Waste Repository Research Articles

Investigation of nuclide migration in complex fractures with filling properties

Natural fractures in rock masses commonly feature filling properties, which greatly impact the process of fluid flow and mass transport in the geological disposal of high-level radioactive waste. This study develops a unified pipe-network method to numerically investigate the mechanism of nuclide migration in rough-walled fractures with filling properties based on mobile–immobile models (MIMs). Benchmark tests are conducted against analytical results with respect to the concentration distribution along a single filled fracture to demonstrate the numerical reliability. A case study is performed at the Xinchang (Beishan) selected site as the geological disposal repository for high-level radioactive waste. The migration process of U-238 in a fracture-network system close to a water-conducting zone is investigated with varying fracture-filling properties, fracture-filling proportions in mobile and immobile domains, and hydrodynamic properties. A safety classifier is developed using a support vector machine (SVM) based on 500 sets of numerical results for the concentration evolution of nuclides in complex fractures. This is to effectively evaluate the avoidance distance between the repository and the water-conducting zone with respect to factors including the fracture delay coefficient, the porosity of the fracture mobile domain, the hydraulic gradient, and the equivalent hydraulic aperture.

25 years of cross-fertilization between HADES and Mont Terri rock laboratory

Abstract The collaboration between HADES and the Mont Terri rock laboratory started in 1995, when granite was considered the most suitable host rock for radioactive waste disposal in Switzerland. When an alternative host formation was looked for by NAGRA, the choice of clay as host rock became rapidly clear. It was then decided to build an underground research laboratory in the Opalinus Clay taking advantage of the excavation of a motorway tunnel crossing the Mont Terri anticline. Exchanges of knowledge and experience on the behaviour of argillaceous formations were focused on the feasibility of constructing a safe geological repository for high-level radioactive waste: from excavation and gallery lining techniques to geochemistry, diffusion of radionuclides and coupled thermo-hydro-mechanical processes. The research programme at Mont Terri and the growing numbers of partners from four up to nine countries worldwide led to successive extensions of the galleries. The scientific and technical advances made possible by the collaboration between both laboratories dealt with the development of common methods and joint experimental and modelling efforts. This review article summarizes the main scientific lessons learned during these exchanges, stressing the added values of the knowledge transfer between partners and the overall cross-fertilization between HADES and Mont Terri.

Presence of uranium(V) during uranium(VI) reduction by Desulfosporosinus hippei DSM 8344T

Microbial U(VI) reduction influences uranium mobility in contaminated subsurface environments and can affect the disposal of high-level radioactive waste by transforming the water-soluble U(VI) to less mobile U(IV). The reduction of U(VI) by the sulfate-reducing bacterium Desulfosporosinus hippei DSM 8344T, a close phylogenetic relative to naturally occurring microorganism present in clay rock and bentonite, was investigated. D. hippei DSM 8344T showed a relatively fast removal of uranium from the supernatants in artificial Opalinus Clay pore water, but no removal in 30 mM bicarbonate solution. Combined speciation calculations and luminescence spectroscopic investigations showed the dependence of U(VI) reduction on the initial U(VI) species. Scanning transmission electron microscopy coupled with energy-dispersive X-ray spectroscopy showed uranium-containing aggregates on the cell surface and some membrane vesicles. By combining different spectroscopic techniques, including UV/Vis spectroscopy, as well as uranium M4-edge X-ray absorption near-edge structure recorded in high-energy-resolution fluorescence-detection mode and extended X-ray absorption fine structure analysis, the partial reduction of U(VI) could be verified, whereby the formed U(IV) product has an unknown structure. Furthermore, the U M4 HERFD-XANES showed the presence of U(V) during the process. These findings offer new insights into U(VI) reduction by sulfate-reducing bacteria and contribute to a comprehensive safety concept for a repository for high-level radioactive waste.

Numerical simulation of long-term performance of deep geological repository placement rooms in crystalline and sedimentary rocks

Evaluation of the stability of placement rooms and damages in the geosphere surrounding a deep geological repository (DGR) for high-level nuclear waste are essential components for assessing the overall repository performance. Assessments of the performance of placement rooms for the duration of the regulatory period (typically 1 million years) usually involves simulations using numerical codes capable of modeling coupled thermo-hydro-mechanical (THM) processes induced by different natural and repository-induced perturbations over different time and length scales. The numerical constitutive model used to represent the host medium should be capable of capturing highly nonlinear responses to stress changes, including development of damage and fracturing. In this study, a novel approach for simulation of damage evolution and fracturing around the repository rooms, based on the bonded block model (BBM) devised for analyzing coupled THM processes, is used to perform a study of the long-term geomechanical performance of the Nuclear Waste Management Organization hypothetical DGR configurations in sedimentary and crystalline geological settings. The perturbation effects of different loading conditions, including in-situ stress changes by room excavation, heat generated from the used fuel canisters, and glaciation were analyzed. Each THM analysis was conducted using a 3D continuum numerical code to generate evolving temperature and pore pressure fields in the rock mass. The temperature and pore pressure data were then imported in the 2D BBM model for simulating evolution of damage around the placement rooms. Sensitivity analysis was conducted to investigate the effect of different poro-mechanical parameters, rock mass permeabilities, and different approaches for calibrating the BBM, on predictions of room stability and extent of the excavation damage zone around the placement room. The modeling results indicate that the confinement provided by the bentonite backfill inside the room clearly prevents any unravelling but also limits the extent of the damage to less than 1.6 m into the room walls in any of the analyzed cases considering different loading conditions and uncertainty of the material properties.

Using geophysical log data to predict the fracture density in a claystone host rock for storing high-level nuclear waste

Previously drilled boreholes of a host rock for a potential nuclear waste repository in Hungary revealed a highly fractured claystone rock body. A crucial step for characterizing the hydrodynamic behavior of such a fractured reservoir is fracture identification and accurate calculation of the fracture density. Although acoustic borehole televiewers provide a reliable base for determining the fracture density, older boreholes usually lack such data. However, conventional borehole geophysical measurements are often accessible in such cases. The aim of this study was to identify any correlations between well log data and fracture density. Multiple linear regression analysis was performed on data from two boreholes penetrating the Boda Claystone Formation in southwest Hungary. The upper section of the BAF-4 borehole was used for training, where the fracture density was estimated with a fit of R2 = 0.767. The computed regression function predicted the fracture density with high accuracy in both boreholes for all intervals with typical lithological features. However, in some sections where anomalous well log data indicated changes in the lithology, the prediction accuracy decreased. For example, the function underestimated the fracture density in sandy intervals.

Study on mechanism of effect of flowing water and transferring heat on rock mass temperature in curved fracture

Domestically and internationally, the effect of fracture flowing water and transferring heat on the temperature field of surrounding rock in high-level radioactive waste repositories is a popular research area. Compared with straight fracture flowing water and transferring heat, there are few relevant literatures about the heat transfer of curved fracture water flow. Based on the conceptive model of flowing water and transferring heat in curved fractured rock mass, the influence of flowing water and transferring heat in “I”, “L”, , and shaped fractures on the temperature field of rock mass is calculated by using discrete element program. The findings indicate that: When the model goes into a stable state under four working conditions, the rock on the x = 0–2 m mostly forms a heat transfer path from left to right; the x = 2–4 m primarily forms a heat transfer path from bottom to top, and the temperature gradient reveals that the isotherm of 40–45 °C is highly similar to the shape of four different fractures, indicating that flowing water and transferring heat in the fracture configuration dominate the temperature field of the right side rock mass. The direction of the flowing water and transferring heat of the fracture exerts a dominant effect on the temperature of the rock mass than the length.

Coupled flow and transport modelling of a large-scale in situ migration experiment with 14 C-labelled natural organic matter colloids in Boom Clay

Abstract Twenty-five years ago, a unique long-term and large-scale in situ experiment with 14 C-labelled natural organic matter (NOM) was set up at the HADES underground research facility in Mol (Belgium) to study its migration behaviour. Natural organic matter plays an important role in the mobility of various safety-relevant radionuclides, which is critical in the context of Safety & Performance Assessment (SA/PA) calculations for a possible nuclear waste repository. The objective of this work is to enlarge the confidence in current NOM transport models by validating them with the in situ experiment, which is still continued to this day. Stepwise adding more complexity to the model resulted in a 10-parameter model with which excellent fits to the data are obtained. The model considers two different fractions that are transported by advection and diffusion and can be subject to both irreversible and reversible immobilization processes. The associated fitted parameter values compare well with values determined on small-scale migration experiments. This builds confidence in the NOM transport model, which in turn contributes to the confidence in the outcome of the radionuclide migration calculations performed in the context of SA/PA. These results again highlight the incredible value of such long-running experiments at underground research facilities like HADES.

Evaluation of adsorption behaviour of selenium onto zeolite-based composite barrier material for intermediate deep radioactive waste repository

The radionuclide 79Se is a potential radio-ecological concern due to its long half-lives and its capacity to be readily incorporated into the natural life cycle from radioactive waste repositories. This study aimed to reveal the role of barrier materials including zeolite in the transfer of selenium from radioactive waste repository areas to the biosphere. The interaction between selenium (IV) and the barrier material was evaluated by examining different parameters. In the event of an accident that may occur, the environmental and health risks that the 79Se may pose were evaluated within the scope of possible dose values using a Monte Carlo-based simulation program. As a result, it has been determined that the composite barrier material used plays an important role in preventing the transfer of selenium from the waste storage area to the biosphere. Total carcinogenic risk (TCR) values for ingestion way were found from 4.93E-17 to 4.03E-16 for adults, and from 6.30E-22 to 5.16E-21 for infants. TCR values for dermal way are from 5.28E-21 to 4.32E-20 for adults and range from 7.74E-31 to 6.34E-30 for infants.

Speciation of iron(II/III) at the iron-cement interface: a review

Steel is used as reinforcement in construction materials and it is also an important component of cement-stabilized waste materials to be disposed of in deep geological repositories for radioactive waste. Steel corrosion releases dissolved Fe(II/III) species that can form corrosion products on the steel surface or interact with cementitious materials at the iron-cement interface. The thermodynamically stable Fe species in the given conditions may diffuse further into the adjacent, porous cement matrix and react with individual cement phases. Thus, the retention of Fe(II/III) by the hydrate assemblage of cement paste is an important process affecting the diffusive transport of the aqueous species into the cementitious materials. The diffusion of aqueous Fe(II/III) species from the steel surface into the adjacent cementitious material coupled with the kinetically controlled formation of iron corrosion products, such as by Fe(II) oxidation, decisively determines the extension of the corrosion front. This review summarises the state-of-the art knowledge on the interaction of ferrous and ferric iron with cement phases based on a literature survey and provides new insights and proper perspectives for future study on interaction systems of iron and cement.

Influence of groundwater composition on the reductive precipitation of U(VI) on corroding iron foil surfaces

In order to assess the disposal of spent nuclear fuel in a deep geological nuclear waste repository, the interactions between U(VI) and corroded iron present in the canister material are of importance. It is important to correctly model the fate of the oxidatively dissolved uranium in order to correctly estimate radium releases from the canister in the long term. The release of radionuclides into the environment depends on the dissolution of the UO2 matrix which is dependent on the redox conditions at the fuel surface. The effect of metallic iron on the reduction of U(VI) was studied under anoxic conditions using synthetic groundwaters with different compositions, chosen to investigate the influence of calcium-uranyl-carbonato complexes on the thermodynamics and kinetics of U(VI) reduction on anoxically corroding iron. The corrosion products formed on the iron surface were investigated using SEM-EDS and XPS to identify elemental composition and oxidation states of uranium and iron on the surface. The iron foils efficiently reduced U(VI) to U(IV) causing its significant sorption and precipitation on the iron foil surfaces in the form of U(IV).

Engineered mineralogical interfaces as radionuclide repositories

Effective capture of fugitive actinides and daughter radionuclides constitutes a major remediation challenge at legacy or nuclear accident sites globally. The ability of double-layered, anionic clay minerals known as hydrotalcites (HTC) to contemporaneously sequester a range of contaminants from solution offers a unique remedy. However, HTC do not provide a robust repository for actinide isolation over the long term. In this study, we formed HTC by in-situ precipitation in a barren lixiviant from a uranium mine and thermally transformed the resulting radionuclide-laden, nanoscale HTC. Atomic-scale forensic examination of the amorphized/recrystallised product reveals segregation of U to nanometre-wide mineral interfaces and the local formation of interface-hosted mineral grains. This U-phase is enriched in rare earth elements, a geochemical analogue of actinides such as Np and Pu, and represents a previously unreported radionuclide interfacial segregation. U-rich phases associated with the mineral interfaces record a U concentration factor of ~ 50,000 relative to the original solute demonstrating high extraction and concentration efficiencies. In addition, the co-existing host mineral suite of periclase, spinel-, and olivine-group minerals that equate to a lower mantle, high P–T mineral assemblage have geochemical and geotechnical properties suitable for disposal in a nuclear waste repository. Our results record the efficient sequestering of radionuclides from contaminated water and this novel, broad-spectrum, nanoscale HTC capture and concentration process constitutes a rapid solute decontamination pathway and solids containment option in perpetuity.

Radiolysis effect on Eu(III)-superplasticiser interactions in artificial cement and squeezed cement pore waters.

In the framework of the French deep geological repository for radioactive waste, cement-based materials are envisaged to immobilize radionuclides and/or provide protection from radiation to the environment. Superplasticisers (SPs) are added to these materials to increase their workability. SPs will undergo degradation by coupled radiolytic and hydrolytic effects in the pore solution leading to the formation of potentially complexing degradation products. The objective was to study the potential effect of radiolyzed superplasticizers contained in cement-based materials on radionuclide uptake. The Eu speciation and solubility with organic ligands resulting from the degradation of SPs were studied for the two solutions and the results were compared. Two different SPs were selected, a polycarboxylate ether and a polynapthalene sulfonate. Two different protocols were followed: direct irradiation of the solution containing the superplasticizer, and irradiation of the compacted cement sample followed by extraction of the pore water. Solubility enhancements observed in artificial cement waters are not representative of real cement pore water interactions, in agreement with other studies. Finally, the effects of alkaline hydrolysis and radiolysis of SPs on Eu solubility in pore water are limited.

Rock Mechanics for GeoEnergy Applications

The discipline of rock mechanics, which emerged in the 1960s and 1970s as a distinct scientific subject, is undergoing rapid development, including a significant shift within the traditional civil, transportation, and petroleum fields. This shift leans toward using Earth resources to mitigate adverse climate change and to boost sustainable and renewable energy production. Energy geotechnics, or “GeoEnergy,” focuses on novel geomechanics and geotechnical engineering strategies to meet emerging sustainability market demands. GeoEnergy applications that employ rock mechanics and engineering include geothermal systems, geologic carbon sequestration, underground hydrogen storage, compressed air energy storage, and nuclear waste repositories.

Radionuclide Transport in Channel Networks with Radial Diffusion in the Porous Rock Matrix

Water flows in only a small fraction of the total area of the fractures in fractured rocks. The width of the “channels” is often in the range of centimeters to tens of centimeters. Nuclides can diffuse into and out of the porous rock matrix, which causes them to be significantly retarded compared to the water velocity. In discrete facture networks, diffusion is modeled to be linear and perpendicular to the fracture surface. From a narrow channel, the diffusion cloud would then be as wide as the channel. When the nuclide has propagated farther than the channel width, the diffusion will become essentially radial, which allows the nuclide flux to increase enormously. For the times of interest for a repository for high-level nuclide waste, this will increase nuclide flux into the matrix by tens to thousands of times, and consequently, the nuclide retardation in the flowing water. Radial diffusion was not invoked in the performance assessment of the Forsmark site, which in January 2022 was chosen by the government to locate Sweden’s high-level waste repository. It is shown, using data from this site, that the effect of radial diffusion from the narrow channels considerably increases the retardation of any escaping radionuclides, potentially allowing for the use of thinner copper canisters.

Molecular Dynamics Study of the Beryllium Interaction with C-S-H Phases

Beryllium has applications in fission and fusion reactors, and accordingly it is expected in specific waste streams in nuclear waste repositories. As a part of the multi-barrier system, cementitious materials were shown to strongly sorb beryllium, but the precise uptake mechanisms remain ill-defined. Computational simulations were used to study Be(II) uptake by calcium-silicate-hydrate (C-S-H) phases. Molecular dynamics (MD) calculations show that Be(II) sorbs on (001), (004), and (100) C-S-H surfaces through Ca-bridges and hydrogen bonds. Energy profiles indicate that surface complexes with the highest number of Ca-bridges are the most stable. MD simulations support also Be(II) retention in the C-S-H interlayer. Be(OH)3– is predominantly bound through the exchange of water molecules for deprotonated silanol groups or through multiple Ca-bridges, whereas Be(OH)42– is immobilized in the interlayer midplane. These results provide key inputs to understand the mechanisms driving Be(II) uptake by cementitious materials of relevance in the context of nuclear waste disposal.

TransPyREnd: a code for modelling the transport of radionuclides on geological timescales

Abstract. The German site selection procedure for a high-level nuclear waste repository is entering a stage in which preliminary safety assessments have to be conducted and the release of radionuclides has to be estimated for a large number of potential sites. Here, we present TransPyREnd, a 1D finite-differences code for modeling the transport of radionuclides in the subsurface at geological timescales. The code simulates the processes advection, diffusion, equilibrium sorption, decay of radionuclides, and the build-up of daughter nuclides. We summarize the modeled physical processes, their mathematical description and our numerical approach to solve the governing equations. Finally, two simple tests are shown, one considering diffusion, sorption, and radioactive decay, the other involving diffusion and a radioactive decay chain. In both tests, the code shows good agreement with the reference solutions. Caveats of the model and future additions are discussed.

Confronting the Uncertainties Associated with Long-Time Scales: Analysis of the Modes of Preservation of Memory of Radioactive Waste Burial Sites

The burial of radioactive waste in deep geological repositories has gradually imposed itself since the 1980s in various countries. Considered more stable, safe, and responsible than storage above ground, this solution is seen as a way of keeping the waste out of human reach, and of freeing oneself of the obligation to monitor repositories. However, it soon became clear that the idea of relying on the relative stability of deep geological repositories for the safe disposal of nuclear waste to remove it from the ‘all too human’ risks associated with history’s turbulences, has produced new uncertainties, and raised new questions, given the multi-millennial time scales involved. This article presents a study of the strategies adopted by the actors in charge of radioactive waste management in the face of the temporal constraints imposed by the length of their radioactive life. More specifically, it is intended to question the representations of temporality that allow the designers of these projects to assume their responsibilities by transmitting information and warnings towards to an extremely distant future, to recipients who are not easily representable and for whom they already have a responsibility even though they do not yet exist.

Anisotropic thermal properties of an argillaceous rock under elevated temperatures and external load conditions

The design and long-term safety of geological repositories for high-level radioactive waste (HLW) are dependent on the precise determination of the thermophysical parameters of mudstone. However, there is no relevant literature on the study of the thermophysical properties of Tamusu mudstone, a prospective rock for HLW disposal in China under the complex HLW disposal conditions. Therefore, in this paper, Tamusu mudstone is examined, and its thermophysical properties are tested at temperatures in the range of 25–80 °C with and without the influence of external forces. The thermophysical parameters exhibited significant anisotropic characteristics and were strongly correlated with temperature. The increase in temperature increases the specific heat capacity while lowering the thermal diffusivity. Due to the external force, the anisotropy of the thermophysical parameters decreases, enhancing the ability of the mudstone to transfer thermal energy. Furthermore, the aforementioned phenomena were interpreted from a microscopic perspective. This work can aid in the thermal-related physical phenomena of argillaceous rock and provide key input parameters for both analytical and numerical modeling in the safety assessment of HLW repositories, and other underground facilities at high temperatures.

Development of a Low-pH Concrete Intended for Deep Geological Repository for Radioactive Waste

This article deals with the development of concretes intended to be used as construction materials in the Czech deep repository for radioactive waste. The basic requirements for this concrete are a reduced pH value, which must maintain a constant reduced pH with a value of around 11 in the long term, and mechanical properties comparable to conventional concrete. The raw materials for the production of the proposed low pH concrete come exclusively from the Czech Republic. Material characteristics were measured on fresh mixtures and concrete after 28, 56, and 90 days of curing. In addition to the basic raw materials (aggregate, cement, water), plasticizers, microsilica or slag, and defoaming agents were added to the mixture. The aggregate:binder ratio was approximately 5:1 and the w/c water coefficient was approximately 0.6. The mechanical properties of the final concrete were similar to the reference recipe of conventional concrete (the decrease was less than 10%) and the pH value was even below 11 after 90 days. The issue of a sprayed variant of the LPC mixture was solved within the project.

Modelling simultaneous transport of natural and anthropogenic radionuclides in fractured media — Diffusion into the heterogeneous layered rock matrix for an arbitrary length decay chain

Transport models used for assessing the safety of radioactive waste repositories hosted in fractured bedrock typically do not consider fluxes of naturally occurring radionuclides in the rock and their further migration in flow-bearing fractures. A consistent model that simultaneously describes the transport of radionuclides from both natural and anthropogenic sources has been developed, where decay chains and rock heterogeneity are accounted for. The model accounts for advective flow in the fracture, a decay chain of arbitrary length, and diffusion into and out of the adjacent rock matrix composed of different geological layers. The proposed solution has been verified against a previously published steady state case which considers a homogeneous rock matrix of infinite extent where porewater ingrowth is not accounted for. The model is also applied to some different calculation examples for both transient and limiting steady state cases to represent typical applications of the model as well as to illustrate the effect of different parameters and processes on the transport of natural radionuclides in fractured rocks. This study presents a novel and powerful tool to simulate migration of both anthropogenic and natural radionuclides in and from crystalline rocks to the biosphere. The presented modelling is essential in safety and performance assessment of deep geological disposal of radioactive waste in fractured rocks. The obtained analytical solution can be used to compare relative fluxes of natural and anthropogenic radionuclides, which is useful for validation of the radionuclide transport parameters obtained from field and laboratory experiments.