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Abstract
It is well known that microbially mediated reduction can result in the removal of U(VI)(aq) from solution by forming poorly soluble U(IV) oxides; however, the fate of U(VI) already associated with mineral surfaces is less clear. Here we describe results from both oxic adsorption and anaerobic microcosm experiments to examine the fate of sorbed U(VI) during microbially mediated bioreduction. The microcosm experiments contained sediment representative of the nuclear facility at Dounreay, UK. In oxic adsorption experiments, uptake of U(VI) was rapid and complete from artificial groundwater and where groundwater was amended with 0.2 mmol l−1 ethylenediaminetetraacetic acid (EDTA) a complexing ligand used in nuclear fuel cycle operations. By contrast, uptake of U(VI) was incomplete in groundwaters amended with 10 mmol l−1 bicarbonate. Analysis of sediments using X-ray adsorption spectroscopy showed that in these oxic samples, U was present as U(VI). After anaerobic incubation of U(VI) labelled sediments for 120 days, microbially mediated Fe(III)- and SO4 2−- reducing conditions had developed and XAS data showed uranium was reduced to U(IV). Further investigation of the unamended groundwater systems, where oxic systems were dominated by U(VI) sorption, showed that reduction of sorbed U(VI) required an active microbial population and occurred after robust iron- and sulfate- reducing conditions had developed. Microbial community analysis of the bioreduced sediment showed a community shift compared to the oxic sediment with close relatives of Geobacter and Clostridium species, which are known to facilitate U(VI) reduction, dominating. Overall, efficient U(VI) removal from solution by adsorption under oxic conditions dominated in unamended and EDTA amended systems. In all systems bioreduction resulted in the formation of U(IV) in solids.
ACKNOWLEDGMENTS
Thanks to Bob Bilsborrow, for invaluable help in XAS data acquisition, to Gareth Law, University of Leeds, for help in XANES data acquisition and analysis and to Miranda Keith-Roach, Stephanie Handley, Rachael Spraggs and Doug McAllister. This work was supported by grants NE/D00473X/1 and NE/D005361/1 from the UK Natural Environment Research Council, NERC studentship NER/S/A/2004/13005 to JDCB and by Daresbury SRS beamtime allocation from the UK Science and Technology Facilities Council.
