Implementation of cryogenic tender X-ray HR-XANES spectroscopy at the ACT station of the CAT-ACT beamline at the KIT Light Source

The ACT experimental station of the CAT-ACT wiggler beamline at the Karlsruhe Institute of Technology (KIT) Light Source is dedicated to the investigation of radionuclide materials with radioactivities up to 1000000 times the exemption limit by various speciation techniques applying monochromatic X-rays. In this article, the latest technological developments at the ACT station that enable high-resolution X-ray absorption near-edge structure (HR-XANES) spectroscopy for low radionuclide loading samples are highlighted – encompassing the investigation of actinide elements down to 1 p.p.m. concentration – combined with a cryogenic sample environment reducing beam-induced sample alterations. One important part of this development is a versatile gas tight plexiglass encasement ensuring that all beam paths in the five-analyzer-crystal Johann-type X-ray emission spectrometer run within He atmosphere. The setup enables the easy exchange between different experiments (conventional X-ray absorption fine structure, HR-XANES, high-energy or wide-angle X-ray scattering, tender to hard X-ray spectroscopy) and opens up the possibility for the investigation of environmental samples, such as specimens containing transuranium elements from contaminated land sites or samples from sorption and diffusion experiments to mimic the far field of a breached nuclear waste repository.

Slip tendency analysis of major faults in Germany

Natural seismicity and tectonic activity are important processes for the site-selection and for the long-term safety assessment of a nuclear waste repository, as they can influence the integrity of underground structures significantly. Therefore, it is crucial to gain insight into the reactivation potential of faults. The two key factors that control the reactivation potential are (a) the geometry and properties of the fault such as strike direction and friction angle, and (b) the orientations and magnitudes of the recent stress field and future changes to it due to exogenous processes such as glacial loading as well as anthropogenic activities in the subsurface. One measure of the reactivation potential of faults is the ratio of resolved shear stress to normal stresses at the fault surface, which is called slip tendency. However, the available information on fault properties and the stress field in Germany is sparse. Geomechanical numerical modelling can provide a prediction of the required 3D stress tensor in places without stress data. Here, we present slip tendency calculations on major faults based on a 3D geomechanical numerical model of Germany and adjacent regions of the SpannEnD project (Ahlers et al., 2021). Criteria for the selection of faults relevant to the scope of the SpannEnD project were identified and 55 faults within the model area were selected. For the selected faults, simplified geometries were created. For a subset of the selected faults, vertical profiles and seismic sections could be used to generate semi-realistic 3D fault geometries. Slip tendency calculations using the stress tensor from the SpannEnD model were performed for both 3D fault sets. The slip tendencies were calculated without factoring in pore pressure and cohesion, and were normalized to a coefficient of friction of 0.6. The resulting values range mainly between 0 and 1, with 6 % of values larger than 0.4. In general, the observed slip tendency is slightly higher for faults striking in the NW and NNE directions than for faults of other strikes. Normal faults show higher slip tendencies than reverse and strike slip faults for the majority of faults. Seismic events are generally in good agreement with the regions of elevated slip tendencies; however, not all seismicity can be explained through the slip tendency analysis.

Impact of the heterogeneity of the sandy Opalinus clay facies at the Mont Terri underground research laboratory on radionuclide migration

The assessment of the safety of a deep geological repository (DGR) for high-level radioactive wastes over assessment time scales of up to 1 million years requires an in-depth understanding of the multi-scale coupled processes that affect the repository system evolution over time, to reduce uncertainties and conservatism in safety analyses. This is in particular required with respect to the challenges of a comparative assessment of different repository concepts in different host rocks within the process of a site selection for a DGR for heat-generating radioactive wastes in Germany. The collaborative project “Integrity of nuclear waste repository systems – Cross-scale system understanding and analysis (iCross)” conducted jointly by five research centres of the Helmholtz Association and co-funded by the Initiative and Networking Fund of the Helmholtz Association and the Federal Ministry of Education and Research (BMBF) has been initiated with the overall objective to improve the understanding of coupled thermal-hydraulic-mechanical-chemical-(micro)biological (THMCB) processes and to develop simulation tools that enable a holistic close to reality description of the long-term evolution of the repository system. Geological formations, such as those foreseen as potential host rocks for DGRs, and their surroundings are heterogeneous on various length scales ranging from nanometers to kilometers. Therefore, the aim of this work in the context of iCross is to evaluate the effects of mineralogical, geochemical and microstructural heterogeneities of repository host rocks on radionuclide transport in the repository far field, using the sandy facies of the Opalinus clay (SF-OPA) from the Mont Terri underground research laboratory (St. Ursanne, Switzerland) as an example. Here, we address in particular the migration behaviour of Ra-226 as an important radionuclide to be considered in safety cases for deep geological disposal of spent nuclear fuel. To assess the impact of the heterogeneities in SF-OPA on radionuclide transport, a complementary approach combining microstructural characterisation methods, experimental techniques for the determination of transport parameters of the rock matrix and the mobility of Ra-226 with innovative developments in reactive transport modelling on the pore and continuum scales was pursued. One of the results was that although the limited clay content in SF-OPA decreases the total amount of Ra bound to the illite phase, the solid solutions of sulphate and carbonate compensate for this and provide a major fixation mechanism.

From a hard nuclear state towards a soft nuclear repository state – participation, co-designing, learning and reversibility in the site selection process for a nuclear waste repository

Since 2013 the site search for a repository for highly radioactive waste has been taking place in Germany within the framework of a new governance architecture and under new political guidelines. Based on experiences with nuclear politics in the past, Jungk (1977) coined the term hard nuclear state, characterized by decisions made in a top-down manner. The Decide-Announce-Defend (DAD) strategy, which branded the nuclear state at that time, led to conflicts, mistrust of authorities and blockages. In particular, massive resistance developed against the planned final repository site at Gorleben. Nowadays, after more than 60 years deploying nuclear energy, the (energy) political balance of power has fundamentally changed. Parts of the anti-nuclear movement have been integrated into the political party system and have contributed significantly to the nuclear phase-out. In the course of this, the unfinished task of final disposal has been readdressed: with the Repository Site Selection Act (StandAG, 2017), which was passed in 2013 and amended in 2017, an ongoing process of public participation is stated. The site selection process is required to be learning, self-questioning, science-based, reversible, and participatory. The StandAG § 5 not only provides a basis for a fundamental dialogue between the regulator, the operator, and the public, but also for „co-design“ by common citizens. The StandAG considers various elements from different participation-friendly theories of democracy as well as specific governance concepts, which we refer to collectively as the soft nuclear repository state (cf. Brunnengräber, 2021). Its characteristics need to be worked out, as the StandAG only provides some indications, but no criteria, for what good and sufficient participation in the site selection process means and what its conditions for success should be. Based on preliminary considerations on democratic theory and governance aspects (part 1), we present what good participation could mean in the current procedure and what the framework conditions for good participation could be (part 2). Additionally, we present main findings from participatory observations from the ongoing site search process and identify conditions and indications of a successful future participation process based on the ongoing process (part 3). In the résumé, we turn to the question of which of the democracy-theoretical elements of the soft repository state are already recognizable in the present procedure, but also whether the current procedure provides additional indications towards the soft nuclear repository state (part 4).

Improving Participation in the German Search for a Nuclear Waste Repository Site: a WebGIS as a Transdisciplinary Approach to Support Dialogue?

The political and social debate on nuclear energy in Germany has been characterized for many decades by a high potential for conflict and dissatisfaction. In particular, the controversies surrounding the Gorleben salt dome achieved international attention and altered the relationship between the population and political decision makers at the local up to international levels. With the Site Selection Act from 2013 (StandAG, first revision 2017) a new approach was selected in order to find a participative, inclusive and transparent search process for the best possible site of a repository for highly radioactive waste in Germany. In connection with this a self-learning process was proclaimed, based on a white (unprejudiced) map, which aimed to give the general public an active role; however, even the first interim report of the Federal Company for Radioactive Waste Disposal (BGE) and the publication of the multicolored map, in which geologically suitable areas were extensively shown, revealed a massive potential for conflict. Many citizens and activists, who had already protested against the Gorleben salt dome, in this early phase of the process criticized the lack of transparency and opportunities to voice an opinion on possible site regions. In order to counter these criticisms, the possibilities for a web geographic information system (WebGIS) application (interactive map) as an online platform were analyzed (Walkobinger and Tauch, 2018; Brown and Kyttä, 2018). The aim was to virtualy present available geodata (Chwalisz, 2021), which enabled people to contribute to spatial information (geological, superficial) and therefore to achieve an interaction and participation option with respect to the possible site regions. For this, available geodata relevant for the site search process, such as subareas (BGE, 2020), nuclear power stations (active/inactive, research stations etc.), storage facilities (repository, central, intermediate storage etc.), historically relevant sites (sites of protest, uranium-enrichment and preparation plants etc.) and basic data on orientation were used. Based on this, two possibilities for participative interaction were analyzed: (1) the inclusion of spatially located notes that contain own experiences or local knowledge (e.g. reports, concerns, suggestions, own expert opinions) and (2) the initiation of a platform for a spatially located discussion. Against the background of transdisciplinary research, the aim was to evaluate the participative value of this application in an iterative process, in which the research process is supported by an accompanying group from civil society. For this panel we want to present our results from the transdisciplinary research process. In addition to testing the suitability of such a participation mode, we want to analyze where problems arise and which information is necessary or can lead to conflicts (Griffin, 2020). Finally, we want to gain information on how such participation modes influence the quality of the dialogue and how they contribute to an overall perception of a legally acceptable process (Rzeszewski and Kotus, 2019).

Can we safely go to 200 °C? An integrated approach to assessing impacts to the engineered barrier system in a high-temperature repository

This presentation gives on overview of the complex thermo-hydro-mechanical-chemical (THMC) processes occurring during the disposal of heat-producing high-level radioactive waste in geologic repositories. A specific focus is on the role of compacted bentonite, which is commonly used as an engineered backfill material for emplacement tunnels because of its low permeability, high swelling pressure, and radionuclide retention capacity. Laboratory and field tests integrated with THMC modeling have provided an effective way to deepen our understanding of temperature-related perturbations in the engineered barrier system; however, most of this work has been conducted for maximum temperatures around 100 ∘C. In contrast, some international disposal programs have recently started investigations to understand whether local temperatures in the bentonite of up to 200 ∘C could be tolerated with no significant changes to safety relevant properties. Raising the maximum temperature is attractive for economical and safety reasons but faces the challenge of exposing the bentonite to significant temperature increases. Strong thermal gradients may induce complex moisture transport processes while geochemical processes, such as cementation and perhaps also illitization effects may occur, all of which could strongly affect the bentonite and near-field rock properties. Here, we present initial investigations of repository behavior exposed to strongly elevated temperatures. We will start discussing our current knowledge base for temperature effects in repositories exposed to a maximum temperature of 100 ∘C, based on data and related modeling analysis from a large heater experiment conducted for over 18 years in the Grimsel Test Site in Switzerland. We then show results from coupled THMC simulations of a nuclear waste repository in a clay formation exposed to a maximum temperature of 200 ∘C. We also explore preliminary data from a bench-scale laboratory mock-up experiment, which was designed to represent the strong THMC gradients occurring in a “hot” repository, and we finally touch on a full-scale field heater test to be conducted soon in the Grimsel Test Site underground research laboratory in Switzerland (referred to as HotBENT).

Claystone formations in Germany: what we (don't) know about them and how we can change this

Deep geological formations are considered for safe long-term disposal of high-level radioactive waste. Such a repository would be requested to prevent radionuclides from entering the biosphere for a period of 1 million years (StandAG, 2017). Consequently, a holistic characterization including lithological, mineralogical, geochemical, hydrological, structural and geomechanical properties of any potential repository-hosting rock formation is required. Nine claystone formations have been identified as “sub-areas” within the German site-selection procedure (BGE, 2020). The area covered by these formations comprises about half of the total area considered as being qualified for further exploration. However, despite its relevance to act as a geological barrier for, e.g. hydrocarbons or radionuclides, the characterization of clay-rich formations at depths exceeding 300 m in Germany has attained substantially less attention than economically more relevant units hosted by, e.g. sandstones or rock salt, which have been intensively explored. The BGR project BASTION aims at contributing to characterizing these claystone formations and emphasizes properties relevant to host a repository for nuclear waste. Investigations comprise (micro)structural/petrographic, mineralogical, geochemical, geophysical, hydraulic and thermomechanical analyses. In project phase I (2013–2019), claystones deposited in Northern Germany during the Lower Cretaceous were studied. These rocks belong to the fourth largest sub-area hosting claystones. Two of the main foci were to explore variations in lithology, mineralogy and geochemistry, and to identify deformation mechanisms (natural and artificial) by microstructural analyses. Although rocks appeared to be quite homogeneous on the 10–100 m scale, the results revealed distinct structural and sedimentary heterogeneities on the meter scale affecting fracture density. Another sub-area located in Southern Germany hosts the Opalinus Clay Formation (OPA). This up to 150 m thick claystone formation was deposited during the Middle Jurassic (Franz and Nitsch, 2009). Owing to its self-sealing capacity and ability to retain fluids, it is supposed to host the nuclear waste repository of Switzerland (Bossart et al., 2017). The OPA is quite well understood in terms of its lithology and (bio)stratigraphy, and there have been mineralogical, hydrological and petrophysical analyses, mostly documented in university theses a few decades old and sometimes difficult to access. However, it is questionable to what extent these investigations reflect the situation at depths relevant for the site-selection procedure. Well-documented data on the OPA and its properties relevant for nuclear waste disposal are available via the Swiss site-selection procedure (Bossart et al., 2017). However, as there remain substantial questions regarding the nature of the German portions of the OPA (e.g. spatial distribution of lithology, mineralogy, microstructures) at depths greater than a few decameters, it is unclear to what degree insights obtained in the Swiss site-selection procedure also account for Germany. Therefore, phase II of BASTION, which began in 2020, aims to use the multidisciplinary approach developed during phase I to characterize properties of the OPA relevant for the save long-term disposal of nuclear waste by identifying and quantifying structural and rheological heterogeneities. This will constitute important input for numerical models in any long-term safety assessment.

An interdisciplinary view of the long-term evolution of repository systems across scales: the iCROSS project

The interdisciplinary project “Integrity of nuclear waste repository systems – Cross-scale system understanding and analysis (iCROSS)” combines research competencies of Helmholtz scientists related to the topics of nuclear, geosciences, biosciences and environmental simulations in collaborations overarching the research fields energy and earth and environment. The focus is to understand and analyze close-to-real long-term evolutionary pathways of radioactive waste repositories across nanoscales to repository scales. The project is subdivided into work packages dealing with laboratory studies, field experiments in underground research laboratories (URLs), advanced modelling studies and the integration and alignment of data and information using virtual reality methods. In this sense, the project structure aims at a holistic view on relevant processes across scales in order to comprehensively simulate potential repository evolutions. Within the multi-barrier system of a repository for heat-generating radioactive waste, a number of complex reactions proceed, including dissolution, redox processes, biochemical reactions, gas evolution and solid/liquid interface and (co)precipitation reactions. At the same time, thermal and external mechanical stress has an impact on the conditions in a deep geological repository. All those processes are highly coupled, with multiple interdependencies on various scales and have a strong impact on radionuclide mobility and retention. In recent years, substantial progress was achieved in describing coupled thermal-hydro-mechanical-chemical-biological (THM/CB) processes in numerical simulations. A realistic and concise description of these coupled processes on different time and spatial scales is, at present, a largely unresolved scientific and computational challenge. The close interaction of experimental and simulation teams aims at a more accurate quantification and assessment of processes and thus, the reduction of uncertainties and of conservative assumptions and eventually to a close-to-real perception of the repository evolution. One focus of iCROSS is directed to relevant processes in a clay rock repository. In this context, the iCROSS team became a full member of the international Mont Terri consortium and worked in close collaboration with international and German institutions in URL projects. Respective experiments specifically deal with coupled processes at the reactive interfaces in a repository near field (e.g. the steel/bentonite and bentonite/concrete interfaces). Within iCROSS, the impact of secondary phase formation on radionuclide transport is investigated. At Mont Terri, experiments are in preparation to study radionuclide transport phenomena in clay rock formations within temperature gradients and in facies exhibiting significant heterogeneities on different scales (nm to cm). Beside those studies, high resolution exploration methods for rock characterization are developed and tested and the effect of temperature and other boundary conditions on the strength, creep properties and healing of faults within Opalinus clay are quantified. Multiphysics models coupled to reactive transport simulation have been further developed and applied to laboratory and field experiments. Results are digitally analyzed and illustrated in a visualization center, in order to enhance the comprehension of coupled processes in repository systems across scales. The present contribution provides an overview on the project and reports selected results. The impact of considering complex coupled processes in repository subsystems for the assessment of the integrity of a given (generic) repository arrangement is discussed.