The safe implementation of geological disposal must be underpinned by sound science. This paper describes the approaches taken by the Nuclear Decommissioning Authority Radioactive Waste Management Directorate, the implementing body for geological disposal in the UK, to build an evidence base of scientific data and understanding which is robust to scrutiny and so provides confidence in the safety of geological disposal.

In the UK, radioactive wastes currently planned for disposal in a geological disposal facility (GDF) include intermediate level waste, some low level waste and high level waste. Disposal of other materials, including spent fuel, uranium and plutonium is also being evaluated to inform the safety case for a GDF, if such materials were to be classified as wastes in the future. This paper describes the generic safety functions through which waste packages can contribute to the safety case of a GDF in the UK. It describes the engineering approach used or envisaged, in the UK and internationally, to ensure that waste packages retain their safety functions for the required periods of time and summarizes the scientific basis underpinning the current understanding of relevant evolution processes. Where gaps in the knowledge exist, the Nuclear Decommissioning Authority Radioactive Waste Management Directorate has identified specific research activities needed to close out such gaps to a level of maturity sufficient for this stage of the disposal programme (generic). This paper describes the latest results from their R&D programme and presents a summary of the research activities planned to meet the current needs of the disposal programme with specific reference to the topics of package evolution and criticality safety.

In the UK, most intermediate level radioactive waste is packaged in stainless steel containers. It is important that containers should maintain their integrity for extended periods of storage prior to final disposal. A prototype 4 metre box fabricated from 304S11 stainless steel was monitored at an inland rural building for over twelve years to gain experience in monitoring environmental conditions and corrosion during storage. A wide range of different types of aerosol particles were observed on the surfaces and in the air. They contained corrosive ions such as chloride, as well as other anions such as sulfate and nitrate. The chloride deposition rate was between 0.1 and 4 μg cm−2 yr−1 depending on the orientation and location of the surface, with a chloride/sulfate ratio ranging from ∼0.3–2. The temperature and relative humidity typically ranged from 0–30°C and 40–90%, respectively. The greatest degree of corrosion developed on the base of the box, which had elevated chloride concentrations (10–140 μg cm−2). However, there was little evidence of corrosion propagation on the surface of the box and no evidence of stress corrosion cracking. The average pit propagation rates on a 316L coupon mounted next to the 4 m box were <1 μm yr−1.

With potential storage of several hundred years underground in a geological disposal facility (GDF) before closure, there is a requirement for radioactive waste packages to perform adequately. Over the past 25 years, cementitous grouts based on blast furnace slag (BFS) and ordinary Portland cement (OPC), have been used in the UK to immobilize intermediate-level waste (ILW), Magnox swarf, and currently such wasteforms are in surface storage awaiting geological disposal. Magnox fuel cladding will slowly corrode when encapsulated in alkaline cementitious grouts to produce hydrogen gas and an expansive corrosion product. Expansive corrosion products may lead to degradation of the wasteform and, if extensive, could affect the container. This study investigated the acute and chronic rates of corrosion of unirradiated Magnox swarf encapsulated in a BFS/OPC grout over a range of temperatures (25, 40, 60, 75 and 90°C) for curing times of up to 2½ years. Structural product degradation starts to develop as the tensile strength of the grout is approached by the expansive forces generated. Deformation of some experimental containers was also noted. An estimate of the time taken for a grouted product to fracture from this study due to the corrosion solely of Magnox is 350 years for storage at 25°C. Although not fully described in this paper, the main cement phases were calcium silicate hydrate, portlandite and gehlenite; the main product of Magnox corrosion was brucite. The curing temperature did not affect the compositions of the Magnox metal, corrosion product or grout.

Separated stocks of UK civil plutonium are currently held as a zero value asset in storage, as there is no final decision about whether they should be treated as a resource for future use as nuclear fuel or as waste. Irrespective of future UK government strategies regarding plutonium, at least a portion of the UK civil plutonium inventory will be designated for geological disposal. In this context, we performed a high-level review of the performance of potential wasteforms for the disposal of separated civil plutonium. The key issues considered were the durability and chemical reactivity of the wasteforms in aqueous environments and the long-term radionuclide release under conditions relevant to geological disposal. The major findings of the review, relevant not only to the situation in the UK but to plutonium disposal in general, are summarized in this paper. The review showed that, in the event of a decision being taken to declare plutonium as a waste for disposal, more systematic studies would be required to constrain the wasteform performance under repository conditions in order to derive realistic source terms for a safety case.

Vitrification is used for the immobilization and conditioning of high-level waste (HLW) arising from the reprocessing of spent nuclear fuel in the UK. Vitrification is also under consideration for the immobilization of certain intermediate-level wastes (ILW), where there may be advantages of volume reduction and removal of uncertainties in long-term waste behaviour, compared to encapsulation in a cement grout. This paper gives an overview of recent work into the chemical durability of UK vitrified wasteforms to inform the technical specification for the disposal facilities for these waste products and the treatment of their long-term behaviour in post-closure performance assessment. This has included: (1) measurements of the initial glass dissolution rates of a simulated HLW Magnox waste glass in a range of groundwater types representative of potential UK host geologies and in simulated high pH near-field porewaters relevant to potential disposal concepts, using Product Consistency Test type-B (PCT-B) at 40°C; and (2) durability testing of three simulant ILW glasses in a saturated calcium hydroxide buffered solution to simulate conditions in cement-based disposal vaults, using PCT-B tests at 50°C.

The experimentally defined initial rate of HLW Magnox waste glass dissolution in a range of simulated groundwater compositions appears to be similar regardless of the ionic strength and major element composition of the solution. The release of caesium from HLW Magnox waste glass appears to be sensitive to solution composition. Caesium is selectively retained in the glass compared to other soluble components in the two low ionic strength solutions, but is released at similar rates to other soluble components in the three groundwaters and Ca(OH)2 solution. Whether this change in caesium retention is an ionic strength effect or is related to changes in the nature of the surface alteration layer formed on the glass, has yet to be established. For HLW Magnox waste glass, dissolution is accelerated at high pH in NaOH solution, however, the presence of calcium acts to mitigate the effects of high pH, at least initially. In Ca(OH)2 solution, calcium is found to react with all the glasses studied leading to the formation of calcium-containing alteration products. The initial dissolution behaviour in Ca(OH)2 solution varies with glass composition and in particular appears to be sensitive to the boron content.

X-ray computed tomography augmented by elemental microanalysis has been used to characterize two drill cores from the Borrowdale Volcanic Group, west Cumbria, UK. Information about the three-dimensional (3D) distribution of mineral phases was obtained non-destructively, and regionsof interest were extracted for thin sectioning and elemental analysis. This revealed the presence of pyrite and other iron- and iron-titanium-bearing minerals. X-ray computed tomography is a very useful tool for 3D visualization, but the limitations of the tomography system used made it difficultto distinguish between regions with similar compositions, such as the different layers within the calcite veins. Methods by which these limitations might be overcome are briefly discussed.

Large volumes of depleted natural and low-enriched uranium exist in the UK waste inventory. This work reports on initial investigations of the leaching performance of candidate glass and cement encapsulation matrices containing UO3 powder as well as that of uranium oxide powders. The surface areas of UO3 powder and the monolith samples of UO3 conditioned in the glass and cement matrices were very different making leaching comparisons difficult. The results showed that for both types of monolith conditioned samples a steady increase of uranium concentration in solution with time was generally not observed. The wt.% of uranium leached from UO3 conditioned in the lead borosilicate glass wasteform was approximately five orders of magnitude less than that leached from UO3 powder. Similarly, the quantities of uranium leached from UO3 conditioned in composite cement made with ordinary Portland cement, and from magnesium phosphate cement, were approximately four and three orders of magnitude, respectively, less than that leached from UO3 powder. The performance of a mixed oxide borosilicate glass wasteform was only slightly better than that of UO3 powder. This work shows that wasteforms based on encapsulation in lead borosilicate glass and cement matrices have the greatest potential for further development.

Intermediate-level wastes (ILW) include substantial quantities of fissile material and controls are required to ensure that its storage, transport and disposal does not present a nuclear criticality hazard. This paper describes the Radioactive Waste Management Directorate's research to develop package fissile material limits (in the form of screening levels) for four different categories of ILW, defined according to uranium or plutonium composition: (1) irradiated natural and slightly enriched uranium (uranium containing up to 1.9 wt.% 235U); (2) low-enriched uranium (uranium containing up to 4 wt.% 235U); (3) high-enriched uranium (uranium containing up to 100 wt.% 235U); and (4) separated plutonium (plutonium containing up to 100 wt.% 239Pu).

The derivation of package screening levels was supported by neutron transport calculations that addressed conditions during waste package transport to a geological disposal facility (GDF), during the GDF operational phase and after GDF closure. The analysis included consideration of combinations of events and processes that could result in fissile material accumulation and concentration after GDF closure, when waste packages have deteriorated sufficiently for fissile material to be mobilized. The results of the calculations have provided input to Radioactive Waste Management Directorate's decision making on setting waste package screening levels.

Intermediate-level radioactive waste is normally encapsulated in cementitious grout. However, for some wastes, grout may not be suitable and polymeric encapsulants are being considered as an alternative. One concern with such encapsulants is their long-term chemical stability and the possibility that release of aggressive degradation products could cause corrosion.

This paper evaluates the potential for three polymeric encapsulants: two epoxy resins (the APS polymer system, (APS) and Alchemix 4760 (ALC)) and a vinyl-ester styrene (VES); to cause internal corrosion of stainless steel waste containers. The corrosion behaviour of stainless steel 316L in contact with each encapsulant was studied in saturated Ca(OH)2 solutions and deionized (DI) water, at 80°C, under non-irradiated and γ-irradiated conditions.

In aerated, alkaline conditions, 316L was resistant to corrosion in all the conditions tested. However, in DI water, the pH fell to values as low as three due to release of acidic species from the polymers. The two epoxy materials (particularly APS) also released significant levels of chloride; VES did not. Chloride release appeared to be increased by γ-irradiation. As a result of the low pH chloride-containing environment created by the APS encapsulant, 316L experienced localized corrosion, whereas coupons in Alchemix 4760 and VES did not. Weight loss measurements correlated with visual observations. γ-irradiation appeared to increase the degree of corrosion.

Geological repository designs employ a multi-barrier approach. The materials, which include wasteforms, backfill and host rock, are typically porous quasi-brittle. Mechanical damage (e.g. nucleation and growth of microcracks) can result in significant changes in permeability. A knowledge of how the permeability is affected is critical to accurate modelling of radionuclide transport. This work proposes a novel 3D lattice-type model for the damage evolution in such materials, referred to as the site-bond model. Its advantages over previous models are that the shape of the lattice cell is physically realistic and that any macroscopic elastic response can be represented, including those of cementitious and geological materials. Damage accumulates as bonds fail upon reaching prescribed failure strengths. These are dictated by a predefined pore size distribution. Concrete is used as a study material. It is demonstrated that the model can predict the macroscopic stress–strain response under unconfined tension and compression with emergent non-linearity due to damage evolution. Ongoing work on the prediction of permeability changes with damage is discussed. This is based on the interaction between the model proposed here and a lattice model of the pore space.

The Nuclear Decommissioning Authority (NDA) is developing a safety case for the long-term management of higher activity wastes. This includes safety assessments of transport to and operations at the repository. One of the main faults and hazards to be considered is waste package response to impact accidents.

The criteria of impact performance for waste packages are based upon activity release of particulates generated from the break up of the waste form during impact. The NDA approach to impact performance is based upon waste package response from finite element modelling in combination with break-up tests.

Previous break up research commissioned by the NDA has concentrated on commercial graphite and glass samples. These extended studies, undertaken by the National Nuclear Laboratory in collaboration with the Department of Aerosol Technology of the Fraunhofer Institute of Toxicology and Experimental Medicine, provide break-up data specific to nuclear facilities and waste materials. These include archived unirrradiated graphite used to construct Magnox reactor cores and reflectors, simulant high level waste glass, selected grout formulations and selected metal-in-grout formulations.

The current route in the UK for the conditioning and immobilization of most intermediate level waste for interim storage and geological disposal is to encapsulate in a cementitious matrix. However, certain waste materials, such as those containing reactive metals (e.g. uranium and aluminium), can corrode in the presence of the highly alkaline water in a cementitious environment. In their initial, undegraded form, polymeric materials can provide the appropriate, unreactive environment needed for the encapsulation of chemically active metals.

This study examines the effects of gamma radiation on the stability of six candidate polymeric encapsulants, including a vinyl ester styrene resin (VES) and five epoxy resin formulations. The polymeric encapsulants were exposed to radiation doses up to 10 MGy using AMEC's cobalt-60 gamma irradiation facility and their radiation and chemical stability characterized by the use of a number of analytical techniques. These included flexural and compressive testing, Fourier transform infrared spectroscopy (FTIR), gel fraction, leach testing and gas evolution. The results show that the most stable resin in terms of radiation resistance and chemical stability was VES. Most of the epoxy resin materials also showed good generic stability, but the FTIR analysis showed the potential for dose-rate effects in one formulation.

The near field, together with the containment and isolation provided by the geosphere, contributes to the long-term safety provided by a geological disposal facility (GDF) after closure. The different engineered barriers can prevent or limit the release of radionuclides and their migration to the undisturbed host rock or geosphere and are expected to fulfil their post-closure safety functions for many thousands to hundreds of thousands of years. They will continue to contribute to containment after their eventual degradation when there would no longer be confidence that they would continue to fulfil all of their safety functions in their totality. By that time, significant radioactive decay will have occurred, substantially reducing the hazard associated with the wastes. Therefore, demonstration of long-term safety requires an understanding of the evolution of the engineered barriers and the consequences for the generic safety functions that the different barriers provide. This paper provides an overview of the research of the Nuclear Decommissioning Authority Radioactive Waste Management Directorate into the evolution of the near field of a GDF.

The heat outputs of higher burn up spent fuels (SF) create problems for disposal in mined repositories, including needs for reduced container loadings and extended pre-disposal cooling. An alternative that is less temperature sensitive is deep borehole disposal (DBD) which offers safety, cost, security and other potential benefits and could be implemented relatively quickly using currently available deep-drilling technology. We have modified our previously proposed version of DBD to be more appropriate for higher burn-up fuels by using smaller (0.36 m diameter) stainless steel containers, a smaller (0.56 m diameter) borehole, and different support matrices. We present the results of new heat-flow modelling for DBD of UO2 and MOX SF with burn ups of 55 and 65 GWd/t showing how temperatures evolve, especially on the outer surface of the containers. Consequences for the performance of the support matrices and the disposal concept are discussed. The thermal modelling indicates DBD is a viable option for higher burn-up SF and could be a practical disposal route for many combinations of fuel types, burn ups, ages and container loadings. Further, the results suggest that DBD of complete fuel assemblies, a desirable option, would be feasible and require much shorter pre-disposal cooling than necessary for disposal in mined repositories.

The Cyprus Natural Analogue Project was carried out due to the requirement to support ongoing laboratory and modelling efforts on the potential reaction of the bentonite buffer with cementitious leachates in the repository engineered barrier system. Although it is known that the higher pH (12.5–13) leachates from ordinary Portland cement will degrade bentonite, it is unclear if this will also be the case for the lower pH (10–11) leachates typical of low alkali cements. Ongoing laboratory and underground rock laboratory programmes, which are currently investigating this, face the obstacle of slow kinetics and the production of short-lived metastable phases, meaning obtaining unambiguous results may take decades. It was therefore decided to implement a focussed natural analogue study on bentonite/low alkali cement leachate reactions to provide indications of the probable long-term reaction products and reaction pathways to provide feedback on the existing short-term investigations noted above and to ascertain if any critical path research and development needs to be instigated now. The results of the analyses presented here, in this short overview of the project, suggest that there has been very limited alkaline groundwater reaction with the bentonite. This is generally supported by both the geomorphological evidence and the natural decay series data which imply groundwater/rock interaction in the last 105 a.

Some of the illustrative concepts for the disposal of intermediate-level waste in a geological disposal facility in the UK employ a cementitious backfill around the waste packages. The concept for higher strength rocks would use a highly alkaline backfill composed of Portland cement (now known as CEM I), hydrated lime and limestone flour, referred to as Nirex reference vault backfill (NRVB).

This paper reports a study of the extensive leaching of cured NRVB in a range of generic leachant compositions (deionized water, 0.1 M and 1 M NaCl solutions) under flow-through conditions using a flexible wall permeameter. The experiments were designed to run for up to two years and to pass at least 1000 volumes of leachant (defined as the cumulative leachate volume produced/NRVB solid specimen volume) through the NRVB samples. Results for the pH evolution profiles of the leachates and the microstructural analysis of the unleached and leached samples are presented.

A range of potential concepts for the geological disposal of high level wastes and spent fuel are being studied and considered in the UK. These include concepts that use bentonite as a buffer material around the waste containers. The bentonite will be required to fulfil certain safety functions, the most important being (1) to protect the waste containers from detrimental thermal, hydraulic, mechanical and chemical processes; and (2) to retard the release of radionuclides from any waste container that fails. The bentonite should have a low permeability and a high sorption capacity.

These safety functions could be challenged by certain features, events and processes (FEPs) that may occur during the evolution of the disposal system. A consideration of how these FEPs may affect the safety functions can be used to identify and to prioritize the important areas for research on bentonite. We identify these important areas (which include hydration of compacted bentonite, illitization and erosion of bentonite), and describe how they are being investigated in current international research on bentonite.

The Äspö EBS Task Force is a collaborative international project designed to carry out research on bentonite. In 2011, the Nuclear Decommissioning Authority Radioactive Waste Management Directorate joined the EBS Task Force partly to benefit from its collective experience. The work of the EBS Task Force is split into two research subareas: (1) the THM subarea, which includes tasks to understand homogenization of bentonite as it resaturates, to investigate the hydraulic interaction between bentonite and fractured rock, and to model in situ experiments; and (2) the THC subarea, which includes tasks to investigate the issue of understanding transport through bentonite, and to model in situ experiments. In particular, the bentonite rock interaction experiment is a large-scale in situ experiment concerned with understanding groundwater exchange across bentonite rock interfaces, with the objective of establishing better understanding of bentonite wetting. In this paper, we describe our work to model the spatial and temporal resaturation of bentonite buffer in a fractured host rock.

A cementitious backfill has been proposed in many geological disposal concepts for intermediate-level waste and low-level waste in the UK and elsewhere. In this paper, the main features of the chemical evolution of backfill and the associated changes in the near-field pH are illustratedwith results from recent work. For example, interaction of the groundwater with calcium silicate hydrate (C-S-H) phases in a backfill is expected to play an important role in the long-term pH-buffering behaviour. Existing experimental data for the dissolution of C-S-H gels are compared withrecent experimental results from leach tests on gels of a lower calcium to silicon ratio (C/S) to provide a consistent set of data across the full C/S range. The results confirm that a congruent dissolution point around C/S = 0.8 is approached by leaching from below (i.e. for gels with 0.29< C/S < 0.8), as well as from above, as reported elsewhere. In addition, a spreadsheet model has been developed to calculate the volume of backfill required at the vault scale to meet specified pH performance criteria. This model includes the major reactions of the backfill with thegroundwater, waste encapsulants and waste components. It can also consider the effects of specific waste packages on local pH performance to allow comparison with the vault-scale calculations.