Cement as a component of the multi-barrier system: radionuclide retention in cementitious environments

Abstract

Abstract. Safety concepts regarding nuclear waste disposal in underground repositories generally rely on a combination of engineered and geological barriers, which minimize the potential release of radionuclides from the containment-providing rock zone or even their transport into the biosphere. Cementitious materials are used for conditioning of certain nuclear waste types, as components of waste containers and overpacks, as well as being constituents of structural materials at the interface between backfilling and host rock in some repository concepts. For instance, the preferred option for the disposal of high-level waste (HLW) in Belgium is based on the supercontainer design, which consists of a carbon steel overpack surrounded by a thick concrete buffer (Bel et al., 2006). In the event of formation water interacting with cementitious materials, pore water solutions characterized by (highly) alkaline pH conditions will form. These boundary conditions define the chemical response of the radionuclides, but also influence the behaviour of neighbouring components of the multi-barrier system, e.g. bentonitic or argillaceous backfilling and host rock. Hardened cement paste or Sorel cement are considered to be main sorbing materials present in the near field of repositories for low- and intermediate-level waste (L/ILW). Hence, interactions of radionuclides with cementitious materials represent a very important mechanism retarding their mobility and potential migration from the near field (Wieland, 2014; Ochs et al., 2016). While the quantitative description of the sorption processes (usually in terms of sorption coefficients, i.e. Kd values) is a key input in the safety analysis of nuclear waste repositories, detailed mechanistic analysis and understanding of sorption phenomena provide additional scientific arguments and important process understanding, and thus enhance both the quality of safety arguments and the overall confidence in the safety assessment process. Research at KIT-INE dedicated to the interaction of cementitious materials with radionuclides is conducted in the context of different repository concepts, including clay (low- and high-ionic strength conditions), crystalline rock or rock salt. Experimental and theoretical studies are performed within the framework of national (GRAZ, BMWi) and international (CEBAMA and EURAD-CORI, EU Horizon 2020 Programme) projects, extending to third-party projects with several waste management organizations in Europe, e.g. SKB (Sweden), ONDRAF-NIRAS (Belgium) or BGE (Germany). The combination of classical experimental (wet chemistry) methods, advanced spectroscopic techniques and theoretical calculations provides both an accurate quantitative evaluation and a fundamental understanding of the sorption processes. Examples of recent studies at KIT-INE on radionuclide behaviour in cementitious systems in the context of both L/ILW and HLW will be presented in this contribution to explain methodologies, scientific approaches and results. The present state of knowledge as well as main remaining uncertainties affecting the retention processes of radionuclides in cementitious environments under different conditions will be critically discussed, also in view of current international research activities and repository projects.