Stimulating the microbial reduction of aqueous uranium(VI) to insoluble U(IV) via electron donor addition has been proposed as a strategy to remediate uranium-contaminated groundwater in situ. However, concerns have been raised regarding the longevity of microbially precipitated U(IV) in the subsurface, particularly given that it may become remobilized if the conditions change to become oxidizing. An alternative mechanism is to stimulate the precipitation of poorly soluble uranium phosphates via the addition of an organophosphate and promote the development of reducing conditions. Here, we selected a sediment sample from a U.K. nuclear site and stimulated the microbial community with glycerol phosphate under anaerobic conditions to assess whether uranium phosphate precipitation was a viable bioremediation strategy. Results showed that U(VI) was rapidly removed from solution and precipitated as a reduced crystalline U(IV) phosphate mineral similar to ningyoite. This mineral was considerably more recalcitrant to oxidative remobilization than the products of microbial U(VI) reduction. Bacteria closely related to Pelosinus species may have played a key role in uranium removal in these experiments. This work has implications for the stewardship of uranium-contaminated groundwater, with the formation of U(IV) phosphates potentially offering a more effective strategy for maintaining low concentrations of uranium in groundwater over long time periods.
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Mechanism of enhanced strontium uptake into calcite via an amorphous calcium carbonate (ACC) crystallisation pathway
Strontium is an important contaminant radionuclide at many former nuclear sites. This paper investigates the effect of changing pH and ionic strength on the sorption of Sr to a range of common soil minerals. Specifically it focuses on the sorption of Sr onto illite, chlorite, goethite, and a mixed sediment. The interplay between ionic strength and pH was determined by varying the background ionic strength of the system using both NaCl (for a constant pH) and NaOH (to also vary pH). Under conditions of moderate pH, Sr sorption decreased with increasing ionic strength, due to competition between the Na and Sr atoms for the outer-sphere complexes. However, where increasing ionic strength was accompanied by increasing pH, Sr sorption remained high. This suggested that Sr was sorbed to the minerals without competition from background Na ions. Extended X-ray absorption fine structure (EXAFS) spectra confirmed that at highly alkaline pH (>12.5) Sr was forming inner-sphere complexes on the surfaces of all minerals. This specific adsorption of the Sr (as SrOH(+)) explains why it was still adsorbed to the minerals under very high ionic strength conditions and was not out-competed by Na.
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