Evaluating the Impacts of Reactive Gas (Carbon Dioxide and Oxygen) Ingress on Leaching from Cementitious Waste Forms - 17482

Cementitious materials are currently being used as the waste forms for low-activity waste disposal (Saltstone) at the Savannah River Site. In addition, cementitious materials have been selected as the waste form (Cast Stone) for secondary wastes and are being investigated for use for supplemental low-activity waste treatment (Cast Stone) at the Hanford Site. These materials are subjected to numerous aging and degradation phenomena in the disposal environment that potentially impact their long-term durability and performance. One important phenomenon is the ingress of reactive gases (i.e., carbon dioxide and oxygen) that can react with and change the chemistry and pore structure and thus mass transport properties of the waste forms. The reaction of carbon dioxide (i.e., carbonation) reduces the pH of the waste form pore solution impacting the solubility of constituents of potential concern (COPCs). In Cast Stone and Saltstone, the reaction of oxygen (i.e., oxidation) impacts the solubility of redox-sensitive COPCs, notably the technetium-99 (Tc-99) and chromium. The objective of this research is to experimentally characterize the carbonation and oxidation impacts on chemistry and leaching behavior in cementitious waste forms using experimental techniques including United States Environmental Protection Agency (U.S. EPA) Method 1313 and U.S. EPA Method 1315. Results of experimental characterization will be used to parameterize reactive mass transport models to project leaching under a range of field scenarios in future applications. (authors)