Radionuclides and isotopes release of spent fuel matrix. Conceptual and mathematical models of wastes behaviour

We have developed a conceptual and numerical model to calculate release of selected radionuclides from spent fuel under repository condition. This has been done in the framework of the Enresa 2000 performance assessment exercise. The model has been developed based on kinetic mass balance equations in order to study the evolution of the spent fuel water interface as a function of time. Several processes have been kinetically modelled: congruent dissolution, radioactive decay, ingrowth and water turnover in the gap. The precipitation/redissolution of secondary solid phases has been taken into account from a thermodynamic point of view. Both approaches have been coupled and the resulting equations solved for a number of radionuclides in both, a conservative and realistic approach. The results show three distinct groups of radionuclides based on their release behaviour: a first group is composed of radioisotopes of highly insoluble elements (e. g., Pu, Am, Pd) whose concentration in the gap is mainly controlled by their solubility and therefore their evolution is identical in both cases. Secondly, a set of radionuclides from soluble elements under these conditions (e. g., I, Cs, Ra) show concentrations kinetically controlled, decreasing with time following the congruent dissolution trend. Their release concentrations are one order of magnitude larger in the conservative case than in the realistic case. Finally, a third group has been identified (e. g., Se, Th, Cm) where a mixed behaviour takes place: initially their solubility limiting phases control their concentration in the gap but the situation reverts to a kinetic control as the chemical conditions change and the secondary precipitates become totally dissolved. The fluxes of the different radionuclides are also given as an assessment of the source term in the performance assessment. (Author)