Effects of aqueous complexation on reductive precipitation of uranium by Shewanella putrefaciens.docVIP

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Effects of aqueous complexation on reductive precipitation of uranium by Shewanella putrefaciens.doc

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Effects of aqueous complexation on reductive precipitation of uranium by Shewanella putrefaciens

GEOCHEMICALTRANSACTIONS VOLUME5,NUMBER3 SEPTEMBER2004 Effectsofaqueouscomplexationonreductiveprecipitation ofuraniumbyShewanellaputrefaciens JohnsonR.Haasa)andAbrahamNorthup DepartmentofGeosciences,WesternMichiganUniversity,Kalamazoo,Michigan49008 ?Received18May2004;accepted17August2004;publishedonline1October2004? We have examined the effects of aqueous complexation on rates of dissimilatory reductive precipitation of uranium by Shewanella putrefaciens. Uranium?VI? was supplied as sole terminal electronacceptortoShewanellaputrefaciens?strain200R?inde?nedlaboratorymediaunderstrictly anaerobic conditions. Media were amended with different multidentate organic acids, and experiments were performed at different U?VI? and ligand concentrations. Organic acids used as complexing agents were oxalic, malonic, succinic, glutaric, adipic, pimelic, maleic, citric, and nitrilotriacetic acids, tiron, EDTA, and Aldrich humic acid. Reductive precipitation of U?VI?, resultinginremovalofinsolubleamorphousUO2fromsolution,wasmeasuredasafunctionoftime bydeterminationoftotaldissolvedU.Reductiveprecipitationwasmeasured,ratherthannetU?VI? reductiontoU?IV?,toassessoverallUremovalratesfromsolution,whichmaybeusedtogaugethe in?uenceofchelationonmicrobialUmineralization.InitiallinearratesofUreductiveprecipitation were found to correlate with stability constants of 1:1 aqueous U?VI?:ligand and U?IV?:ligand complexes. In the presence of strongly complexing ligands ?e.g., NTA, Tiron, EDTA?, UO2 precipitation did not occur. Our results are consistent with ligand-retarded precipitation of UO2, whichisanalogoustoligand-assistedsolidphasedissolutionbutinreverse:ligandexchangewith the U4? aquo cation acts as a rate-limiting reaction moderating coordination of water molecules with U4?, which is a necessary step in UO2 precipitation. Ligand exchange kinetics governing dissociation rates of ligands from U?VI?-organic complexes may also in?uence overall UO2 production rates, although the magnitude of t