The degradation of strong basic anion exchange resins and mixed-bed ion-exchange resins: Effect of degradation products on radionuclide speciation

The most important water-soluble products of the radiolytic degradation of anion exchange resins in a cementitious environment are ammonia and methylamines. These ligands do not form complexes with most radionuclides. Exceptions are Ni, Ag, and Pd, which form strong complexes with amines. Other degradation products of anion and mixed-bed ion-exchange resins are of no importance concerning the complexation of trivalent radionuclides. This is shown indirectly by adsorption experiments: The degradation products do not have a significant effect on the adsorption of Eu(III) on calcite. The effect of ammonia and methylamines on the complexation of Ni, Ag, and Pd is investigated by chemical modeling. For Ni and Ag, rather reliable predictions can be made using available thermodynamic data. In the case of Pd, large uncertainties are encountered due to unreliable data and gaps in the set of important species. The system Pd(II)-ammonia-water is explored in detail. Predominant species are inferred by chemical analogy, and their thermodynamic data are estimated. The uncertainty in these estimated and measured but unreliable data is bound by qualitative and quantitative chemical reasoning