Methodology in Corrosion Testing of Container Materials for Radioactive Waste Disposal in a Geological Clay Repository

Abstract

Abstract The current worldwide trend for the final disposal of conditioned high-level, medium-level and long-lived alpha-bearing radioactive waste focuses on deep geological disposal. During the geological disposal, the isolation between the radioactive waste and the environment (biosphere) is realised by the multibarrier principle, which is based on the complementary nature of the various natural and engineered barriers. One of the main engineered barriers is the metallic container (overpack) that encloses the conditioned waste. In Belgium, the Boom Clay sediment is being studied as a potential host rock formation for the final disposal of conditioned high-level radioactive waste (HLW) and spent fuel. Since the mid 1980’s, SCK•CEN has developed an extensive research programme aimed at evaluating the suitability of a wide variety of metallic materials as candidate overpack material for the disposal of HLW. A multiple experimental approach is applied consisting of i) in situ corrosion experiments, ii) electrochemical experiments (cyclic potentiodynamic polarisation measurements and monitoring the evolution of ECORR as a function of time), and iii) immersion experiments. The in situ corrosion experiments were performed in the underground research facility, the High Activity Disposal Experimental Site, or HADES, located in the Boom clay layer at a depth of 225 metres below ground level. These experiments aimed at predicting the long-term corrosion behaviour of various candidate container materials. It was believed that this could be realised by investigating the medium-term interactions between the container materials and the host formation. These experiments resulted in a change of reasoning at the national authorities concerning the choice of over-pack material from the corrosion-allowance material carbon steel towards corrosion-resistant materials such as stainless steels. The main arguments being the severe pitting corrosion during the aerobic period and the large amount of hydrogen gas generated during the subsequent anaerobic period. The in situ corrosion experiments however, did not allow to unequivocally quantify the corrosion of the various investigated candidate overpack materials. The main shortcoming was that they did not allow to experimentally separate the aerobic and anaerobic phase. This resulted in the elaboration of a new laboratory programme. Electrochemical corrosion experiments were designed to investigate the effect of a wide variety of parameters on the localised corrosion behaviour of candidate overpack materials: temperature, SO42−, Cl−, S2O32−, oxygen content (aerobic - anaerobic),… Three characteristic potentials can be derived from the cyclic potentiodynamic polarisation (CPP) curves: i) the open circuit potential, OCP, ii) the critical potential for pit nucleation, ENP, and iii) the protection potential, EPP. Monitoring the open circuit potential as a function of time in clay slurries, representative for the underground environment, provides us with a more reliable value for the corrosion potential, ECORR, under disposal conditions. The long-term corrosion behaviour of the candidate overpack materials can be established by comparing the value of ECORR relative to ENP and EPP (determined from the CPP-curves). The immersion tests were developed to complement the in situ experiments. These experiments aimed at determining the corrosion rate and to identify the corrosion processes that can occur during the aerobic and anaerobic period of the geological disposal. Also, some experiments were elaborated to study the effect of graphite on the corrosion behaviour of the candidate overpack materials.