Remediation of Technetium in Vadose Zone Sediments Using Ammonia and Hydrogen Sulfide Gases
The feasibility of applying a combination of H 2 S and NH 3 gases for Tc-99 remediation in vadose zone sediments evaluated in laboratory experiments showed a significant mobility decrease from 75 to 95% leachable Tc-99 in untreated sediments to 15 to 48% leachable Tc-99 after gas treatment. Individual H 2 S or NH 3 gas treatment of sediments had little lasting effect. For the combined gas treatment, the H 2 S gas created reducing conditions at the pore water/mineral interface that pertechnetate was temporarily reduced/precipitated. The NH 3 gas created alkaline pore water, which induces some mineral dissolution and subsequent aluminosilicate precipitation as the pH neutralizes, which may coat Tc-99 surface phases and render them less mobile. Surface phase analysis showed Tc-99 associated with weathered basalt clasts and sulfur, possibly from the precipitation of TcS x . Treatment performance was nearly the same at different Tc-99 concentration (34 to 6500 pCi/g), water content (1 to 8%), and gas injection rate, but was sensitive to gas concentrations. Low gas concentrations (< 3%) had insufficient reductant or slower mineral dissolution. High gas concentrations (>30%) formed NH 4 SH precipitate. The 15 - 23% mobile Tc-99 remaining after gas treatment may be caused by limited time for aluminosilicates to precipitate in experiments. Nitrogen species concentrations showed no nitrate or nitrite production and a significant decrease in the sediment microbial population over three months, suggesting nitrification of added ammonia was inhibited. Overall, this study showed that combined H 2 S and NH 3 gas treatment of low water content sediments was a robust technology to significantly decrease Tc-99 mobility.