300 Area Uranium Stabilization Through Polyphosphate Injection: Final Report

Vermeul, Vincent R. ; Bjornstad, Bruce N. ; Fritz, Brad G. ; Fruchter, Jonathan S. ; Mackley, Rob D. ; Newcomer, Darrell R. ; Mendoza, Donaldo P. ; Rockhold, Mark L. ; Wellman, Dawn M. ; Williams, Mark D.

Pacific Northwest National Laboratory (U.S.)

关键词: 58 Geosciences;    Uranyl Phosphates;    Phosphates;    Stabilization;    Autunite;   

DOI  :  10.2172/967237
RP-ID  :  PNNL-18529
RP-ID  :  AC05-76RL01830
RP-ID  :  967237

美国|英语

来源: UNT Digital Library

【 摘 要 】

The objective of the treatability test was to evaluate the efficacy of using polyphosphate injections to treat uranium-contaminated groundwater in situ. A test site consisting of an injection well and 15 monitoring wells was installed in the 300 Area near the process trenches that had previously received uranium-bearing effluents. This report summarizes the work on the polyphosphate injection project, including bench-scale laboratory studies, a field injection test, and the subsequent analysis and interpretation of the results. Previous laboratory tests have demonstrated that when a soluble form of polyphosphate is injected into uranium-bearing saturated porous media, immobilization of uranium occurs due to formation of an insoluble uranyl phosphate, autunite [Ca(UO2)2(PO4)2•nH2O]. These tests were conducted at conditions expected for the aquifer and used Hanford soils and groundwater containing very low concentrations of uranium (10-6 M). Because autunite sequesters uranium in the oxidized form U(VI) rather than forcing reduction to U(IV), the possibility of re-oxidation and subsequent re-mobilization is negated. Extensive testing demonstrated the very low solubility and slow dissolution kinetics of autunite. In addition to autunite, excess phosphorous may result in apatite mineral formation, which provides a long-term source of treatment capacity. Phosphate arrival response data indicate that, under site conditions, the polyphosphate amendment could be effectively distributed over a relatively large lateral extent, with wells located at a radial distance of 23 m (75 ft) reaching from between 40% and 60% of the injection concentration. Given these phosphate transport characteristics, direct treatment of uranium through the formation of uranyl-phosphate mineral phases (i.e., autunite) could likely be effectively implemented at full field scale. However, formation of calcium-phosphate mineral phases using the selected three-phase approach was problematic. Although amendment arrival response data indicate some degree of overlap between the reactive species and thus potential for the formation of calcium-phosphate mineral phases (i.e., apatite formation), the efficiency of this treatment approach was relatively poor. In general, uranium performance monitoring results support the hypothesis that limited long-term treatment capacity (i.e., apatite formation) was established during the injection test. Two separate overarching issues affect the efficacy of apatite remediation for uranium sequestration within the 300 Area: 1) the efficacy of apatite for sequestering uranium under the present geochemical and hydrodynamic conditions, and 2) the formation and emplacement of apatite via polyphosphate technology. In addition, the long-term stability of uranium sequestered via apatite is dependent on the chemical speciation of uranium, surface speciation of apatite, and the mechanism of retention, which is highly susceptible to dynamic geochemical conditions. It was expected that uranium sequestration in the presence of hydroxyapatite would occur by sorption and/or surface complexation until all surface sites have been depleted, but that the high carbonate concentrations in the 300 Area would act to inhibit the transformation of sorbed uranium to chernikovite and/or autunite. Adsorption of uranium by apatite was never considered a viable approach for in situ uranium sequestration in and of itself, because by definition, this is a reversible reaction. The efficacy of uranium sequestration by apatite assumes that the adsorbed uranium would subsequently convert to autunite, or other stable uranium phases. Because this appears to not be the case in the 300 Area aquifer, even in locations near the river, apatite may have limited efficacy for the retention and long-term immobilization of uranium at the 300 Area site..