Uranium Mobility During In Situ Redox Manipulation of the 100 Areas of the Hanford Site
A series of laboratory experiments and computer simulations was conducted to assess the extent of uranium remobilization that is likely to occur at the end of the life cycle of an in situ sediment reduction process. The process is being tested for subsurface remediation of chromate- and chlorinated solvent-contaminated sediments at the Hanford Site in southeastern Washington. Uranium species that occur naturally in the +6 valence state {approximately}(VI) at 10 ppb in groundwater at Hanford will accumulate as U(N) through the reduction and subsequent precipitation conditions of the permeable barrier created by in situ redox manipulation. The precipitated uranium will W remobilized when the reductive capacity of the barrier is exhausted and the sediment is oxidized by the groundwater containing dissolved oxygen and other oxidants such as chromate. Although U(N) accumulates from years or decades of reduction/precipitation within the reduced zone, U(W) concentrations in solution are only somewhat elevated during aquifer oxidation because oxidation and dissolution reactions that release U(N) precipitate to solution are slow. The release rate of uranium into solution was found to be controlled mainly by the oxidation/dissolution rate of the U(IV) precipitate (half-life 200 hours) and partially by the fast oxidation of adsorbed Fe(II) (half- life 5 hours) and the slow oxidation of Fe(II)CO{sub 3} (half-life 120 hours) in the reduced sediment. Simulations of uranium transport that incorporated these and other reactions under site-relevant conditions indicated that 35 ppb U(VI) is the maximum concentration likely to result from mobilization of the precipitated U(IV) species. Experiments also indicated that increasing the contact time between the U(IV) precipitates and the reduced sediment, which is likely to occur in the field, results in a slower U(IV) oxidation rate, which, in turn, would lower the maximum concentration of mobilized U(W). A six-month-long column experiment confirmed that uranium accumulated in reduced sediment was released slowly into solution with U(W) concentrations at only slightly greater than influent U(W) concentrations. This experiment also demonstrated that dissolved chromate, another oxidant likely to be present in some field systems, did not increase the release rate of uranium into solution.
- Research Organization:
- Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
- Sponsoring Organization:
- US Department of Energy (US)
- DOE Contract Number:
- AC06-76RL01830
- OSTI ID:
- 2120
- Report Number(s):
- PNNL-12048; EW40; R&D Project: 26706; EW40; TRN: US0101284
- Resource Relation:
- Other Information: PBD: 3 Dec 1998
- Country of Publication:
- United States
- Language:
- English
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