PNNL

Abstract

Technetium-99 is a radioactive contaminant of high concern at many nuclear waste storage sites. At the U.S. Department of Energy Hanford Site, 99Tc is a component of low-activity waste (LAW) fractions of the nuclear tank waste, which are highly caustic, high ionic strength and have high concentrations of chromate. Removal of 99Tc from LAW streams would greatly benefit the site remediation process. In this study, we investigated the removal of 99Tc(VII), as pertechnetate, from deionized water (DIW) and a LAW simulant using two solid sorbents, tin (II) apatite (Sn-A) and SnCl2 through batch sorption testing and solid phase characterization. Sn-A showed higher levels of removal of Tc from both DIW and LAW simulant compared with the SnCl2. Scanning electron microscopy/energy dispersive X-ray spectroscopy (SEM/XEDS) and X-ray adsorption spectroscopy (XAS) of Sn-A following batch experiments in DIW showed that TcO4- is reduced to Tc(IV) on the Sn-A surface with no incorporation into the lattice structure of Sn-A. The performance of Sn-A in the LAW simulant was lowered due to a combined effect of the high alkalinity, which lead to an increased dissolution of Sn from the Sn-A, and a preference for the reduction of Cr(VI) over Tc(VII).