In the United Kingdom, disposal of radioactive waste may involve packages of grouted waste being placed in a geological disposal facility (GDF) and surrounded by a cementitious backfill. This paper describes modelling that has been carried out to develop an understanding of the possible spatial and temporal evolution within the GDF.

A single waste package is assumed to be filled with an encapsulation grout, placed in an underground vault and surrounded by a cementitious backfill. Groundwater from the host rock flows into the vault and through the backfill. A simplified model system examines the interactions between groundwater, cementitious backfill and grout.

In most cases the model predicts a reduction in the backfill porosity due to precipitation and dissolution reactions, particularly at the upstream edge of the vault. The degree to which this occurs depends on the groundwater composition. The model also predicts precipitation and dissolution reactions would occur in the grouts close to their interface with the backfill, reducing the local porosity significantly which may isolate the grouts from the backfill, so that the pH within the grouts would be unchanged over an extended period.

In the UK, disposal of packaged intermediate-level radioactive waste may involve waste packages being placed in a geological disposal facility (GDF) and surrounded by a cementitious backfill. Cracking of the backfill could occur due to a number of mechanisms, and this could affect the post-closure performance of the GDF.

This work has assessed potential cracking in the backfill during the backfilling and early post-closure period of GDF vaults with an open crown space in a higher strength rock. From the comprehensive range of processes considered, three were identified as potentially causing cracking: (1) during backfilling, plastic settlement under solid horizontal surfaces could result in horizontal gaps beneath waste packages; (2) within days of backfilling, early-age thermal contraction of the backfill could result in primarily vertical cracks; (3) over a number of years, expansion of waste packages could result in large horizontal cracks.

A groundwater flow model incorporating a representation of the cracks was used to calculate flows through a backfilled GDF vault, and through the cracks themselves. Including cracks increased the flow rate significantly. A reactive transport model was used to estimate the evolution of the pore water chemistry as groundwater flows through the cracked backfill. Calcite and brucite were predicted to precipitate, with brucite subsequently dissolving. Calcite build-up could seal some cracks.

Batch experiments have been used to assess the sorption properties of a potential cementitious repository backfill, NRVB (Nirex reference vault backfill), using Eu3+ as a model trivalent radionuclide and ethylenediaminetetraacetic acid (EDTA) as a competing ligand. The NRVB is an effective scavenger of Eu from solution, with most sorbed within minutes onto the crushed material and less than 1.5% remaining in solution after one day (R d values in the range 0.3–2.4 × 104 l kg−1). Ultrafiltration showed that nearly all of this remaining Eu (>94%) is attached to NRVB derived colloids or particulates that are mainly retained by a 100 kDa ultrafilter. High concentrations of EDTA (>0.01 M) reduced the extent of sorption at apparent equilibrium. The addition of EDTA to a pre-equilibrated system of Eu3+ and NRVB resulted in a temporary suspension of some Eu, but this very quickly returned to the solid phase. There is some irreversibility in these systems, with EDTA able to prevent removal of Eu(III) from solution, but unable to bring it back into solution under the same conditions.

Around the world large quantities of sludge wastes derived from nuclear energy production are currently kept in storage facilities. In the UK, the British government has marked sludge removal as a top priority as these facilities are nearing the end of their operational lifetimes. Therefore chemical understanding of uranium uptake in Mg-rich sludge is critical for successful remediation strategies. Previous studies have explored uranium uptake by the calcium carbonate minerals, calcite and aragonite, under conditions applicable to both natural and anthropogenically perturbed systems. However, studies of the uptake by Mg-rich minerals such as brucite [Mg(OH)2], nesquehonite [MgCO3·3H2O] and hydromagnesite [Mg5(CO3)4 (OH)2·4H2O], have not been previously conducted. Such experiments will improve our understanding of the mobility of uranium and other actinides in natural lithologies as well as provide key information applicable to nuclear waste repository strategies involving Mg-rich phases. Experiments with mineral powders were used to determine the partition coefficients (Kd) and coordination of UO22+ during adsorption and co-precipitation with brucite, nesquehonite and hydromagnesite. The Kd values for the selected Mg-rich minerals were comparable or greater than those published for calcium carbonates. Extended X-ray absorption fine structure analysis results showed that the structure of the uranyl-triscarbonato [UO2(CO3)3] species was maintained after surface attachment and that uptake of uranyl ions took place mainly via mineral surface reactions.

This paper gives an overview of the geosphere research studies being undertaken by the Radioactive Waste Management Directorate (RWMD) of the Nuclear Decommissioning Authority. The approach of the RWMD in the current generic phase of the UK managing radioactive waste safely (MRWS) programme is to maintain an understanding of key processes and to carry out research and development into techniques so capability can be built. Although RWMD can demonstrate a general understanding of geosphere processes at this stage in the UK project, it is recognized that this will need to be made site-specific as the MRWS programme progresses. An understanding of the geosphere at the selected site(s) will be an important part of the future programme. Where possible, the RWMD will participate in international studies so that relevant site-based information can be accessed. In this way, the RWMD will be prepared for site-specific work in stage 5 of the MRWS process.

The concept of effective stress is one of the basic tenets of rock mechanics where the stress acting on a rock can be viewed as the total stress minus the pore water pressure. In many materials, including clay-rich rocks, this relationship has been seen to be imperfect and a coefficient (χ) is added to account for the mechanical properties of the clay matrix. Recent experimental results during the flow testing (both gas and water) of several rocks (Callovo-Oxfordian claystone, Opalinus Clay, Boom Clay) and geomaterials (bentonite, kaolinite) has given evidence for stable high pressure differentials. The design of the experiments allows multiple measurements of pore pressure, which commonly shows a complex distribution for several different experimental geometries. The observed stable high pressure differentials and heterogeneous pore pressure distribution makes the describing of stress states in terms of effective stress complex. Highly localized pore pressures can be sustained by argillaceous materials and concepts of evenly distributed pore pressures throughout the sample (i.e. conventional effective stress) do not fit many clay-rich rocks if the complexities observed on the micro-scale are not incorporated, especially when considering the case of gas flow.

The Nuclear Decommissioning Authority Radioactive Waste Management Directorate have been participating in the current DECOVALEX-2011 project (development of coupled models and their validation against experiments) one task of which has been examining the Mont Terri Ventilation Experiment (VE). This long-term (>9 years), field-scale experiment in the Opalinus Clay near the Swiss–French border, was designed to examine the coupled hydraulic–mechanical–chemical changes caused in the tunnel and in the surrounding geology, by the controlled ventilation of a 1.65 m diameter micro-tunnel.

In contrast to many conventional benchmarking and validation exercises, a key aspect of the VE as examined in DECOVALEX was that some data were held back and participants were required to make predictions of key metrics for the future evolution of the system. This paper presents an overview of the work conducted by the Quintessa and University of Edinburgh team including selected results. The coupled models developed include multiphase flow, elastic deformation and chemical processes in both detailed and upscaled geometries.

The models have been able to replicate the observed desaturation around the tunnel, tunnel deformation and localized failure, vapour migration in the tunnel, and the transition in redox conditions into the host rock.

In support of the disposal system safety case for a geological disposal facility (GDF) there is a requirement to consider 'what-if' hypothetical scenarios for post-closure nuclear criticality. Although all such scenarios are considered very unlikely, one 'what-if' scenario is the mobilization of fissile material from a number of waste packages and its slow accumulation within the GDF or the immediate surroundings. Should sufficient fissile material accumulate a quasi-steady-state (QSS) transient criticality event could result. A computer model has been developed to understand the evolution and consequences of such an event.

Since a postulated QSS criticality could persist for many millennia, building confidence in the modelling approach is difficult. However, the Oklo natural reactors in Africa operated for similar durations around two billion years ago, providing a natural analogue for comparison. This paper describes the modelling approach, its application to hypothetical criticality events for a GDF, and how the model can be compared to Oklo. The model results are found to be in agreement with the observational evidence from Oklo, building confidence in the use of the QSS model to simulate postulated post-closure criticality events in GDFs.

The Environment Agency Guidance on Requirements for Authorisation (GRA) of a geological disposal facility (GDF) requires a demonstration that "the possibility of a local accumulation of fissile material such as to produce a neutron chain reaction is not a significant concern." A neutron chain reaction that is just self-sustaining is also known as critical.

Waste packages can be designed to ensure that criticality is impossible during the transport and operational phases of a GDF, and for a significant period post-closure. Over longer times, however, packages may degrade, and groundwater flows could lead to a localized accumulation of fissile material. Hence, even though the initial distribution of materials would need to change substantially, criticality cannot be ruled out completely.

This paper describes how an accumulation of fissile material could, hypothetically, lead to a critical configuration; how such a system could evolve; what the local consequences could be; and how the engineered and geological barriers could be affected. The conclusion from studies to date is that, even for large (and very unlikely) fissile accumulations, the consequences of a post-closure criticality event are not a significant concern.

Understanding flow along fractures and faults is of importance to the performance assessment (PA) of a geological disposal facility (GDF) for radioactive waste. Flow can occur along pre-existing fractures in the host-rock or along fractures created during the construction of the GDF within the excavation damage zone (EDZ). The complex fracture network will have a range of orientations and will exist within a complex stress regime. Critical stress theory suggests that fractures close to localized shear failure are critically stressed and therefore most conductive to fluid flow. Analysis of fault geometry and stress conditions at Sellafield has revealed that no features were found to be, or even close to being, classified as critically stressed, despite some being conductive. In order to understand the underlying reasons why non-critically stressed fractures were conductive a series of laboratory experiments were performed. A bespoke angled shear rig (ASR) was built in order to study the relationship between fluid flow (water and gas) through a fracture surface as a function of normal load. Fluid flow reduced with an increase in normal load, as expected. During unloading considerable hysteresis was seen in flow and shear stress. Fracture flow was only partially recovered for water injection, whereas gas flow increased remarkably during unloading. The ratio of shear stress to normal stress seems to control the fluid flow properties during the unloading stage of the experiment demonstrating its significance in fracture flow. The exhumation of the Sellafield area during the Palaeogene–Neogene resulted in considerable stress relaxation and in fractures becoming non-critically stressed. The hysteresis in shear stress during uplift has resulted in faults remaining, or becoming, conductive. The field and laboratory observations illustrate that understanding the stress-history of a fractured rock mass is essential, and a mere understanding of the current stress regime is insufficient to estimate the flow characteristics of present-day fractures.

Fluid flow through a two-dimensional fracture network has been simulated using a discrete fracture model. The computed field-scale permeabilities were then compared to those obtained using an equivalent continuum approach in which the permeability of each grid block is first obtained by performing fine-scale simulations of flow through the fracture network within that region. In the equivalent continuum simulations, different grid-sizes were used, corresponding to N by N grids with N = 10, 40, 100 and 400. The field-scale permeabilities found from the equivalent continuum simulations were generally within 10% of the values found from the discrete fracture simulations. The discrepancies between the two approaches seemed to be randomly related to the grid size, as no convergence was observed as N increased. An interesting finding was that the equivalent continuum approach gave accurate results in cases where the grid block size was clearly smaller than the 'representative elementary volume'.

An extensive set of porosity, ε, effective diffusion coefficient, D e, and hydraulic conductivity, K, data were obtained from 45 granitic samples from the Bohemian Massif, Czech Republic. The measured dataset can be used to define parameter ranges for data to be used in safety assessment calculations for a deep (>400 m) radioactive waste repository, even though the samples originated from shallower depths (<108 m). The dataset can also be used for other purposes, such as evaluating the migration of contaminants in granitic rock (e.g. from shallow intermediate-level radioactive waste repositories and chemical waste repositories).

Sample relaxation and ageing processes should be taken into account in research otherwise migration parameters might be overestimated in comparisons between lab results and those determined in situ.

An experimental technique has been developed and applied to the problem of determining effective diffusion coefficients and partition coefficients of Sr in low permeability geological materials. This technique, the micro-reactor simulated channel method (MRSC), allows rapid determination of contaminant transport parameters with resulting values comparable to those determined by more traditional methods and also creates product surfaces that are amenable for direct chemical analysis. An attempt to further constrain mass flux was completed by detailed ion beam analysis of polished tuff surfaces (tuff is a polycrystalline polyminerallic aggregate dominated by silicate phases) that had been reacted with Sr solutions at concentrations of 10−5, 10−3 and 10−1 mol l−1. Ion beam analysis was carried out using beams of both protons (using particle induced X-ray emission and elastic backscattering spectrometry or EBS) and alpha-particles (using Rutherford backscattering spectrometry). The ion beam analyses showed that increased solution concentrations resulted in increased surface concentrations and that in the highest concentration experiment, Sr penetrated to at least 4 μm below the primary interface. The Sr surface concentrations determined by EBS were 0.06 (±0.05), 0.87 (±0.30) and 2.40 (±1.0) atomic weight % in the experiments with starting solution concentrations of 10−5, 10−3, and 10−1 mol l−1, respectively.

This paper gives an overview of the Nuclear Decommissioning Authority, Radioactive Waste Management Directorate approach to representing the biosphere in post-closure safety assessment studies. The assessments consider potential releases of radionuclides and chemically toxic substances from a geological disposal facility that may reach the biosphere by transport in groundwater and gas. It gives an outline of the key processes and understanding underpinning the representation of the biosphere and how the biosphere may evolve over the long timescales of relevance to post-closure safety. The current biosphere assessment approach and associated models are supported by research studies and collaboration that ensure they are consistent with international recommendations. Research studies are also commissioned to reduce uncertainty surrounding key contaminants and potential exposure pathways and to help ensure that the approach and models are adaptable and flexible enough to incorporate future developments, as the geological disposal programme moves towards site selection.

Higher activity radioactive wastes remain hazardous for extremely long timescales, of up to hundreds of thousands of years. Disposing of such wastes deep underground presents the internationally accepted best solution for isolating them from the surface environment on associated timescales. Geological disposal programmes need to assess potential releases from such facilities on long timescales to inform siting and design decisions and to help build confidence that they will provide an adequate degree of safety. Assessments of geological disposal include consideration of the wastes, the engineered facility, the host geology and the surface and near-surface environment including the biosphere. This paper presents an overview of recent post-closure biosphere assessment studies undertaken in support of the Nuclear Decommissioning Authority Radioactive Waste Management Directorate disposal system safety case for geological disposal of the United Kingdom's higher activity radioactive wastes. Recent biosphere studies have included: (1) ensuring that the United Kingdom's approach to consideration of the biosphere in safety case studies continues to be fit for purpose, irrespective of which site or sites are considered in the United Kingdom's geological disposal programme; (2) updating projections of global climate and sea level, together with consideration of the potential importance of transitions between climate states; (3) considering geosphere–biosphere interface issues and their representation, including redox modelling and catchment-scale hydrological modelling; and (4) identifying key radionuclides and developing a series of reports describing their behaviour in the biosphere together with an evaluation of associated implications for post-closure assessment calculations.

Consideration of the biosphere is important in the post-closure safety assessment of a geological disposal facility (GDF) as the biosphere acts as the receptor for any contaminants that may be released from the geosphere. Considerable uncertainty exists in the characteristics of the biosphere at times in the far future when any contaminant releases from a GDF would reach the accessible environment. These uncertainties include human behaviour, affecting environmental change as well as exposure modes.

A number of critical scientific issues have been identified through the practical application of the International Atomic Energy Agency reference biosphere approach within both site generic and site specific repository assessment projects. These issues are being addressed through an international collaboration programme, BIOPROTA. The purpose of this paper is to describe the BIOPROTA programme, its objectives and typical working method. The approach is illustrated with examples from the recent work programme including model intercomparison studies for the radionuclides 36Cl and 79Se.

Carbon-14 has been identified as one of the more significant radionuclides in solid radioactive wastes in a repository, due to the potential radiological impact arising if 14C were to be released and enter the biosphere. However, the assessment of radiation doses is complicated by the major role of carbon in biological processes, and this has tended to lead to the adoption of a cautious assessment approach.

An international comparison of five models used to predict uptake of 14C to agricultural crops has been undertaken, within the BIOPROTA framework. Processes investigated include conversion of 14C-labelled CH4 into CO2 in soils, carbon accumulation in and release from soil carbon pools, gaseous emanation to, and dispersion from, the plant canopy atmosphere and, incorporation into plants by photosynthesis.

For a unit rate of entry of 14C to soil, modelled activity concentrations in cereal crops differ by three to five orders of magnitude. This reflects, in part, differing assumptions for mixing and dispersion of air above the soil surface and within the crop canopy layer. For a unit activity concentration of 14C in air, the modelled uptake to cereal crops converges significantly. Following an assumed irrigation of crops with groundwater containing unit activity of 14C, the predicted uptake to crops varied by two to four orders of magnitude, again largely dominated by assumptions regarding the canopy atmosphere. In all cases, there is some convergence in model predictions as field size increases.

A continuing programme of field research is being undertaken in parallel with the assessment work.

The role of the microbial activity on the transport properties of host rocks for geological repositories, particularly in the far-field, is an area of active research. This paper compares results from experiments investigating changes in transport properties caused by microbial activity in sedimentary rocks in Japan (mudstones) and sandstone (UK).

These experiments show that both Pseudomonas denitrificans and Pseudomonas aeruginosa appear to survive and thrive in pressurized flow-through column experiments which utilized host rock materials of relevance to radioactive waste disposal. Indeed, despite there being a difference in the numbers of organisms introduced into both biotic experiments, numbers appear to stabilize at ∼105 ml−1 at their completion. Post experimental imaging has highlighted the distinct differences in biofilm morphology, for the chosen rock types and bacteria, with Pseudomonas aeruginosa derived biofilms completely covering the surface of the sandstone host and Pseudomonas denitrificans forming biofilament structures. Regardless of substrate host or choice of microbe, microbial activity results in measurable changes in permeability. Such activity appears to influence changes in fluid flow and suggests that the transport of radionuclides through the far-field will be complicated by the presence of microbes.

Microbial metabolism has the potential to control the biogeochemistry of redox-active radionuclides in a range of geodisposal scenarios. In this study, sediments from a high pH lime workings site were incubated under carefully controlled anaerobic conditions, at a range of alkali pH values with added electron donors and electron acceptors, to explore the limits and rates of bioreduction in a sediment system analogous to intermediate-level nuclear waste. There was a clear succession in the utilization of electron acceptors (in the order nitrate > Fe(III)-citrate > Fe(III) oxyhydroxide > sulfate), in accordance with calculated free energy yields and Eh values over the pH range 10–12. The rate and extent of bioreduction decreased at higher pH, with an upper limit for the processes studied at pH 12. The biochemical limits for such processes are discussed, alongside the potential impact of such forms of microbial metabolism on the solubility of a range of redox active radionuclides that will feature heavily in the safety case for the geological disposal of intermediate-level nuclear waste.

Gases will be generated in waste packages during their transport to a geological disposal facility (GDF), this generation will continue during GDF operations and after GDF closure. The range of gases produced will include flammable, radioactive and chemotoxic species. These must be managed to ensure safety during transport and operations, and the post-closure consequences need to be understood. The two primary post-closure gas issues for a GDF are the need for the system pressure to remain below a value at which irreversible damage to the engineered barrier system and host geology could occur, and the need to ensure that any flux of gas (in particular gaseous radionuclides) to the biosphere does not result in unacceptable risk. This paper provides an overview of the research of the Nuclear Decommissioning Authority, Radioactive Waste Management Directorate into gas generation and its migration from a GDF.