Potential impact of cementitious leachates on the buffer porewater chemistry in the Finnish repository for spent nuclear fuel – A reactive transport modelling assessment (original) (raw)
Related papers
Applied Clay Science, 2014
The Swedish Nuclear Fuel and Waste Management Company (SKB) is conducting a series of long term tests at the Äspö Hard Rock Laboratory to assess the behaviour of the bentonite buffer under conditions similar to those expected in a KBS-3 repository for high level nuclear waste. The LOT A2 experiment consists of a vertical borehole with a central heater inside a copper tube surrounded by compacted bentonite. During four years, the temperature of the copper tube was maintained at 130°C, while the bentonite was progressively water saturated by the injection of groundwater. During this period, physical and hydro-geochemical data were collected. By using the code TOUGHREACT, a model was made to simulate the processes of solute transport which control the chemical and the mineralogical distribution observed in the bentonite at the end of the test. Additionally, a series of sensitivity analyses was performed to assess the influence of key parameters controlling the thermalhydro-geochemical processes. Numerical results indicate that, within the first year, the heated bentonite blocks are completely water saturated, which agree with the measured data. The simulated transport of chloride, the dissolution/precipitation of Ca sulphate minerals, and the cation redistribution in the montmorillonite interlayer also agree with data measured at the end of the experiment.
Journal of contaminant hydrology, 2017
Radioactive waste disposal in deep geological repositories envisages engineered barriers such as carbon-steel canisters, compacted bentonite and concrete liners. The stability and performance of the bentonite barrier could be affected by the corrosion products at the canister-bentonite interface and the hyper-alkaline conditions caused by the degradation of concrete at the bentonite-concrete interface. Additionally, the host clay formation could also be affected by the hyper-alkaline plume at the concrete-clay interface. Here we present a non-isothermal multicomponent reactive transport model of the long-term (1Ma) interactions of the compacted bentonite with the corrosion products of a carbon-steel canister and the concrete liner of the engineered barrier of a high-level radioactive waste repository in clay. Model results show that magnetite is the main corrosion product. Its precipitation reduces significantly the porosity of the bentonite near the canister. The degradation of the...
Applied Geochemistry, 2016
Here we present a long-term nonisothermal reactive transport model for the interactions of the corrosion products of a carbon-steel canister and the compacted bentonite of the engineered barrier of a highlevel radioactive waste repository in granite. Canister corrosion causes an increase in the pH and the concentration of dissolved Fe 2þ of the bentonite porewater. Iron precipitates as magnetite and siderite and sorbs via cation exchange and surface complexation on weak sites. Magnetite precipitation reduces significantly the porosity of the bentonite near the canister. The thickness of the zone of reduced porosity is 7 cm at t ¼ 1 Ma. This thickness increases significantly when the dependence of the corrosion rate on the chemical conditions is considered and decreases 3 cm when smectite dissolution and analcime precipitation are taken into account. Model results are not significantly sensitive to the thermal transient and the effect of temperature on the corrosion rate. The conclusions of our simulations are consistent for the most part with those reported by others for engineered barrier systems at similar chemical conditions.
Nuclear Technology
Finnish spent nuclear fuel disposal is planned to be based on the KBS-3V concept. Within this concept, the role of the bentonite buffer has been considered to be central. The aim was to model the evolution of a final repository during the thermal phase (heatgenerating period of spent fuel), when the bentonite is partially saturated at the beginning, and the rock matrix surrounding it is fully saturated. It is essential to study how temperature affects saturation and how both of these affect the chemistry of bentonite. In order to make the modelling more concrete, an experimental case was adopted: the Long Term Test of Buffer Materials (LOT) A2-parcel test at the Äspö Hard Rock Laboratory (HRL) in Sweden. In the A2-parcel the MX-80 bentonite was exposed to adverse (120-150 o C) temperature conditions and high-temperature gradients. The test parcel diameter was smaller than in the KBS-3V concept to speed up the saturation. Different kinds of thermodynamic and kinetic properties of minerals cause a redistribution of phases inside the bentonite. For example, according to laboratory tests, gypsum seems to dissolve and anhydrite seems to precipitate near the heater-bentonite interface. Also incoming groundwater affects the bentonite porewater and its properties. These changes may affect the mechanical properties of bentonite and it has to be clarified if these phenomena have to be taken into account in safety assessment. The applied model is a coupled thermo-hydro-chemical model, which means that all the mechanical alterations and effects are not considered. The purpose of the model was first to obtain similarity to the results compared to the experiment, and thus, the time frame was limited to 10 years (the LOT A-2 parcel test lasted approximately 6 years). The system is simplified to 1-D in order to reduce the computational work, which is significant mostly due to complex chemical calculations. TOUGH and TOUGHREACT was applied to model the reactive unsaturated transport processes in 1-D and the grid was pitched at uniform intervals. The results may be used to gain knowledge of the bentonite evolution during the thermal phase, and after a good match with experiment the modelling can be continued until the end of the thermal phase for thousands of years.
Minerals
The construction of a repository for the geological disposal of radioactive waste will include the use of cement-based materials. Following closure, groundwater will saturate the repository, and the extensive use of cement will result in the development of a highly alkaline porewater, pH > 12.5; this fluid will migrate into and react with the host rock. The chemistry of the fluid will evolve over time, initially with high Na and K concentrations, evolving to a Ca-rich fluid, and finally returning to the natural background groundwater composition. This evolving chemistry will affect the long-term performance of the repository, altering the physical and chemical properties, including radionuclide behaviour. Understanding these changes forms the basis for predicting the long-term evolution of the repository. This study focused on the determination of the nature and extent of the chemical reaction, as well as the formation and persistence of secondary mineral phases within a granite,...
Applied Sciences
Bentonite is used as a buffer material in most high-level radioactive waste (HLW) repository designs. Smectite clay is the main mineral component of bentonite and plays a key role in controlling the buffer’s physical and chemical behaviors. Moreover, the long-term functions of buffer clay could be lost through smectite dehydration under the prevailing temperature stemming from the heat of waste decay. Therefore, the influence of waste decay temperatures on bentonite performance needs to be studied. However, seldom addressed is the influence of the thermo-hydro-chemical (T-H-C) processes on buffer material degradation in the engineered barrier system (EBS) of HLW disposal repositories as related to smectite clay dehydration. Therefore, we adopted the chemical kinetic model of smectite dehydration to calculate the amount of water expelled from smectite clay minerals caused by the higher temperatures of waste decay heat. We determined that the temperature peak of about 91.3 °C occurred...
Minerals
The construction of a repository for geological disposal of radioactive waste will include the use of cement-based materials. Following closure, groundwater will saturate the repository and the extensive use of cement will result in the development of a highly alkaline porewater, pH > 12.5; this fluid will migrate into and react with the host rock. The chemistry of the fluid will evolve over time, initially high [Na] and [K], evolving to a Ca-rich fluid, and finally returning to the groundwater composition. This evolving chemistry will affect the long-term performance of the repository, altering the physical and chemical properties, including radionuclide behaviour. Understanding these changes forms the basis for predicting the long-term evolution of the repository. This study focused on the determination of the nature and extent of the chemical reaction, as well as the formation and persistence of secondary mineral phases within a mudstone, comparing data from sequential flow ex...
2009
The bentonite barrier is an essential part of a safe spent fuel repository in granitic bedrock. In this work COMSOL Multiphysics® is used in modelling the thermal (T), hydrological (H), mechanical (M) and chemical (C) phenomena and processes taking place in a bentonite buffer. Special interest lies in systems in which the density of bentonite or bentonite pore water varies. Typically, variation occurs during the erosion and wetting stage of bentonite. The reason for developing COMSOL models for this purpose is the lack of commercially available software, which typically covers either THC or THM models; M and C are not modelled together.