Advanced waste form and melter development for treatment of troublesome high-level wastes

Abstract

A number of waste components in US defense high level radioactive wastes (HLW) have proven challenging for current Joule heated ceramic melter (JHCM) operations and have limited the ability to increase waste loadings beyond already realized levels. Many of these "troublesome" waste species cause crystallization in the glass melt that can negatively impact product quality or have a deleterious effect on melter processing. Recent efforts at US Department of Energy laboratories have focused on understanding crystallization behavior within HLW glass melts and investigating approaches to mitigate the impacts of crystallization so that increases in waste loading can be realized. Advanced glass formulations have been developed to highlight the unique benefits of next-generation melter technologies such as the Cold Crucible Induction Melter (CCIM). Crystal-tolerant HLW glasses have been investigated to allow sparingly soluble components such as chromium to crystallize in the melter but pass out of the melter before accumulating. The Hanford site AZ-101 tank waste composition represents a waste group that is waste loading limited primarily due to high concentrations of Fe 2 O 3 (also with high Al 2 O 3 concentrations). Systematic glass formulation development utilizing slightly higher process temperatures and higher tolerance to spinel crystals demonstrated that an increase in waste loading of more than 20% could be achieved for this waste composition, and by extension higher loadings for wastes in the same group. An extended duration CCIM melter test was conducted on an AZ-101 waste simulant using the CCIM platform at the Idaho National Laboratory (INL). The melter was continually operated for approximately 80 hours demonstrating that the AZ-101 high waste loading glass composition could be readily processed using the CCIM technology. The resulting glass was close to the targeted composition and exhibited excellent durability in both the as poured state and after being slowly cooled according to the canister centerline cooling (CCC) profile. Glass formulation development was also completed on other Hanford tank wastes that were identified to further challenge waste loading due to the presence of appreciable quantities (>750 g) of plutonium in the waste tanks. In addition to containing appreciable Pu quantities, the C-102 waste tank and the 244-TX waste tank contain high concentrations of aluminum and iron, respectively that will further challenge vitrification processing. Glass formulation testing also demonstrated that high waste loadings could be achieved with these tank compositions using the attributes afforded by the CCIM technology.