Timing of Getter Material Addition in Cementitious Wasteforms

Abstract:

A cementitious waste form, Cast Stone, is being evaluated as a possible supplemental immobilization technology for the Hanford sites’s low activity waste (LAW), which contains radioactive ⁹⁹Tc and ¹²⁹I, as part of the tank waste cleanup mission. Cast Stone is made of a dry blend 47% blast furnace slag, 45% fly ash, and 8% ordinary Portland cement, mixed with a low-activity waste (LAW). To improve the retention of Tc and/or I in Cast Stone, materials with a high affinity for Tc and/or I, termed “getters,” can be added to provide a stable domain for the radionuclides of concern. Previous testing conducted with a variety of getters has identified Tin(II)-Apatite and Silver Exchanged Zeolite as promising candidates for Tc and I, respectively. Investigation into the sequence in which getters are added to Cast Stone was performed following two methods: 1) adding getters to the Cast Stone dry blend, and then mixing with liquid waste, and 2) adding getters to the liquid waste first, followed by addition of the Cast Stone dry blend. Cast Stone monolith samples were prepared with each method and leach tests, following EPA method 1315, were conducted in either distilled water or simulated vadose zone porewater for a period of up to 63 days. The leachate was analyzed for Tc, I, Na, NO₃^-, NO₂^- and Cr with ICP-MS, ICP-OES and ion chromatography and the results indicated that the Cast Stone with getter addition in the dry blend mix (method 1) has lower rates of Tc and I leaching. The mechanisms of radionuclide release from the Cast Stone were also investigated with a variety of solid phase characterization techniques of the monoliths before and after leaching, such as XRD, SEM/EDS, TEM/SAED and other spectroscopic techniques.