Climate Considerations in Long-Term Safety Assessments for Nuclear Waste Repositories

For a deep geological repository for spent nuclear fuel planned in Sweden, the safety assessment covers up to 1 million years. Climate scenarios range from high-end global warming for the coming 100 000 years, through deep permafrost, to large ice sheets during glacial conditions. In contrast, in an existing repository for short-lived waste the activity decays to low levels within a few tens of thousands of years. The shorter assessment period, 100 000 years, requires more focus on climate development over the coming tens of thousands of years, including the earliest possibility for permafrost growth and freezing of the engineered system. The handling of climate and climate change in safety assessments must be tailor-made for each repository concept and waste type. However, due to the uncertain future climate development on these vast time scales, all safety assessments for nuclear waste repositories require a range of possible climate scenarios.     

Contribution to a more realistic approach in assessing the release of C-14 from low-level radioactive waste repositories

The contribution of C-14 to radiation exposure in the biosphere can be significant as compared to that of other radionuclides disposed in a repository for low-level radioactive waste. The release pathways of C-14 and processes relevant to its release from a closed final repository for low-level radioactive waste are discussed. Because a conservative approach may lead to undue overestimation of the potential radiation exposure, a more realistic approach is outlined. At the present level of refinement, our approach helps to provide a sufficient safety margin to German dose limits for radiation exposure of 0.3 mSv and can thus facilitate licence approval.     

A mountain-scale thermal-hydrologic model for simulating fluid flow and heat transfer in unsaturated fractured rock

A multidimensional, mountain-scale, thermal-hydrologic (TH) numerical model is presented for investigating unsaturated flow behavior in response to decay heat from the proposed radioactive waste repository in the Yucca Mountain unsaturated zone (UZ), The model, consisting of both two-dimensional (2-D) and three-dimensional (3-D) representations of the UZ repository system, is based on the current repository design, drift layout, thermal loading scenario, and estimated current and future climate conditions. This mountain-scale TH model evaluates the coupled TH processes related to mountain-scale UZ flow. It also simulates the impact of radioactive waste heat release on the natural hydrogeological system, including heat-driven processes occurring near and far away from the emplacement tunnels or drifts. The model simulates predict thermally perturbed liquid saturation, gas- and liquid-phase fluxes, and water and rock temperature elevations, as well as the changes in water flux driven by evaporation/condensation processes and drainage between drifts. These simulations provide insights into mountain-scale thermally perturbed flow fields under thermal loading conditions.     

Degradation of tetraphenylphosphonium bromide at high pH and its effect on radionuclide solubility

Recently, tetraphenylphosphonium bromide (TPPB) has been used to remove technetium from some radioactive waste streams. However, before TPPB could be approved for use it was necessary to show that TPPB and its degradation products would not have a significant detrimental effect on post-closure performance of a radioactive waste repository. TPPB is known to be stable at neutral pH, however, under alkaline conditions it degrades by an alkaline hydrolysis mechanism to triphenylphosphonium oxide (TPPO). Degradation can also occur by radiolysis to produce triphenylphosphine (TPP). The kinetics of the alkaline hydrolysis degradation of TPPB is described and the solubility of europium, iodine, nickel, technetium(VII) and uranium(VI) in aqueous solutions of TPPB and its degradation products is reported. These results were used to support the use of TPPB in removing technetium from some waste streams.     

A carbon budget of a small humic lake: an example of the importance of lakes for organic matter cycling in boreal catchments

Lakes play an important role in the cycling of organic matter in the boreal landscape, due to the frequently high extent of bacterial respiration and the efficient burial of organic carbon in sediments. Based on a mass balance approach, we calculated a carbon budget for a small humic Swedish lake in the vicinity of a potential final repository for radioactive waste in Sweden, in order to assess its potential impact on the environmental fate of radionuclides associated with organic matter. We found that the lake is a net heterotrophic ecosystem, subsidized by organic carbon inputs from the catchment and from emergent macrophyte production. The largest sink of organic carbon is respiration by aquatic bacteria and subsequent emission of carbon.dioxide to the atmosphere. Although the annual burial of organic carbon in the sediment is a comparatively small sink, it results in the build-up of the largest carbon pool in the lake. Hence, lakes may simultaneously disperse and accumulate organic-associated radionuclides leaking from a final repository.     

Long-term oxygen depletion from infiltrating groundwaters: model development and application to intra-glaciation and glaciation conditions

Processes that control the redox conditions in deep groundwaters have been studied. The understanding of such processes in a long-term perspective is important for the safety assessment of a deep geological repository for high-level nuclear waste. An oxidising environment at the depth of the repository would increase the solubility and mobility of many radionuclides, and increase the potential risk for radioactive contamination at the ground surface. Proposed repository concepts also include engineered barriers such as copper canisters, the corrosion of which increases considerably in an oxidising environment compared to prevailing reducing conditions. Swedish granitic rocks are typically relatively sparsely fractured and are best treated as a dual-porosity medium with fast flowing channels through fractures in the rock with a surrounding porous matrix, the pores of which are accessible from the fracture by diffusive transport. Highly simplified problems have been explored with the aim to gain understanding of the underlying transport processes, thermodynamics and chemical reaction kinetics. The degree of complexity is increased successively, and mechanisms and processes identified as of key importance are included in a model framework. For highly complex models, analytical expressions are not fully capable of describing the processes involved, and in such cases the solutions are obtained by numerical calculations. Deep in the rock the main source for reducing capacity is identified as reducing minerals. Such minerals are found inside the porous rock matrix and as infill particles or coatings in fractures in the rock. The model formulation also allows for different flow modes such as flow along discrete fractures in sparsely fractured rocks and along flowpaths in a fracture network. The scavenging of oxygen is exemplified for these cases as well as for more comprehensive applications, including glaciation considerations. Results show that chemical reaction kinetics control the scavenging of oxygen during a relatively short time with respect to the lifetime of the repository. For longer times the scavenging of oxygen is controlled by transport processes in the porous rock matrix. The penetration depth of oxygen along the flowpath depends largely on the hydraulic properties, which may vary significantly between different locations and situations. The results indicate that oxygen, in the absence of easily degradable organic matter, may reach long distances along a flow path during the life-time of the repository (hundreds to thousands of metres in a million years depending on e.g. hydraulic properties of the flow path and the availability of reducing capacity). However, large uncertainties regarding key input parameters exist leading to the conclusion that the results from the model must be treated with caution pending more accurate and validated data. Ongoing and planned experiments are expected to reduce these uncertainties, which are required in order to make more reliable predictions for a safety assessment of a nuclear waste repository.     

Geochemical evaluation of different groundwater–host rock systems for radioactive waste disposal

The geochemical suitability of a deep bedrock repository for radioactive waste disposal is determined by the composition of geomatrix and groundwater. Both influence radionuclide solubility, chemical buffer capacity and radionuclide retention. They also determine the chemical compatibility of waste forms, containers and backfill materials. Evaluation of different groundwater–host rock systems is performed by modeling the geochemical environments and the resulting radionuclide concentrations. In order to demonstrate the evaluation method, model calculations are applied to data sets available for various geological formations such as granite, clay and rocksalt.The saturation state of the groundwater–geomatrix system is found to be fundamental for the evaluation process. Hence, calculations are performed to determine if groundwater is in equilibrium with mineral phases of the geological formation. In addition, corrosion of waste forms in different groundwater is examined by means of reaction path modeling. The corrosion reactions change the solution compositions and pH, resulting in significant changes of radionuclide solubilities. The results demonstrate that geochemical modeling of saturation state and compatibility of the host formation environment with the radioactive waste proves to be a feasible tool for evaluation of various sites considered as deep underground repositories.     

Characterization of flow and transport processes within the unsaturated zone of Yucca Mountain, Nevada, under current and future climates

This paper presents a large-scale modeling study characterizing fluid flow and tracer transport in the unsaturated zone of Yucca Mountain, Nevada, a potential repository site for storing high-level radioactive waste. The study has been conducted using a three-dimensional numerical model, which incorporates a wide variety of field data and takes into account the coupled processes of flow and transport in the highly heterogeneous, unsaturated fractured porous rock. The modeling approach is based on a dual-continuum formulation of coupled multiphase fluid and tracer transport through fractured porous rock. Various scenarios of current and future climate conditions and their effects on the unsaturated zone are evaluated to aid in the assessment of the proposed repository's system performance using different conceptual models. These models are calibrated against field-measured data. Model-predicted flow and transport processes under current and future climates are discussed.     

Assessment of Long-Term Radiological Effects on Plants and Animals from a Deep Geological Repository: No Discernible Impact Detected

This study investigates whether non-human biota are protected against harmful effects of ionizing radiation after a possible future release of radioactive matter from a planned repository for spent nuclear fuel. Radiation dose rates to a broad spectrum of organisms were calculated based on data from sampled organisms and modeled activity concentrations. Calculations were performed with the ERICA Tool, a software program which applies a screening dose-rate value of 10 microgray per hour (μGy h^?1) for all types of organisms. Dose rates below this value are thought to result in minimal risk to the individual or population. All calculated dose rates were below the screening value and below the lowest relevant band of “derived consideration levels” proposed by the International Commission on Radiological Protection. This provides a sound basis for arguing that no individuals or populations of examined species would be harmfully affected by a possible radioactive release from the repository.     

The effect of coupled transport phenomena in the Opalinus Clay and implications for radionuclide transport

In this study, the potential effects of coupled transport phenomena on radionuclide transport in the vicinity of a repository for vitrified high-level radioactive waste (HLW) and spent nuclear fuel (SF) hosted by the Opalinus Clay in Switzerland, at times equal to or greater than the expected lifetime of the waste canisters (about 1000 years), are addressed. The solute fluxes associated with advection, chemical diffusion, thermal and chemical osmosis, hyperfiltration and thermal diffusion have been incorporated into a simple one-dimensional transport equation. The analytical solution of this equation, with appropriate parameters. shows that thermal osmosis is the only coupled transport mechanism that could, on its own, have a strong effect on repository performance. Based on the results from the analytical model, two-dimensional finite-difference models incorporating advection and thermal osmosis, and taking conservation of fluid mass into account, have been formulated. The results show that, under the conditions in the vicinity of the repository at the time scales of interest, and due to the constraints imposed by conservation of fluid mass, the advective component of flow will oppose and cancel the thermal-osmotic component. The overall conclusion is that coupled phenomena will only have a very minor impact on radionuclide transport in the Opalinus Clay, in terms of fluid and solute fluxes, at least under the conditions prevailing at times equal to or greater than the expected lifetime of the waste canisters (about 1000 years).     

A laboratory experiment for determining both the hydraulic and diffusive properties and the initial pore-water composition of an argillaceous rock sample: a test with the Opalinus clay (Mont Terri, Switzerland)

Argillaceous formations are thought to be suitable natural barriers to the release of radionuclides from a radioactive waste repository. However, the safety assessment of a waste repository hosted by an argillaceous rock requires knowledge of several properties of the host rock such as the hydraulic conductivity, diffusion properties and the pore water composition. This paper presents an experimental design that allows the determination of these three types of parameters on the same cylindrical rock sample. The reliability of this method was evaluated using a core sample from a well-investigated indurated argillaceous formation, the Opalinus Clay from the Mont Terri Underground Research Laboratory (URL) (Switzerland). In this test, deuterium- and oxygen-18-depleted water, bromide and caesium were injected as tracer pulses in a reservoir drilled in the centre of a cylindrical core sample. The evolution of these tracers was monitored by means of samplers included in a circulation circuit for a period of 204 days. Then, a hydraulic test (pulse-test type) was performed. Finally, the core sample was dismantled and analysed to determine tracer profiles. Diffusion parameters determined for the four tracers are consistent with those previously obtained from laboratory through-diffusion and in-situ diffusion experiments. The reconstructed initial pore-water composition (chloride and water stable-isotope concentrations) was also consistent with those previously reported. In addition, the hydraulic test led to an estimate of hydraulic conductivity in good agreement with that obtained from in-situ tests.     

Geochemical evaluation of different groundwater-host rock systems for radioactive waste disposal

The geochemical suitability of a deep bedrock repository for radioactive waste disposal is determined by the composition of geomatrix and groundwater. Both influence radionuclide solubility, chemical buffer capacity and radionuclide retention. They also determine the chemical compatibility of waste forms, containers and backfill materials. Evaluation of different groundwater-host rock systems is performed by modeling the geochemical environments and the resulting radionuclide concentrations. In order to demonstrate the evaluation method, model calculations are applied to data sets available for various geological formations such as granite, clay and rocksalt. The saturation state of the groundwater-geomatrix system is found to be fundamental for the evaluation process. Hence, calculations are performed to determine if groundwater is in equilibrium with mineral phases of the geological formation. In addition, corrosion of waste forms in different groundwater is examined by means of reaction path modeling. The corrosion reactions change the solution compositions and pH, resulting in significant changes of radionuclide solubilities. The results demonstrate that geochemical modeling of saturation state and compatibility of the host formation environment with the radioactive waste proves to be a feasible tool for evaluation of various sites considered as deep underground repositories.     

Modelling geochemical and microbial consumption of dissolved oxygen after backfilling a high level radiactive waste repository

Dissolved oxygen (DO) left in the voids of buffer and backfill materials of a deep geological high level radioactive waste (HLW) repository could cause canister corrosion. Available data from laboratory and in situ experiments indicate that microbes play a substantial role in controlling redox conditions near a HLW repository. This paper presents the application of a coupled hydro-bio-geochemical model to evaluate geochemical and microbial consumption of DO in bentonite porewater after backfilling of a HLW repository designed according to the Swedish reference concept. In addition to geochemical reactions, the model accounts for dissolved organic carbon (DOC) respiration and methane oxidation. Parameters for microbial processes were derived from calibration of the REX in situ experiment carried out at the Asp? underground laboratory. The role of geochemical and microbial processes in consuming DO is evaluated for several scenarios. Numerical results show that both geochemical and microbial processes are relevant for DO consumption. However, the time needed to consume the DO trapped in the bentonite buffer decreases dramatically from several hundreds of years when only geochemical processes are considered to a few weeks when both geochemical reactions and microbially-mediated DOC respiration and methane oxidation are taken into account simultaneously.     

Bacterial interactions with uranium: An environmental perspective

The presence of actinides in radioactive wastes is of major concern because of their potential for migration from the waste repositories and long-term contamination of the environment. Studies have been and are being made on inorganic processes affecting the migration of radionuclides from these repositories to the environment but it is becoming increasingly evident that microbial processes are of importance as well. Bacteria interact with uranium through different mechanisms including, biosorption at the cell surface, intracellular accumulation, precipitation, and redox transformations (oxidation/reduction). The present study is intended to give a brief overview of the key processes responsible for the interaction of actinides e.g. uranium with bacterial strains isolated from different extreme environments relevant to radioactive repositories. Fundamental understanding of the interaction of these bacteria with U will be useful for developing appropriate radioactive waste treatments, remediation and long-term management strategies as well as for predicting the microbial impacts on the performance of the radioactive waste repositories.     

Scoping analyses of geochemical sealing of early cracks in a waste container and associated drip shield, Yucca Mountain, Nevada

Early after final emplacement of the nuclear waste containers at the proposed Yucca Mountain, Nevada, high-level-waste repository, tiny cracks (less than 200 microm wide, 1 to 2 cm deep, and a few centimeters long at most) could appear in the containers and in the drip shield protecting them. Modeling calculations were performed to understand how fast those cracks could be sealed. Under dripping conditions, they are expected to be bridged with water. If cracks are located in the drip shield, any further dripping on the waste containers located underneath will be limited. If cracks are located in a container, potentially harmful radionuclides could only travel by diffusion. In addition, water-bridged cracks will be sealed through at least two processes: precipitation of calcite with minor silica following evaporative concentration of the water residing in the cracks and continuous corrosion of the crack walls. The sealing rate is calculated as the intersection of the time of emergence of the cracks, the water dripping rate, and the decreasing evaporation rate. The evaporative driving force declines as short-lived radioactive elements, having given up much of the heat affecting the repository, are progressively depleted from the waste. Depending on the crack initiation time and environmental conditions, crack sealing varies from a few tens of years to a few thousand years. Because environmental conditions in the vicinity of the cracks and at the crack scale have not been produced, a parametric method scaling drift scale conditions is used.     

A natural analogue of high-pH cement pore waters from the Maqarin area of northern Jordan: Comparison of predicted and observed trace-element chemistry of uranium and selenium

Current design concepts for low-/intermediate-level radioactive waste disposal in many countries involve emplacement underground in a cementitious repository. The highly alkaline groundwaters at Maqarin, Jordan, are a good analogue for the cementitious pore waters that will be present within such a repository. A geochemical modelling study of these groundwaters has been carried out in order to test the applicability of equilibrium models in geochemical programs and their associated thermodynamic databases in such hyperalkaline conditions. This was achieved by comparison of elemental solubilities and speciations predicted by the programs with observations in the natural system. Five organisations took part in the study: AEA Technology, U.K.; Chalmers University of Technology, Sweden; MBT Tecnología Ambiental, Spain; Nagra, Switzerland; and SKB, Sweden. The modelling study was coordinated by the University of Berne.The results of the study showed good agreement between the predictions of the programs employed. Comparison of the observed solids with those predicted by the models has allowed limited validation of the databases. The results for U and Se are presented here.     

Preliminary 3-D site-scale studies of radioactive colloid transport in the unsaturated zone at Yucca Mountain,Nevada

The U.S. Department of Energy (DOE) is actively investigating the technical feasibility of permanent disposal of high-level nuclear waste in a repository to be situated in the unsaturated zone (UZ) at Yucca Mountain (YM), Nevada. In this study we investigate, by means of numerical simulation, the transport of radioactive colloids under ambient conditions from the potential repository horizon to the water table. The site hydrology and the effects of the spatial distribution of hydraulic and transport properties in the Yucca Mountain subsurface are considered. The study of migration and retardation of colloids accounts for the complex processes in the unsaturated zone of Yucca Mountain, and includes advection, diffusion, hydrodynamic dispersion, kinetic colloid filtration, colloid straining, and radioactive decay. The results of the study indicate that the most important factors affecting colloid transport are the subsurface geology and site hydrology, i.e., the presence of faults (they dominate and control transport), fractures (the main migration pathways), and the relative distribution of zeolitic and vitric tuffs. The transport of colloids is strongly influenced by their size (as it affects diffusion into the matrix, straining at hydrogeologic unit interfaces, and transport velocity) and by the parameters of the kinetic-filtration model used for the simulations. Arrival times at the water table decrease with an increasing colloid size because of smaller diffusion, increased straining, and higher transport velocities. The importance of diffusion as a retardation mechanism increases with a decreasing colloid size, but appears to be minimal in large colloids.     

Issues in Low-Level Radioactive Waste Management

As a result of the breakdown of the nation’s radioactive waste management system in 1979, Congress has set a 1992 deadline for states to join together in regional "compacts" to manage and dispose of their own low-level radioactive waste. This article describes the challenges and opportunities associated with developing a new generation of waste management technologies and their institutional infrastructure, and earning the public’s confidence in them. It is written from the perspective of the Chair of the Central Midwest Compact (IL-KY) Compact Commission, but the issues are generic. In fact, their resolution is likely to set precedents for the way we deal with other hazardous wastes in the future.     

Solute transport properties of compacted Ca-bentonite used in FEBEX project

The present Spanish concept of a deep geological high level waste repository includes an engineered clay barrier around the canister. The clay presents a very high sorption capability for radionuclides and a very small hydraulic conductivity, so that the migration process of solutes is limited by sorption and diffusion processes. Therefore, diffusion and distribution coefficients in compacted bentonite (i.e. in "realistic" liquid to solid ratio conditions) are the main parameters that have to be obtained in order to characterise solute transport that could be produced after the canister breakdown. Through-Diffusion (TD) and In-Diffusion (ID) experiments with HTO, Sr, Cs and Se were carried out using compacted FEBEX bentonite, which is the reference material for the Spanish concept of radioactive waste disposal. Experiments were interpreted by means of available analytical solutions that allow the estimation of diffusion coefficients and, in some cases, distribution coefficients. Analytical solutions are simple to use, but rely on hypotheses that do not hold in all the experiments. These experiments were interpreted also using an automatic parameter estimation code that overcomes the limitations of analytical solutions. Numerical interpretation allows the simultaneous estimation of porosity, diffusion and distribution coefficients, accounts for the role of porous sinters and time-varying boundary concentrations, and can use different types of raw concentration data.     

Uranium transfer phenomena in rock matrix: petrophysical and geochemical study of El Berrocal experimental site, Spain

The role played by the petrophysical characteristics of the rock matrix in the radioelement transfer phenomena through the geosphere is considered. The aim of this paper is to correlate information provided by the microcrack network, mineralogy and U-micromapping studies which can be used to quantify the extent of radioelement migration/retention in the granite. This study is part of an interdisciplinary research project on the El Berrocal site (Spain), which forms part of the R & D Programme “Management and Disposal of Radioactive Waste” of the Commission of the European Communities.The experimental procedure combines complementary microscopic techniques: polarizing light, fluorescence, confocal laser scanning, acoustic, scanning electron microscopy and uranium-induced fission-track micromapping. All of these techniques are applied for quantifying the rock matrix characteristics.Data on preferential fissure zones in relation to mineralogy, and the correlation between these data and uranium microdistribution are obtained. These results are discussed in terms of radionuclide mobility and can be used, with other information, for evaluating the retardation capacity of the crystalline rock matrix around a high-level radioactive waste repository.