Rhenium Uptake as Analogue 96Tc by Steel Corrosion Products

Abstract

Static batch experiments were used to examine the sorption of dissolved perrhenate [Re(VII)], as a surrogate for pertechnetate [Tc(VII)], on corrosion products of A-516 carbon steel coupons contacted with synthetic groundwater or dilute water. After 109 days of contact time, the concentration of dissolved Re(VII) in the synthetic groundwater matrix decreased by approximately 26%; the dilute water matrix experienced a 99% decrease in dissolved Re(VII) over the same time period. Bulk x-ray diffraction (XRD) results for the corroded steel coupons showed that the corrosion products consisted primarily of maghemite, lepidocrocite, and goethite. Analyses of the coupons by scanning electron microscopy/energy dispersive spectroscopy (SEM/EDS) indicated that Re was present with the morphologically complex assemblages of Fe oxide/hydroxide corrosion products for samples spiked with the highest dissolved Re(VII) concentration (1.0 mmol/L) used for these experiments. Analyses of corroded steel coupons contacted with solutions containing 1.0 mmol/L Re(VII) by synchrotron-based methods confirmed the presence of Re sorbed with the corrosion product on the steel coupons. Analyses showed that the Re sorbed on these corroded coupons was in the +7 oxidation state, suggesting that the Re(VII) uptake mechanism did not involve reduction of Re to a lower oxidation state, such as +4. The results of our studies using Re(VII) as an analogue for {sup 99}Tc(VII) suggest that {sup 99}Tc(VII) would also be sorbed with steel corrosion products and that the inventory of {sup 99}Tc(VII) released from breached waste packages would be lower than what is now conservatively estimated