Evaluation of the corrosion behavior of modern spent nuclear fuels under repository conditions

Abstract. In Germany it is planned to directly dispose spent nuclear fuel (SNF) from nuclear power plants together with other high-level radioactive wastes (HLW) from former SNF reprocessing (e.g., vitrified waste), in a deep geological repository for heat-generating wastes – the siting process for this repository was started in 2017 and is ongoing. Based on several decades of research, development, and demonstration (RD&D) it is generally accepted at the technical and scientific level that direct disposal of HLW and SNF in deep mined geological repositories is the safest and most sustainable option (CEC, 2011; IAEA, 2004). The current efforts to improve the performance and accident tolerance of fuels in nuclear power generation resulted in an increased utilization of a variety of new types of light-water reactor (LWR) fuels such as fuels doped with Cr, Al, and Si. This doping leads to a significant change of the microstructure of the fuel matrix. The corrosion behavior of these types of fuels under conditions relevant to deep geological disposal has hardly been studied so far; however, this is of crucial importance as the development of a robust safety case for deep geological disposal of SNF requires a solid understanding of its dissolution behavior over very long time scales (up to 1 million years). To fill this knowledge gap, additional systematic studies on modern doped UO2 fuels were needed. Corrosion experiments with SNF cannot entirely unravel all of the various concurring effects of the dissolution mechanism due to the chemical and structural complexity of SNF and its high beta and gamma radiation field during the first 1000 years; moreover, technical restrictions only allow a very limited number of experiments. Therefore, within the EU-DisCo project ( https://www.disco-h2020.eu , last access: 11 October 2021), a very ambitious programme of corrosion studies on irradiated Cr and Al / Cr doped fuels was carried out, which was complemented by systematic single-effect dissolution studies (e.g., with respect to doping level, grain size and thermodynamic aspects) performed on carefully prepared and characterized, simplified UO2 -based model materials. Here, we present recent results on the dissolution behavior of tailor-made UO2 model materials in accelerated static batch experiments using H2O2 as simulant for radiolytic oxidants, present in long-term disposal scenarios for SNF in failed container conditions due to the alpha irradiation of water. In these dissolution experiments pure UO2 reference pellets exhibiting different densities and grain sizes, as well as Cr-doped UO2 pellets with various Cr-doping levels, produced using different doping methods having different grain sizes, were used. In addition, Nd-doped and industrially produced Cr- and Cr / Nd -doped UO2 pellets were used to determine the influence of these parameters on the dissolution rates. The dissolution experiments were performed under strictly controlled conditions with respect to exclusion of oxygen, temperature control, and exclusion of light. This bottom-up approach was followed to understand how the addition of Cr-oxide into the fuel matrix affects SNF dissolution behavior under repository relevant conditions. The results of the dissolution experiments performed with real SNF and the model materials obtained by the DisCo partners build the basis for numerical simulations on the dissolution behavior of modern SNF. First results of the data evaluation indicate that the addition of dopants and the consequential modification of the fuel matrix does not lead to a significant change of the dissolution behavior of these fuels under repository relevant conditions compared to standard SNF (i.e. dissolution rates agree within an order of magnitude).