To study the dissolution of UOX spent nuclear fuel in a deep geological environment and the fast release of a selection of relevant radionuclides for long-term safety of this high level waste, leaching experiments were performed with spent nuclear fuel samples originating from the pressurized water reactors (PWRs) Tihange 1 and Gösgen with a similar burnup (50 – 55 MWd.kgHM−1) but different irradiation histories. Six experiments were conducted to investigate the effect of two critical parameters: (1) the highly alkaline environment caused by the presence of cementitious materials in the “Supercontainer design”, which is currently the reference design for the long-term management of the high-level nuclear waste forms in Belgium, and (2) the reducing conditions imposed by the presence of hydrogen from the corrosion of iron-based materials present in the engineered barriers. The experiments were performed using autoclaves under pressure from 1 to 40 bar with a pure Ar atmosphere or a mixture of H2/Ar. Divided into two consecutive phases, the total experimental duration was about 1400 days. The Phase I provided mainly information about the fast release of the fission products while the perspective of the Phase II was to study the long-term evolution of the spent fuel matrix. During the leaching experiment, concentrations of a selection of radionuclides (238U, 129I, 137Cs, 90Sr and 99Tc) were monitored in solution and the amounts of Kr and Xe were measured in the gas phase. Based on results of the experiments conducted for up to 40 months (i.e. during Phase I of the experimental program), we observe that there is a continuous release of 137Cs, 90Sr and of the fission gases and a clear impact of the irradiation history on the release of certain fission products
