Radionuclide geochemistry: solubility and thermodynamics in an HLW repository

Deep geological disposal is the internationally favoured option to isolate high-level nuclear waste (HLW) from the biosphere and to minimise the potential radiological risk for future generations. Potentially contacting aqueous solutions such as groundwater may, however, lead to the corrosion of the solid casks containing the nuclear waste, and the formation of aqueous radionuclide systems in the near-field of the emplacement rooms. As dissolved species, radionuclides can in principle further migrate into the far-field and finally reach the biosphere on medium and long timescales. Like all chemical species, the radionuclides are subject to fundamental (geo)chemical laws. Relevant reactions that control retention and release, and hence, the migration behaviour and fate of radionuclides in a repository, are solubility equilibria, formation of soluble complexes, redox reactions, sorption on and incorporation into mineral surfaces, transport phenomena etc. These processes depend directly on the (geo)chemical boundary conditions, and, consequently, can differ greatly for various host rock systems such as clay rock, rock salt, and crystalline rock. Many of the radionuclides in HLW are heavy metals that are sparingly soluble under various repository-relevant conditions, e.g. actinides, lanthanides, transition metals, so that only partial dissolution (mobilisation) from the solid waste matrices is expected. This underlines the importance of evaluating the radionuclide solubility within a geochemically based safety assessment for repositories as it provides reliable upper-limit concentrations of the mobile, potentially migrating radionuclide fraction in the near-field. In this contribution, we discuss relevant aspects related to the topic radionuclide solubility and thermodynamics in a HLW repository. This includes a summary of recent laboratory studies on the solubility behaviour and speciation of key radionuclides in repository-relevant solutions, which are an important basis for obtaining (geo)chemical information and models, and the corresponding fundamental thermodynamic constants on aqueous radionuclide systems. National and international thermodynamic database projects, where quality-assured thermodynamic data (solubility products, complex formation constants, and ion-interaction parameters) are evaluated and compiled, e.g. the Nuclear Energy Agency Thermochemical Database (http://www.oecd-nea.org, last access: 1 November 2021) or the Thermodynamic Reference Database (http://www.thereda.de, last access: 1 November 2021), are highlighted and the main remaining uncertainties discussed. The experimental information and the quantitative thermodynamic data are applied within a generic case study to demonstrate the impact of different geochemical solution conditions representing different host rock systems considered as HLW repositories in Germany on the solubility and speciation of selected radionuclides.

Experimental and Numerical Study on Hydromechanical Coupled Deformation Behavior of Beishan Granite considering Permeability Evolution

Beishan granite is a potential host rock for a high-level radioactive waste (HLW) repository in China. Understanding the hydromechanical (HM) behavior and permeability evolution of Beishan granite is important for the HLW repository safety. Therefore, the granite of Beishan in Gansu province was studied. HM coupled tests are carried out on Beishan granite under different pore pressures. The results show that the initial pressure difference has little influence on permeability measurement before dilatancy starts. However, after onset of dilatancy, the permeability increases with the increasing initial pressure difference. The initial permeability of Beishan granite is about 10−18 m2 under a confining pressure of 20 MPa. In the initial loading phase, the permeability shows a relatively large reduction. Then, the permeability almost keeps constant until dilatancy starts. From dilatancy point to peak stress, permeability increases linearly with volumetric strain. The proposed permeability evolution rule is implemented into a numerical code to perform HM coupled simulations. The simulation results show that the damaged zone first appears at the model boundary and then extends to the inside, forming high volumetric strain areas. And it provides seepage channels for fluid flow. The macroscopic fracture patterns indicate that pore pressure accelerates rock degradation during HM coupling. The obtained results help to understand the damage mechanisms of granite caused by pore pressures and are of great importance for the safety of a HLW repository.

Creating a generic model of a high level waste (HLW) repository in crystalline rock and determining hydraulic parameters to investigate minimum requirements to the host rock for a safe storage location according to national German law

<p>Nuclear power generation became popular in the 1950s in industrialised countries as an alternative to fossil energy sources to provide large amounts of low cost, low carbon energy. Currently 6% of the world’s energy supply is produced in 451 nuclear reactors across 30 countries. However, nuclear power generation has a serious disadvantage and hidden cost: the accumulation and disposal of spent fuel or high level nuclear waste (HLW) - notably highly radioactive nuclear fission products and the absence of suitable long-term storage solutions, threatening livestock and the environment. Sustainable disposal of HLW holds many challenges: fluid and heat transfer may induce strongly coupled undesirable thermal, hydrological, mechanical and chemical processes.</p><p>A crystalline rock repository construction license has been accomplished by Finland in 2015 for the first long-term HLW repository worldwide. In Germany, a consortium of federal offices is exploring the opportunity of establishing a long-term underground repository in crystalline rock for HLW as an alternative to potential repositories in salt rock and mudrock.</p><p>The aim of this research is to de-risk hypothetical storage solutions for long-term HLW repositories in Germany in crystalline rock. As no geological site must be alluded to for legal reasons during the repository site investigation process at the time being, flow is modelled for a generic fractured rock site based on academic studies of crystalline rock. An inverse problem approach is applied to investigate hydraulic site requirements for the long-term storage of HLW and provide footing for the analysis of coupled thermal, hydrological, mechanical and chemical processes. </p><p>This work demonstrates progress towards finding a long-term storage solution for HLW in Germany through evaluating hydrological processes in a generic crystalline rock site. Through Oda analysis and simulating steady-state flow and particle tracking in a synthetic discrete fracture network (DFN), degrees of fracture connectivity and hydraulic conductivity of fractures have been identified for the hydraulic (boundary) conditions in a repository in crystalline rock.</p>