DOE OSTI2018
At the Savannah River Site (SRS) low activity salt solution is stabilized via encapsulation within a grout termed salt-stone. Salt-stone is emplaced into large (multi-million liter) concrete storage containers referred to as Salt-stone Disposal Units (SDUs). Technetium-99 (Tc-99) and iodine-129 (I-129) are long-lived radionuclides contained in the low activity salt waste and subsequently incorporated into the grout waste form: both radionuclides are contributors to the potential long-term radiation exposure of the public and environment surrounding the SDUs. With respect to Tc-99, in the reducing, high pH environment within the grout, Tc-99 is expected to be relatively immobile since it exists in a reduced Tc(IV) oxidation state in the form of sparingly soluble hydrated oxides (TcO{sub 2}.xH{sub 2}O) or sulfides (TcS{sub x}). However, in the presence of O{sub 2} (associated with the future infiltration of air or oxygenated ground waters into the salt-stone monolith) it is possible for redox-sensitive Tc(IV) to transition into highly soluble (and mobile) Tc(VII) species, such as pertechnetate (TcO{sub 4}{sup -}), which are more readily transported to the surrounding environment. In contrast, I-129 is highly soluble and its leaching behavior is not anticipated to be significantly impacted by potential changes in redox environment or pH within salt-stone. Traditional approaches to quantifying the leaching behavior of Tc-99 and I-29 from cementitious matrices have involved partitioning experiments using size-reduced (crushed/ground) samples, and determination of the radionuclide fraction immobilized by the cementitious solids. Such experiments create artificially high solid-liquid contact areas that likely result in higher Tc-99 and I-129 leachate concentrations than would be expected for intact, monolithic samples. In the current study a new technique, termed the Dynamic Leaching Method (DLM), is being used to initially investigate the Tc-99 leaching behavior from monolithic salt-stone samples; the system will be used at a later date to evaluate the leaching characteristics of I-129. The data derived using this technique is intended to inform the SRS Salt-stone Disposal Facility (SDF) Performance Assessment (PA) which models the long-term transport of radionuclides from the SDUs to the environment. The DLM utilizes a flexible-wall permeameter to achieve saturated leaching under an elevated hydraulic gradient to simulate and accelerate the future transport of groundwater through salt-stone. Leachates are regularly analyzed with respect to radionuclide concentrations, key constituent concentrations (e.g., Al, Ca, Mg, Na, Si, CO{sub 3}{sup 2-}, NO{sub 2}{sup -}, NO{sub 3}{sup -}, SO{sub 4}{sup 2-}), pH, and reduction potential (E{sub h}) in order to develop an understanding of how chemical changes associated with the pore solution influence grout weathering and radionuclide leaching behavior. This paper provides a brief update with respect to data derived from preliminary Tc-99 leaching evaluations as the DLM was being developed, but the paper is predominantly focused on new sample data in which the DLM technique, pre- and post-DLM salt-stone sample characterization, and leachate analysis protocols have been optimized. (authors)
12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗