In the Swedish KBS-3 repository concept, there is potential for gas to be generated from corrosion of ferrous materials under anoxic conditions, combined with the radioactive decay of the waste and radiolysis of water. A full understanding of the probable behaviour of this gas phase within the engineered barrier system (EBS) is therefore required for performance assessment. We demonstrate key features from gas transport experiments on pre-compacted Mx80 bentonite, under laboratory and field conditions, and discuss their implications in terms of a conceptual model for gas migration behaviour. On both scales, major gas entry is seen to occur close to the sum of the porewater and swelling pressures of the bentonite. In addition, gas pressure at breakthrough is profoundly sensitive to the number and location of available sinks for gas escape. Observations of breakthrough can be explained by the creation of dilatational pathways, resulting in localized changes in the monitored porewater pressures and total stresses. These pathways are highly unstable, evolving spatially and temporally, and must consequently influence the gas permeability as their distribution/geometry develops.

Such observations are poorly embodied by conventional concepts of two-phase flow, which do not fully represent the key processes involved. Although dilatancy based models provide a better description of these processes, the paucity of data limits further development and validation of these models at present.

The release and migration of gaseous carbon-14 has been identified as a key issue for geological disposal of intermediate-level radioactive wastes in the UK. A significant fraction of carbon-14 in the UK inventory is in irradiated graphite. This paper describes measurements of gaseous carbon-14 releases from irradiated graphite on immersion in alkaline solution. Apparatus has been developed to discriminate organic and inorganic (14CO/14CO2) species in the gas phase by means of selective oxidation and capture. In the initial experiment, small amounts of gaseous carbon-14 (∼4 Bq) were released from 9 g of crushed graphite within a two-week period. In a long-term experiment, cumulative releases were measured periodically from an intact specimen of graphite over a 14 month period. A small fraction of the graphite carbon-14 inventory was released to the gas phase (∼0.004% as CO/CO2 and ∼0.001% associated with organic compounds). A larger quantity of carbon-14, about 0.1%, was released to the solution phase and was thought to be mainly 14CO2, with some possible organic component. In general, the rate of gaseous carbon-14 release decreased with time. The results suggest a small initial release of relatively labile, accessible carbon-14, with longer term release occurring at a much slower rate. Tritium (T) releases were also measured.

To understand the fate and impact of gas produced within a repository for radioactive waste, a series of laboratory and field scale experiments have been performed on the Callovo-Oxfordian claystone (COx), the proposed host rock for the French repository. Results show the movement of gas is through a localized network of pathways, whose properties vary temporarily and spatially within the claystone. Significant evidence exists from detailed laboratory studies for the movement of gas along highly unstable pathways, whose aperture and geometry vary as a function of local stress, gas and porewater pressures. The coupling of these parameters results in the development of significant time-dependent effects, impacting on all aspects of COx behaviour, from gas breakthrough time, to the control of deformation processes. Variations in gas entry, breakthrough and steady-state pressures are indicative of microstructural heterogeneity which exerts an important control on the movement of gas. The localization of gas flow is also evident in preliminary results from the large scale gas injection test (PGZ) where gas flow is initially focussed within the excavation damaged zone (EDZ), which acts as a preferential pathway for gas. Numerical models based on conventional two-phase flow theory are unable to adequately describe the detailed observations from laboratory tests.

The Radioactive Waste Management Directorate of the UK Nuclear Decommissioning Authority has prepared a generic disposal system safety case (DSSC) that covers a range of possible host rock environments. In many of the waste packages considered in the DSSC, the formation of gases by chemical and microbial processes is likely to occur. In order to demonstrate safety, it is necessary to understand the rates at which the gases are generated and their subsequent migration from a disposal facility after closure. This paper is concerned with modelling gas migration through a fractured higher strength host rock. A first set of simulations compares alternative approaches to modelling gas migration through a fractured rock. The approaches differ in their representation of the interaction between the fractures and the rock matrix. As expected, the gross features of many of the simulations are very similar, with a single continuum approach in which the porosity is set equal to either the fracture porosity or the matrix porosity providing the bounding cases. Gas migration is slower for those simulations where the gas can access more of the rock matrix. A final simulation, with a heterogeneous permeability field, is compared with the other simulations, again showing a very similar evolution.

Corrosion, water radiolysis and microbial degradation will result in the generation of gas within repositories designed for the geological disposal of high-level radioactive waste. It is therefore crucial in the design of such facilities that the relevant mechanisms allowing gas migration through repository materials, both engineered barriers and clay-based candidate host rocks, are correctly identified. In Belgium, the Boom Clay represents a candidate host material for which the advective gas breakthrough characteristics and transport properties have been extensively tested and are well defined by numerous studies. The Boom Clay displays a significant capacity for self-sealing and both laboratory and field tests indicate that advective gas transport occurs not by visco-capillary flow, but instead through the formation of pressure-induced dilatant pathways. In this study, we present results from a gas injection test designed to demonstrate the presence of these features by injecting nanoparticulate tracers with helium gas into a sample of Boom Clay. The results provide conclusive evidence for the formation of transient, dilatant gas pathways within a candidate clay-based host rock. This technique provides a novel diagnostic tool for the identification of processes governing multi-phase flow, supporting robust long-term assessments of repository performance.

At the post-closure stage of a geological disposal facility for higher activity radioactive waste several species of gas are likely to be generated in the near-field environment. These could alter the sealing and chemical properties of the bentonite buffer and the local geochemical environment significantly. The authors' attempt to simulate multicomponent gas flow through variably saturated porous media is presented. Governing equations have been developed for a reactive gas-flow model to simulate the thermo-hydro-gas-chemical-mechanical behaviour, with specific reference to the performance of highly compacted bentonite buffer subjected to repository gas generation and migration. The developed equations have been included in the bespoke numerical model COMPASS and some generic simulations are also presented. The model presented extends current capability to assess buffer performance.

The degree of transport and retention of 14CH4 in soil is being investigated in a series of laboratory experiments in preparation for field scale trials at the University of Nottingham. The experimental programme focusses on the behaviour and fate of 14CH4 injected into subsoil and its subsequent incorporation into vegetation under field conditions. Due to restrictions on the use of radioactive tracers in the field, 13CH4 is being used as a surrogate gas which can be handled conveniently in the laboratory and field and which can be measured with high precision using gas chromatography with isotope ratio mass spectrometry. The laboratory data indicate significant differences between the diffusion and oxidation rates of 13CH4 in re-packed and undisturbed soil columns, with both rates appearing to be significantly lower in undisturbed soils. Data from both laboratory and field experiments will be used to inform the development of a model of 14CH4 migration and its fate in the biosphere above a geological disposal facility.

A new data analysis toolkit which is suitable for the analysis of large-scale, long-term datasets and the phenomenon/anomalies they represent is described. The toolkit aims to expose and quantify scientific information in a number of forms contained within a time-series based dataset in a quantitative and rigorous manner, reducing the subjectivity of observations made, thereby supporting the scientific observer. The features contained within the toolkit include the ability to handle non-uniform datasets, time-series component determination, frequency component determination, feature/event detection and characterization/parameterization of local behaviours. An application is presented of a case study dataset arising from the 'Lasgit' experiment.

Understanding the behaviour of gas in a geological disposal facility (GDF) is an essential component of analysing the facility evolution and long-term (post-closure) safety performance. This includes the impacts of gas on the physico-chemical evolution of the GDF, and the release and migration of radionuclides in water and gas.

The Nuclear Decommissioning Authority Radioactive Waste Management Directorate is participating in the EC FORGE (fate of repository gases) project (www.forgeproject.org) and conducting independent research. Key research themes are modelling the impacts of different host rocks on facility evolution including coupled processes, and upscaling the effects of small scale features that can significantly influence the evolution of the whole facility.

Recent code developments have enabled coupled processes to be represented more realistically in models. This has significantly advanced understanding of facility evolution, as discussed in this paper, and will improve future assessment models. There is potential to further improve approaches to upscaling the effects of small scale features on strongly coupled processes, within the context of the EC FORGE project.

In the UK, radioactive wastes currently planned for disposal in a geological disposal facility (GDF) are intermediate-level waste, some low-level waste and high-level waste. Disposal of other materials, including spent fuel, separated uranium and separated plutonium are also included in the planning of a GDF, if such materials are classified as wastes in the future. This paper gives an overview of the radionuclide behaviour research studies of the Nuclear Decommissioning Authority Radioactive Waste Management Directorate (NDA RWMD). The NDA RWMD's current understanding of the processes that control radionuclide behaviour in groundwater and how the engineered and natural barriers in a GDF would contain radionuclides is presented. Areas requiring further work are also identified.

Cellulose degradation products (CDPs) can complex with radioelements causing solubility enhancement and sorption reduction, effects which are detrimental to the containment of radionuclides in the near field of a geological disposal facility and surrounding geosphere. Isosaccharinic acid (ISA) is the principal component of CDPs formed under the alkaline anaerobic conditions of a cement-based near field and appears to be largely responsible for the impact of CDPs on radionuclide solubility and sorption under near-field conditions. However, the situation appears to be more complicated under near-neutral pH geosphere conditions.

A combined experimental and modelling study was undertaken to compare the impact of a CDP leachate to ISA in a simple model ternary sorption system consisting of hematite as a single mineral substrate, thorium as the radioelement and ISA or a CDP leachate as the complexant. Thorium sorbs strongly to hematite. A triple layer model for thorium sorption to hematite was refined to fit to the experimental data in the absence of ISA or CDP leachate; the effect of ISA on thorium sorption was then predicted.

In the presence of CDP leachate, a significant reduction in thorium sorption was observed from pH 6 to 12 in good agreement with model predictions based on a high concentration of ISA. However, only a limited impact of ISA on thorium sorption was observed at pH 6 to 12, in contrast to predictions. The effects of ISA could be accounted for by assuming the formation of a ternary thorium–ISA–surface complex. The model has yet to be extended to the more complex CDP systems. Differences in the thorium speciation in solution due to the formation of a ternary calcium–thorium–ISA complex in the CDP leachate, which is absent from solutions with ISA only, provides the most likely explanation for the differences observed experimentally.

Few studies have sought to investigate the potential for dissolved organic matter (DOM) to bind (and thus potentially transport) radionuclides under the high pH regimes that are expected in cementitious disposal. We have used equilibrium dialysis to investigate uranyl binding to humic acid over a pH range of ∼10 to 13. The experimental results provide evidence that DOM can bind uranyl ions over this pH range, including in the presence of competing ions. There is a general decrease in binding with increasing pH, from ∼80% of total uranyl bound at pH 9.8 to ∼10% at pH 12.9. Modelling of the system with WHAM/Model VII can yield representative results up to pH ∼10.5.

The sorption behaviour of I−, Cs+, Ni2+, Eu3+, Th4+ and UO2+ 2on NRVB (Nirex reference vault backfill) a possible vault backfill, at pH 12.8 was studied. Sorption isotherms generated were compared to results obtained in the presence of cellulose degradation products (CDP). Whereas Cs was not affected by the presence of the organic compounds, a notable reduction in the sorption of Th and Eu to cement was observed. The results also indicated limited removal of Ni from solution (with or without an organic ligand) by sorption, the concentration in solution seemingly being determined solely by solubility processes. In the case of uranium, the presence of CDP increased the sorption to cement by almost one order of magnitude. Further studies into the uptake of CDP by cement are being undertaken to identify the mechanism(s) responsible.

Samples of artificially aged Nirex reference vault backfill (NRVB) were prepared by progressive leaching with deionized water, after which some of the samples underwent hydrothermal treatment. Compared to unaltered NRVB, X-ray diffraction (XRD) and differential scanning calorimetry (DSC) provided evidence for the ageing resulting in alteration of the mineralogy, in particular the absence of portlandite was observed. The specific surface area of NRVB initially increased due to leaching, but then decreased after further leaching.

Sorption distribution ratios (R D values) of uranium(VI), neptunium(IV), tin and zirconium onto aged NRVB samples were measured using the batch sorption technique. For all four elements, there was little difference between R D values for aged NRVB and those for untreated material. The most probable explanation for these findings is that even though the ageing treatments altered the NRVB mineralogy, calcium silicate hydrate (C-S-H) phases are responsible for most of the radionuclide uptake and their transformation to more crystalline forms has little effect on the bulk sorption capacity of the aged material.

The effect of competition from other metal ions on the complexation of Ni with isosaccharinic acid, gluconic acid and picolinic acid, at high pH, is described. The competing metal ions used were divalent Co, trivalent Eu and tetravalent Th. In the majority of cases, competition from these metal ions followed the predicted pattern, with most anomalies seeming to be caused by sorption of Ni to the many different solid phases formed in presence of the competing ions. The Ni solid phase was shown to change with time during the course of the study. No major unexplained competition effects were found.

In the UK, technetium may be disposed of in a high pH, low Eh cementitious repository. In such a scenario, its chemistry would be dominated by TcO4 −, in aerobic conditions and the sparingly soluble TcO2(s) in anaerobic conditions. Repository heterogeneity could mean that both Tc(VII) and Tc(IV) are present simultaneously. The anthropogenic ligands EDTA and picolinic acid are commonly used as decontamination agents and are likely to be present in intermediate-level waste (ILW). They could complex with Tc(IV) increasing its aqueous concentration and mobility in the cement porewaters and beyond. The conditional stability constants (measured in 0.3 mol dm−3 NaOH) for the Tc(IV)–EDTA and Tc(IV)–picolinic acid complexes have been determined to be: βTc(IV)−EDTA = 1.6 × 1026, which corresponds to log β = 25.2±0.6; and βTc(IV)−PA = 8.65 × 1026, which corresponds to log β = 26.9±0.1, respectively.

Several European waste management organizations have started work on creating a technology platform to accelerate the implementation of deep geological disposal of radioactive waste in Europe. There is an increasing consensus in the international community about geological disposal as the preferred option for solving the long-term management of spent fuel, high-level waste and other longlived radioactive wastes. At the same time, European citizens have a widespread desire for a permanent solution for high-level radioactive waste disposal. A majority of European countries with nuclear power have active waste-management programmes, but the current status and the main challenges of those programmes vary. The most advanced waste management programmes in Europe (i.e. those in Sweden, Finland and France) are prepared to start the licensing process of deep geological disposal facilities within the next decade. Despite the differences between the timing and the challenges of the different programmes, there is a joint awareness that cooperation on the scientific, technical and social challenges related to geological disposal is needed, and that it is beneficial for the timely and safe implementation of the first geological disposal facilities. Such a demonstration of a viable solution for the management of high-level radioactive waste will enhance stakeholder confidence in Europe. It is envisaged that a technology platform would enhance European cooperation in this area. The platform will provide a tool for reducing overlapping work, to produce savings in total costs of research and implementation, and to make better use of existing competence and research infrastructures. From 2008, SKB (Sweden) and Posiva (Finland) led the preparation work to set up the implementing geological disposal of radioactive waste technology platform (IGD-TP). Since then other implementers from France, Germany, Switzerland, United Kingdom, Spain and Belgium have joined the project. To date a strategic research agenda for the platform has been prepared and consulted upon, which is now the basis for taking the platform into a deployment phase.

The international long-term cement studies (LCS) project aims to increase the understanding of the behaviour of cement within a radioactive waste disposal system and how hyper-alkaline leachates may interact with host rock. Such an understanding enables confident, robust and safety-relevant statements to be made concerning future system behaviour, irrespective of host rock, engineered barrier system, or waste type. The LCS project involves laboratory experiments, in situ tests and numerical modelling to address these issues. The agencies participating are Nagra (Switzerland), JAEA (Japan), the Nuclear Decommissioning Authority, Radioactive Waste Mangement Directorate (UK), Posiva (Finland) and SKB (Sweden).

Project activities have included: the development of conceptual and theoretical models of cement–rock interaction; testing of numerical models against data from laboratory experiments and industrial and natural analogues of cement–rock reaction; and the synthesis and incorporation of performance assessment (PA) relevant data from analogue studies. Key threads running through these studies include an analysis of issues relating to upscaling of processes and data to the greater temporal and spatial scales relevant to PA, and investigations of modelling the changes in physical properties that accompany geochemical reaction. Here we present examples of the results from model test cases, highlighting the important issues that have arisen.

The implementation of a geological disposal facility requires the demonstration of confidence that such a facility would be safe during both the operational period and in the long-term after the closure of such a facility. The generic environmental safety case described in this paper is the vehicle used to demonstrate an understanding of environmental safety. It will be used to prepare a site-specific environmental safety case in due course. The approach taken will be consistent with a staged development and approval process, as advocated by the environmental regulators.

This paper provides a summary of the research programme undertaken in support of the Low Level Waste Repository's 2011 environmental safety case (ESC). The programme has been developed, based on an understanding of safety issues and the requirements of the ESC. The research requirements to underpin the safety case have been identified by means of an auditable process, and subjected to scrutiny by both the regulators and a peer review group. Key research priorities for the future are identified.