摘要：Abstract The long-term performance, or resistance to elemental release, is the defining characteristic of a nuclear waste form. In the case of multiphase ceramic waste forms, correlating the long-term performance of multiphase ceramic waste forms in the environment to accelerated chemical durability testing in the laboratory is non-trivial owing to their complex microstructures. The fabrication method, which in turn affects the microstructure, is further compounding when comparing multiphase ceramic waste forms. In this work, we propose a “designer waste form” prepared via spark plasma sintering to limit interaction between phases and grain growth during consolidation, leading to monolithic high-density waste forms, which can be used as reference materials for comparing the chemical durability of multiphase waste forms. Designer waste forms containing varying amounts of hollandite in the presence of zirconolite and pyrochlore in a fixed ratio were synthesized. The product consistency test (PCT) and vapor hydration test (VHT) were used to assess the leaching behavior. Samples were unaffected by the VHT after 1500 h. As measured by the PCT, the fractional Cs release decreased as the amount of hollandite increased. Elemental release from the zirconolite and pyrochlore phases did not appear to significantly contribute to the elemental release from the hollandite phase in the designer waste forms.
其他摘要：Abstract The long-term performance, or resistance to elemental release, is the defining characteristic of a nuclear waste form. In the case of multiphase ceramic waste forms, correlating the long-term performance of multiphase ceramic waste forms in the environment to accelerated chemical durability testing in the laboratory is non-trivial owing to their complex microstructures. The fabrication method, which in turn affects the microstructure, is further compounding when comparing multiphase ceramic waste forms. In this work, we propose a “designer waste form” prepared via spark plasma sintering to limit interaction between phases and grain growth during consolidation, leading to monolithic high-density waste forms, which can be used as reference materials for comparing the chemical durability of multiphase waste forms. Designer waste forms containing varying amounts of hollandite in the presence of zirconolite and pyrochlore in a fixed ratio were synthesized. The product consistency test (PCT) and vapor hydration test (VHT) were used to assess the leaching behavior. Samples were unaffected by the VHT after 1500 h. As measured by the PCT, the fractional Cs release decreased as the amount of hollandite increased. Elemental release from the zirconolite and pyrochlore phases did not appear to significantly contribute to the elemental release from the hollandite phase in the designer waste forms.
