Coupling of Nuclear Waste Form Corrosion and Radionuclide Transports in Presence of Relevant Repository Sediments

Assessments of waste form and disposal options start with the degradation of the waste forms and consequent mobilization of radionuclides. Long-term static tests, single-pass flow-through tests, and the pressurized unsaturated flow test are often employed to study the durability of potential waste forms and to help create models that predict their durability throughout the lifespan of the disposal site. These tests involve the corrosion of the material in the presence of various leachants, with different experimental designs yielding desired information about the behavior of the material. Though these tests have proved instrumental in elucidating various mechanisms responsible for material corrosion, the chemical environment to which the material is subject is often not representative of a potential radioactive waste repository where factors such as pH and leachant composition will be controlled by the near-field environment. Near-field materials include, but are not limited to, the original engineered barriers, their resulting corrosion products, backfill materials, and the natural host rock. For an accurate performance assessment of a nuclear waste repository, realistic waste corrosion experimental data ought to be modeled to allow for a better understanding of waste form corrosion mechanisms and the effect of immediate geochemical environment on these mechanisms. Additionally, the migrationmore » of radionuclides in the resulting chemical environment during and after waste form corrosion must be quantified and mechanisms responsible for migrations understood. The goal of this research was to understand the mechanisms responsible for waste form corrosion in the presence of relevant repository sediments to allow for accurate radionuclide migration quantifications. The rationale for this work is that a better understanding of waste form corrosion in relevant systems will enable increased reliance on waste form performance in repository environments and potentially decrease the need for expensive engineered barriers.Our current work aims are 1) quantifying and understanding the processes associated with glass alteration in contact with Fe-bearing materials; 2) quantifying and understanding the processes associated with glass alteration in presence of MgO (example of engineered barrier used in WIPP); 3) identifying glass alteration suppressants and the processes involved to reach glass alteration suppression; 4) quantifying and understanding the processes associated with Saltstone and Cast Stone (SRS and Hanford cementitious waste forms) in various representative groundwaters; 5) investigating positron annihilation as a new tool for the study of glass alteration; and 6) quantifying and understanding the processes associated with glass alteration under gamma irradiation.« less