A science-based approach to understanding waste form durability in open and closed nuclear fuel cycles

There are two compelling reasons for understanding source term and near-field processes in a radioactive waste geologic repository. First, almost all of the radioactivity is initially in the waste form, mainly in the spent nuclear fuel (SNF) or nuclear waste glass. Second, over long periods, after the engineered barriers are degraded, the waste form is a primary control on the release of radioactivity. Thus, it is essential to know the physical and chemical state of the waste form after hundreds of thousands of years. The United States Department of Energy’s Yucca Mountain Repository Program has initiated a long-term program to develop a basic understanding of the fundamental mechanisms of radionuclide release and a quantification of the release as repository conditions evolve over time. Specifically, the research program addresses four critical areas: (a) SNF dissolution mechanisms and rates; (b) formation and properties of U ⁶⁺-secondary phases; (c) waste form–waste package interactions in the near-field; and (d) integration of in-package chemical and physical processes. The ultimate goal is to integrate the scientific results into a larger scale model of source term and near-field processes. This integrated model will be used to provide a basis for understanding the behaviour of the source term over long time periods (greater than 10 ⁵ years). Such a fundamental and integrated experimental and modelling approach to source term processes can also be readily applied to development of advanced waste forms as part of a closed nuclear fuel cycle. Specifically, a fundamental understanding of candidate waste form materials stability in high temperature/high radiation environments and near-field geochemical/hydrologic processes could enable development of advanced waste forms ‘tailored’ to specific geologic settings.