Remediation of Technetium in Vadose Zone Sediments Using Ammonia and Hydrogen Sulfide Gases

The feasibility of applying a combination of H2S and NH3 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 H2S or NH3 gas treatment of sediments had little lasting effect. For the combined gas treatment, the H2S gas created reducing conditions at the pore water/mineral interface that pertechnetate was temporarily reduced/precipitated. The NH3 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 TcSx. 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 ( 30%) formed NH4SH 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 concentrationsmore » 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 H2S and NH3 gas treatment of low water content sediments was a robust technology to significantly decrease Tc-99 mobility.« less