PNNL

Abstract

The behavior of non-pertechnetate (Tc(I)) aqueous species was studied by preparing three portions of dried low-activity waste-glass feed, combining it with either the [fac-Tc(CO)3(OH)]4 “tetramer,” the [fac-Tc(CO)3(OH)(H2O)2] “monohydroxo,” or the [fac-Tc(CO)3Cl3]2- “trichloro,” and then heating samples to 600, 800, and 1000°C. For the feeds and the heat-treated samples, Tc concentrations were measured by liquid scintillation counting (LSC) after NaOH and HNO3 fusion, and the results were used to determine the Tc volatility. For unheated samples and samples heated to 600°C, the redox of the Tc was measured by X-ray absorption near-edge structure (XANES) analysis, while partitioning of Tc in the glass-forming melt was determined by leaching the samples in water and measuring the Tc concentration of the leachate. The current results are discussed in connection with previously reported data for Tc(VII) and Tc(IV) species to rationalize the potential mechanism on how different speciation of Tc affect its retention in glass.