.37 at.%. However, observations on He-implanted UO2, α-doped UO2 pellets and natural analogues evidence a macroscopic damage only for He concentrations, which are more than one order of magnitude higher.


Energies ◽  
2020 ◽  
Vol 13 (9) ◽  
pp. 2239
Author(s):  
Leszek Lankof

Together with renewable energy sources, nuclear power represents an important contribution to a sustainable energy mix in many countries and has an important impact on sustainable development. Nuclear energy production is also a source of high-level radioactive waste (HLW) and spent nuclear fuel (SNF), which require special concern. Disposal in deep geological formations is one of the solutions for the long-term management of HLW and SNF. It requires the development of a concept ensuring long-term safe isolation of waste and its validation applying the safety case methodology, which is a formal compilation of evidence, analyses and arguments that quantify and justify a claim that the repository will be safe. The results of laboratory testing of a potential repository host rock are an important component of the evidence that helps in the safety assessment of the deep geological disposal concept. This paper presents results of research focused on the physical, geomechanical and sorption properties of the Brown and Red Zuber unit rocks from the Kłodawa Salt Mine in Poland, which together with rock salt are an important component of Polish salt domes. The Brown and Red Zubers are typical evaporite lithostratigraphic units for the Polish part of the Zechstein Basin. They consist of halite (15–85%) and water-insoluble minerals, such as anhydrite, clay minerals, carbonates, quartz and feldspar, which occurred in varying proportions in the tested samples. The properties of the zuber rocks have been compared with those of rock salt, which is considered a suitable host rock for deep geological disposal of radioactive waste.


2006 ◽  
Vol 932 ◽  
Author(s):  
Sonia Salah ◽  
Christelle Cachoir ◽  
Karel Lemmens ◽  
Norbert Maes

ABSTRACTSince reprocessing is no longer the reference policy in Belgium, studies on the direct disposal of spent fuel in a clay formation have gained increased interest in the last years. In order to determine to what extent the clay properties and the α-activity influence the dissolution kinetics of spent fuel for the long term disposal, static dissolution tests have been performed on 5 different types of α-doped UO2, representing a PWR fuel with a burn-up of 45 or 55 GWd · tHM−1 and fuel ages ranging between 150 and 90,000 years, in different Boom Clay (BC) media at room temperature and in an anoxic atmosphere for 90 to 720 days. The uranium activity in the clay fraction over time was found to be much higher than the U-activity in the leachates, which has been mainly ascribed to the high retention capacity of the BC. The average dissolution rate between 0 and 90 days obtained for the 5 types of α-doped UO2 were all found to be high and quite similar at ~263 µg · m−2 · d−1and a “longer-term” rate (181 to 720 days) ranging between zero and 15 µg · m−2· d−1. These results suggest that the activity of the fuels does not seem to have an effect on the UO2 dissolution rates under the considered test conditions. In order to study the partition/redistribution of U during UO2dissolution, sequential extraction experiments were performed. Results of the latter have provided a better mechanistic understanding of BC/spent fuel interaction processes as well as information on the role of the different minerals controlling the U-retention/immobilization.


MRS Advances ◽  
2016 ◽  
Vol 1 (61) ◽  
pp. 4075-4080
Author(s):  
Fredrik Vahlund

ABSTRACTSince 1988 the Swedish Nuclear Fuel and Waste Management Co. operates a repository for low- and intermediate-level short-lived radioactive waste, SFR, in Forsmark, Sweden. Due to decommissioning of the nuclear power plants additional storage capacity is needed. In December 2014, an application to extend the repository was therefore submitted. One key component of this application was an assessment of post-closure safety of the extended SFR. For this safety assessment, a methodology based on that developed by SKB for the spent nuclear fuel repository was used and the impact of the degradation of repository components, the evolution of the surface system and changes of future climate on the radiological safety of the repository was assessed over a period of 100,000 years. The central conclusion of the SR-PSU safety assessment is that the extended SFR repository meets requirements on protection of human health and of the environment that have been established by the Swedish radiation safety authority for the final disposal of radioactive waste. Furthermore, the design of the repository was shown suitable for the waste selected and the applied methodology suitable for the safety assessment.


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