Hanford tank residual waste – Contaminant source terms and release models

Residual waste is expected to be left in 177 underground storage tanks after closure at the US Department of Energy’s Hanford Site in Washington State, USA. In the long term, the residual wastes may represent a potential source of contamination to the subsurface environment. Residual materials that cannot be completely removed during the tank closure process are being studied to identify and characterize the solid phases and estimate the release of contaminants from these solids to water that might enter the closed tanks in the future. As of the end of 2009, residual waste from five tanks has been evaluated. Residual wastes from adjacent tanks C-202 and C-203 have high U concentrations of 24 and 59 wt.%, respectively, while residual wastes from nearby tanks C-103 and C-106 have low U concentrations of 0.4 and 0.03 wt.%, respectively. Aluminum concentrations are high (8.2–29.1 wt.%) in some tanks (C-103, C-106, and S-112) and relatively low (<1.5 wt.%) in other tanks (C-202 and C-203). Gibbsite is a common mineral in tanks with high Al concentrations, while non-crystalline U–Na–C–O–P ± H phases are common in the U-rich residual wastes from tanks C-202 and C-203. Iron oxides/hydroxides have been identified in all residual waste samples studied to date. Contaminant release from the residual wastes was studied by conducting batch leach tests using distilled deionized water, a Ca(OH)2-saturated solution, or a CaCO3-saturated water. Uranium release concentrations are highly dependent on waste and leachant compositions with dissolved U concentrations one or two orders of magnitude higher in the tests with high U residual wastes, and also higher when leached with the CaCO3-saturated solution than with the Ca(OH)2-saturated solution. Technetium leachability is not as strongly dependent on the concentration of Tc in the waste, and it appears to be slightly more leachable by the Ca(OH)2-saturated solution than by the CaCO3-saturated solution. In general, Tc is much less leachable (<10 wt.% of the available mass in the waste) than previously predicted. This may be due to the coprecipitation of trace concentrations of Tc in relatively insoluble phases such as Fe oxide/hydroxide solids.

► Residual waste from five Hanford spent fuel process storage tanks was evaluated.
► Gibbsite is a common mineral in tanks with high Al concentrations.
► Non-crystalline U–Na–C–O–P ± H phases are common in the U-rich residual.
► Iron oxides/hydroxides have been identified in all residual waste samples.
► Uranium release is highly dependent on waste and leachant compositions.