Humans and Ecosystems Over the Coming Millennia: Overview of a Biosphere Assessment of Radioactive Waste Disposal in Sweden

This is an overview of the strategy used to describe the effects of a potential release from a radioactive waste repository on human exposure and future environments. It introduces a special issue of AMBIO, in which 13 articles show ways of understanding and characterizing the future. The study relies mainly on research performed in the context of a recent safety report concerning a repository for spent nuclear fuel in Sweden (the so-called SR-Site project). The development of a good understanding of on-site processes and acquisition of site-specific data facilitated the development of new approaches for assessment of surface ecosystems. A systematic and scientifically coherent methodology utilizes the understanding of the current spatial and temporal dynamics as an analog for future conditions. We conclude that future ecosystem can be inferred from a few variables and that this multidisciplinary approach is relevant in a much wider context than radioactive waste.     

Land Use and Food Intake of Future Inhabitants: Outlining a Representative Individual of the Most Exposed Group for Dose Assessment

The radiation doses to humans resulting from a potential release of radionuclides from a geological repository for long-lived waste are assessed over tens or even hundreds of thousands of years. Ingestion is expected to be the major exposure pathway, and the group with the highest exposures will be those that consume the most contaminated food. In this paper, we characterize the group of individuals with the highest exposures by considering the physical and biological characteristics of the contaminated area and human requirements for energy and nutrients. We then calculate intake rates based on land-use scenarios drawn from self-sustained communities spanning prehistoric times to an industrial-age agrarian culture. The approach is illustrated by simulating groundwater release of four radionuclides to an expected discharge area. We argue that the derived intake rates may serve as credible bounding cases when projected doses are evaluated for compliance with regulatory criteria.     

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.     

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.     

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.     

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.     

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.     

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.     

Characteristics of dioxins and metals emission from radwaste plasma arc melter system

This study investigated the emission characteristics of PCDD/Fs and the partitioning of three heavy metals (Cd, Hg and Pb) and two radioactive metal surrogates (Co and Cs) in a radwaste plasma arc melter system. Typical mixtures of low-level radioactive wastes were simulated as the trial burn surrogate wastes. The emission of PCDD/Fs and the partitioning of the metals were strongly influenced by the feed waste stream and melter operating temperature, respectively. The emissions of PCDD/Fs, cadmium and lead were greatly enhanced when the polyvinyl chloride was included in the feed waste stream. Most of the nonvolatile cobalt partitioned into the glass. A significant quantity of cesium, cadmium and lead was vaporized during the highest melter temperature test. A lower melter temperature resulted in more cesium, cadmium and lead species remaining in the glass. The results of this study suggest that wet scrubbing as well as a low-temperature two-step fine filtration, or both of them together could not effectively capture the gas-phase or fine particle phase PCDD/Fs and mercury species. In order to effectively treat low-level radioactive waste streams, the tested high-temperature melter should include an adsorption system, which could collect the gas-phase PCDD/Fs and mercury species.     

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.     

Use of tritium to predict soluble pollutants transport in Ebro River waters (Spain)

The Ebro River, in Northeast Spain, discharges into the Mediterranean Sea after flowing through several large cities and agricultural, mining and industrial areas. The Ascó nuclear power plant (NPP) is located in its lower section and comprises two pressurised water reactor units, from which low-level liquid radioactive waste is released to river waters under authority control. Tritium routinely released by the NPP was used as a radiotracer to determine the longitudinal dispersion coefficient and velocity of the river waters. Several field experiments, in co-ordination with the NPP, were carried out during 1991 and 1992. During each field experiment, the flow rate was kept constant by dams located upstream from the NPP. After each tritium release, water was sampled downstream at periodic intervals over several hours and tritium was measured with a low-background liquid scintillation counter. Velocity and dispersion coefficient were determined in river waters for several river discharges using an analytical, box-type and numerical approach to solve the one-dimensional advection-diffusion equation. The set of calibrated parameters was used to predict the displacement and dispersion of soluble pollutants in river waters. Velocity was determined as a function of river discharge and river slope, and dispersion coefficient was determined as a function of distance. Finally, sensitivity of the model predictions was studied and uncertainties of the fitted parameters were estimated.     

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).     

Modelling the fate of sulphur-35 in crops. 2. Development and validation of the CROPS-35 model

Gas-cooled nuclear power plants in the UK release sulphur-35 during their routine operation, which can be readily assimilated by vegetation. It is therefore necessary to be able to model the uptake of such releases in order to quantify any potential contamination of the food chain. A model is described which predicts the concentration of (35)S in crop components following an aerial gaseous release. Following deposition the allocation to crop components is determined by an export function from a labile pool, the leaves, to those components growing most actively post exposure. The growth rates are determined by crop growth data, which is also used to determine the concentration. The loss of activity is controlled by radioactive decay only. The paper describes the calibration and the validation of the model. To improve the model, further experimental work is required particularly on the export kinetics of (35)S. It may be possible to adapt such a modelling approach to the prediction of crop content for gaseous releases of (3)H and (14)C from nuclear facilities.     

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.     

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.     

Evaluation of Parts-per-billion Organic Cylinder Gases for Use as Audits During Hazardous Waste Trial Burn Tests

A repository of 14 gaseous organic compounds at parts-per-billion levels (7-430 ppb) in compressed gas cylinders has been established by the Environmental Protection Agency. This repository was established to provide audit materials for use in conducting performance audits to assess the accuracy and precision of principal organic hazardous constituent (POHC) measurements, especially those performed during hazardous waste trial burn tests. Five- and nine-component mixtures In a balance gas of nitrogen were prepared in aluminum cylinders for use in the performance audit program. The five-component mixtures contain carbon tetrachloride, chloroform, perchloroethylene, vinyl chloride, and benzene. The ninecomponent mixtures contain trichloroethylene, 1,2-dichloroethane, 1,2-dibromoethane, acetonitrile, trichlorofjuoromethane, dichlorodifluoromethane, bromomethane, methyl ethyl ketone and 1,1,1-trichloroethane.

Studies of all 14 gaseous organic compounds were performed to determine the stability of the compounds and the feasibility of using them in performance audits. Results indicate that ail of the 14 compounds were adequately stable to be used as reliable audit materials. Also, the estimation of specific uncertainties associated with the analysis of these audit materials and how those uncertainties are used to assign a total uncertainty to the final analyte concentration for 14 organics Is described.

Subsequent to completion of the stability studies, several performance audits were conducted using the repository gases to assess the accuracy and precision of the volatile organic sampling train (VOST) and bag measurement methods. The audit results indicate that laboratories can use these methods to analyze POHC with accuracy usually to within ± 50 percent of the audit concentrations.     

论江苏省城市放射性废物库的作用

介绍了江苏省城市放射性废物库的建设及其运行对环境的影响，论述了为确保全省核与辐射的安全，省城市放射性废物库发挥的重要作用。     

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.