Static dissolution tests of α-doped UO2 under repository relevant conditions: Influence of Boom Clay and α-activity on fuel dissolution rates

2006 ◽  
Vol 932 ◽  
Author(s):  
Sonia Salah ◽  
Christelle Cachoir ◽  
Karel Lemmens ◽  
Norbert Maes
Keyword(s):  
Clay Fraction ◽  
Dissolution Kinetics ◽  
Spent Fuel ◽  
Dissolution Rates ◽  
Retention Capacity ◽  
Boom Clay ◽  
Dissolution Tests ◽  
Clay Formation ◽  
Α Activity

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.

Static dissolution tests of α-doped UO2 under repository relevant conditions: Influence of Boom Clay and α-activity on fuel dissolution rates

2006 ◽  
Vol 932 ◽  
Author(s):  
Sonia Salah ◽  
Christelle Cachoir ◽  
Karel Lemmens ◽  
Norbert Maes
Keyword(s):  
Clay Fraction ◽  
Dissolution Kinetics ◽  
Spent Fuel ◽  
Dissolution Rates ◽  
Retention Capacity ◽  
Boom Clay ◽  
Dissolution Tests ◽  
Clay Formation ◽  
Α Activity

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.

UO2 dissolution in high pH conditions of the Belgian Supercontainer

2012 ◽  
Vol 1475 ◽  
Author(s):  
Th. Mennecart ◽  
C. Cachoir ◽  
K. Lemmens
Keyword(s):  
Spent Fuel ◽  
Dissolution Rates ◽  
High Ph ◽  
Neutral Ph ◽  
Dissolution Tests ◽  
Alkaline Conditions ◽  
Ph Conditions ◽  
Ph Range ◽  
Long Term Behavior

ABSTRACTTo assess the long-term behavior of spent fuel in alkaline conditions representative for the Belgian Supercontainer design, static and dynamic dissolution tests were performed with depleted and Pu-doped UO2 , simulating medium burn-up UOX fuels of different fuel ages. The experiments were performed under argon atmosphere at 25 – 30°C in cement waters in the pH range 11.7 – 13.5 and at different SA/V ratios. This paper presents the observed UO2 matrix dissolution rates based on the (238U or 233U) release, and proposes a selection of reference dissolution rates for performance assessment. We demonstrate that the dissolution rates at high pH are equivalent to the dissolution rates reported in the literature for neutral pH conditions. The α-activity threshold below which radiolytical fuel oxidation becomes negligible, seems to be close to the threshold reported for anoxic media at neutral pH.

Measurement of Glass Corrosion in Boom Clay Disposal Conditions

2001 ◽  
Author(s):  
Karel Lemmens ◽  
Marc Aertsens ◽  
Véra Pirlet ◽  
Hélène Serra ◽  
Elie Valcke ◽  
...  
Keyword(s):  
Dissolution Rate ◽  
Kinetic Modeling ◽  
Dissolution Time ◽  
Dissolution Test ◽  
Dissolution Rates ◽  
Boom Clay ◽  
Glass Dissolution ◽  
Dissolution Tests ◽  
Environmental Materials

Abstract To estimate the life-time of vitrified high level waste (HLW-glass) in geological disposal conditions in Boom Clay, the dissolution behaviour of waste glass has been studied in experiments in surface laboratories and in the HADES underground research facility of SCK•CEN since the 1980’s. The programme consists mainly of dissolution tests. The purpose of these tests is to understand the basic glass dissolution mechanisms, and to demonstrate realistic long-term dissolution rates. The main experimental variables are glass composition, environmental materials, temperature, and test duration. The studied glasses are the COGEMA glass R7T7, and the PAMELA glasses with SM539, SM527 and SM513 glass frit. The environmental materials comprise Boom Clay, metallic corrosion products and engineered barrier materials. Dissolution tests have been performed at temperatures from 40 to 190°C, for test durations from days to several years. The tests are performed with inactive glasses, which can be doped with radionuclides of interest. Because of the importance of silica sorption by the environmental materials, the dissolution test programme was extended with silica diffusion- and sorption tests in Boom Clay and FoCa clay. The interpretation of the experimental results is supported by geochemical and kinetic modeling. In the area of kinetic modeling, both analytical and Monte Carlo codes are applied. The dissolution tests have demonstrated that, although the presence of Boom Clay initially increases the glass dissolution rate, the long-term dissolution rate decreases for diluted clay / clay water slurries. This decrease has not yet been demonstrated for the R7T7 glass in compact Boom Clay, but is expected to occur here also on the long term. The dissolution rate decreases faster after sufficient addition of glass powder to the medium. This was tested in experiments with the R7T7 glass at relatively high clay concentration (2000 g of humid Boom Clay per liter clay water, this is about half the solid/liquid ratio of compact Boom Clay), at 40 and 90°C. Linear interpolation of the long-term mass losses resulted in dissolution rates of ∼ 0.01 g.m−2.day−1. The statistical uncertainties on the dissolution test results did not allow to demonstrate smaller rates. The minimum statistically significant dissolution rate depends on the test conditions. Therefore, the present SCK•CEN programme includes dissolution tests at long-term near-field conditions (this is at 30°C, with compact Boom Clay and FoCa clay), which are considered more representee for the long-term situation. In view of the uncertainties on the experimental long-term dissolution rates and on the long-term dissolution mechanisms, rates smaller than 0.01 g.m−2.day1 (about 1 μ/year) should not be used as best estimate in the present performance assessment studies for disposal in Boom Clay. A constant dissolution rate of 0.01 g.m−2.day−1 would correspond to a dissolution time for a R7T7 glass package of approximately 150 000 years. The minimum dissolution time is of the order of 104 years.

Functional Requirements and Performance Assessment: Application to the Case of Spent Fuel Disposal in Clay

2001 ◽  
Author(s):  
Jan Marivoet ◽  
Xavier Sillen ◽  
Peter De Preter
Keyword(s):  
Molecular Diffusion ◽  
Slow Release ◽  
Near Field ◽  
Functional Requirements ◽  
Spent Fuel ◽  
Systematic Analysis ◽  
Boom Clay ◽  
Safety Function ◽  
Clay Formation

Abstract Geological repository systems for the disposal of radioactive waste are based on a multi-barrier design. Individual barriers contribute in different ways to the overall long-term performance of the repository system, and furthermore, the contribution of each barrier can considerably change with time. In a systematic analysis of the functional requirements for achieving long-term safety a number of basic safety functions can be defined: physical confinement, retardation / slow release, dispersion / dilution and limited accessibility. In the case of the geological disposal of spent fuel in a clay formation a series of barriers are designed or chosen to contribute to the realisation of the basic safety functions. The physical confinement is realised by the watertight, high-integrity container, which prevents contact between groundwater and the confined radionuclides. In first instance the retardation / slow release function is realised by the slow dissolution of the waste matrix and by the limited solubility of many elements in the near field. However, the natural clay barrier provides the main contribution to this safety function. The migration of radionuclides through the Boom Clay is mainly due to molecular diffusion, which is an extremely slow process. Furthermore, many elements are strongly sorbed by the clay minerals what makes their migration even much slower. The dispersion / dilution function mainly occurs in the aquifer and the rivers draining the aquifer in the surroundings of the disposal system. Various performance indicators are used to quantify the contributions of each safety function and to explain the functioning of the repository system.

Testing Safety and Performance Indicators in an Assessment of the Long-Term Performance of the Geological Disposal of Spent Fuel in Boom Clay

2003 ◽  
Author(s):  
Xavier Sillen ◽  
Jan Marivoet ◽  
Wim Cool ◽  
Peter de Preter
Keyword(s):  
Dose Rate ◽  
Performance Indicators ◽  
Spent Fuel ◽  
Geological Disposal ◽  
Boom Clay ◽  
And Performance ◽  
The Individual ◽  
High Level ◽  
Clay Formation

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.

On the Role of H2 as an Inhibitor of UO2 Matrix Dissolution

2007 ◽  
Author(s):  
Juan Merino ◽  
Xavier Gaona ◽  
Lara Duro ◽  
Jordi Bruno ◽  
Aurora Marti´nez-Esparza
Keyword(s):  
Chemical Composition ◽  
Partial Pressure ◽  
Water Radiolysis ◽  
Water Interface ◽  
Spent Fuel ◽  
Dissolution Rates ◽  
Term Stability ◽  
Long Term Stability

The study of spent fuel behaviour under disposal conditions is usually based on conservative approaches assuming oxidising conditions produced by water radiolysis at the fuel/water interface. However, the presence of H2 from container corrosion can inhibit the dissolution of the UO2 matrix and enhance its long-term stability. Several studies have confirmed the decrease in dissolution rates when H2 is present in the system, although the exact mechanisms of interaction have not been fully established. This paper deals with a radiolytic modelling exercise to explore the consequences of the interaction of H2 with radicals generated by radiolysis in the homogeneous phase. The main conclusion is that in all the modelled cases the presence of H2 in the system leads to a decrease in matrix dissolution. The extent of the inhibition, and the threshold partial pressure for the inhibition to take place, both depend in a complex way on the chemical composition of the water and the type of radiation present in the system.

The Effect of Nearfield Constraints on the Corrosion Behavior of High Burnup Spent Fuel

2006 ◽  
Vol 932 ◽  
Author(s):  
Andreas Loida ◽  
Manfred Kelm ◽  
Bernhard Kienzler ◽  
Horst Geckeis ◽  
Andreas Bauer
Keyword(s):  
Host Rock ◽  
Near Field ◽  
Experimental Studies ◽  
Spent Fuel ◽  
Mutual Support ◽  
Significant Extent ◽  
Dissolution Rates ◽  
The Matrix ◽  
Container Material

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.

scholarly journals Dissolution Rates of DWPF Glasses from Long-Term PCT

1996 ◽  
Vol 465 ◽  
Author(s):  
W. L. Ebert ◽  
S.-W. Tam
Keyword(s):  
Dissolution Rate ◽  
Surface Area ◽  
Spherical Particles ◽  
Dissolution Rates ◽  
Glass Dissolution ◽  
Dissolution Tests ◽  
Dissolution Model ◽  
Advanced Stages ◽  
Radionuclide Release

ABSTRACTWe have characterized the corrosion behavior of several Defense Waste Processing Facility (DWPF) reference waste glasses by conducting static dissolution tests with crushed glasses. Glass dissolution rates were calculated from measured B concentrations in tests conducted for up to five years. The dissolution rates of all glasses increased significantly after certain alteration phases precipitated. Calculation of the dissolution rates was complicated by the decrease in the available surface area as the glass dissolves. We took the loss of surface area into account by modeling the particles to be spheres, then extracting from the short-term test results the dissolution rate corresponding to a linear decrease in the radius of spherical particles. The measured extent of dissolution in tests conducted for longer times was less than predicted with this linear dissolution model. This indicates that advanced stages of corrosion are affected by another process besides dissolution, which we believe to be associated with a decrease in the precipitation rate of the alteration phases. These results show that the dissolution rate measured soon after the formation of certain alteration phases provides an upper limit for the long-term dissolution rate, and can be used to determine a bounding value for the source term for radionuclide release from waste glasses. The long-term dissolution rates measured in tests at 20,000 m−1 at 90°C in tuff groundwater at pH values near 12 are about 0.2,0.07, and 0.04 g/(m2•d) for the Environmental Assessment glass and glasses made with SRL 131 and SRL 202 frits, respectively.

Corrosion Behavior of High Burnup Spent Fuel in Highly Alkaline Solutions

2009 ◽  
Vol 1193 ◽  
Author(s):  
A. Loida ◽  
R. Gens ◽  
V. Metz ◽  
K. Lemmens ◽  
C. Cachoir ◽  
...  
Keyword(s):  
Nuclear Fuel ◽  
Spent Nuclear Fuel ◽  
Waste Product ◽  
Alkaline Solutions ◽  
Spent Fuel ◽  
Boom Clay ◽  
Matrix Bound ◽  
Engineered Barriers ◽  
Clay Formation ◽  
Fractional Release

AbstractThis study is focused on the alteration behavior of spent nuclear fuel when exposed to highly alkaline groundwater. Contact of highly alkaline solution with the waste product is considered in the Belgian concept for disposal in the Boom Clay formation. According to the “supercontainer design” the fuel will be encapsulated in carbon steel canisters, surrounded by a concrete over-pack. After saturation of the engineered barriers by porewater, interactions with the concrete will result in solutions rich in NaOH, KOH and Ca(OH)2. Using this type of solution at pH 12.5, spent nuclear fuel corrosion experiments were conducted over 378 days. Under anoxic conditions, parallel experiments were performed (a) in the absence of Fe phases and (b) in the presence of solid Fe phases representing container (corrosion) products. Both types of experiments resulted in relatively low matrix dissolution rates, around 10-7 per day, according to the fractional release of Sr. Solution concentrations of actinides are close to or below the detection limit, indicating an effective retention of these radioelements in the system. The observed precipitation of a Ca rich phase onto the surfaces of the corroded fuel samples may be related to the inhibited re-lease of actinides, Sr and other matrix bound radioelements.

Safety Assessment of Geological Disposal of High-Level Radioactive Waste in Boom Clay: Relation With the Radionuclide Inventory

2009 ◽  
Author(s):  
Pierre Van Iseghem ◽  
Jan Marivoet
Keyword(s):  
Radioactive Waste ◽  
Safety Assessment ◽  
High Level Waste ◽  
Spent Fuel ◽  
Geological Disposal ◽  
High Level Radioactive Waste ◽  
Boom Clay ◽  
High Level ◽  
Clay Formation ◽  
Parameter Values

This paper discusses the impact of the parameter values used for the transport of radionuclides from high-level radioactive waste to the far-field on the long-term safety of a proposed geological disposal in the Boom Clay formation in Belgium. The methodology of the Safety Assessment is explained, and the results of the Safety Assessment for vitrified high-level waste and spent fuel are presented. The radionuclides having the strongest impact on the dose-to-man for both HLW glass and spent fuel are 79Se, 129I, 126Sn, 36Cl, and 99Tc. Some of them are volatile during the vitrification process, other radionuclides are activation products, and for many of them there is no accurate information on their inventory in the waste form. The hypotheses in the selection of the main parameter values are further discussed, together with the status of the R&D on one of the main dose contributing radionuclides (79Se).

Sign in / Sign up

Export Citation Format

Share Document