M3SF-25LL010302052 - Radionuclide Interaction with Hydrothermally Altered Repository Materials

Abstract

This progress report (Level 3 Milestone Number M3SF-25LL010302052) summarizes research conducted at Lawrence Livermore National Laboratory (LLNL) within the Crystalline Host Rock Properties & Processes - LLNL Number SF-25LL01030205. Observed changes in radionuclide sorption after bentonite/clay heating have implications for radionuclide diffusive transport through engineered barriers and must be considered when designing waste disposal repositories. Recent research performed at Los Alamos National Laboratory (LANL) has provided key insights regarding the hydrothermal alteration behavior of bentonite backfill in the presence of repository materials (steel, concrete, etc.). We are examining how this mineral alteration affects retardation behavior of a suite of radionuclides of interest to repository performance assessment. Sorption experiments and data analysis for 233 U were initiated in FY24 following earlier experiments performed on 243 Am, 90 Sr, 137 Cs. In FY25, we completed the 233 U study and initiated and completed a study of 237 Np sorption. Below, we summarize the results and potential impacts of hydrothermal alteration on radionuclide retardation and assess the importance of this process to radionuclide migration from a GHRDC. We also use statistical tools (i.e. PCA) to help us determine the major drivers in affecting changes in measured Kd values induced by hydrothermal alteration. These experiments also allow us to test the predictive ability of our component additivity approach to surface complexation and ion exchange. Our guiding hypothesis is that a robust surface complexation/ion exchange model and associated database can effectively predict changes in radionuclide sorption behavior resulting from the hydrothermal alteration of mineralogy in a repository near field. In November 2024 the paper “Selenium interaction with iron minerals: Quantitative comparison of sorption and coprecipitation impacts on mobility” was published in Applied Geochemistry. A short update of results to date is presented below. In FY25, we also actively supported the DITUSC project, which is part of the EURADII initiative, as associate partners. We are executing the Migration2025 conference and support associated the NEA-TDB and Thermochimie workshops that will provide critical international engagements and develop consensus and synergy in thermodynamics as it relates to supporting the US nuclear waste repository program.