title: Effects of organic carbon supply rates on uranium mobility in a previously bioreduced contaminated sediment.
abstract: Bioreduction-based strategies for remediating uranium (U)-contaminated sediments face the challenge of maintaining the reduced status of U for long times. Because groundwater influxes continuously bring in oxidizing terminal electron acceptors (O2, NO3(-)), it is necessary to continue supplying organic carbon (OC) to maintain the reducing environment after U bioreduction is achieved. We tested the influence of OC supply rates on mobility of previously microbial reduced uranium U(IV) in contaminated sediments. We found that high degrees of U mobilization occurred when OC supply rates were high, and when the sediment still contained abundant Fe(III). Although 900 days with low levels of OC supply minimized U mobilization, the sediment redox potential increased with time as did extractable U(VI) fractions. Molecular analyses of total microbial activity demonstrated a positive correlation with OC supply and analyses of Geobacteraceae activity (RT-qPCR of 16S rRNA) indicated continued activity even when the effluent Fe(II) became undetectable. These data support our hypothesis on the mechanisms responsible for remobilization of U under reducing conditions; that microbial respiration caused increased (bi)carbonate concentration and formation of stable uranyl carbonate complexes, thereby shifted U(IV)/U(VI) equilibrium to more reducing potentials. The data also suggested that low OC concentrations could not sustain the reducing condition of the sediment for much longer time. Bioreduced U(IV) is not sustainable in an oxidizing environment for a very long time.
authors.affiliation: Lawrence Berkeley National Laboratory, Berkeley, CA 94720, USA. jwan@lbl.gov
authors.forename: Jiamin
authors.initials: J
authors.lastname: Wan
authors.forename: Tetsu K
authors.initials: TK
authors.lastname: Tokunaga
authors.forename: Yongman
authors.initials: Y
authors.lastname: Kim
authors.forename: Eoin
authors.initials: E
authors.lastname: Brodie
authors.forename: Rebecca
authors.initials: R
authors.lastname: Daly
authors.forename: Terry C
authors.initials: TC
authors.lastname: Hazen
authors.forename: Mary K
authors.initials: MK
authors.lastname: Firestone
mesh_terms: D001673:Biodegradation, Environmental; D002244:Carbon / Q000032:analysis*; D002254:Carbonates / Q000737:chemistry; D045302:Geobacter / Q000378:metabolism*; D019015:Geologic Sediments / Q000382:microbiology*; D007501:Iron / Q000032:analysis; D010084:Oxidation-Reduction; D012329:RNA, Bacterial / Q000032:analysis; D012989:Soil Pollutants / Q000737:chemistry*; D013997:Time Factors; D014501:Uranium / Q000032:analysis / Q000302:isolation & purification*
chemical_list: D002254:Carbonates; D012329:RNA, Bacterial; D012989:Soil Pollutants; D014501:Uranium; D002244:Carbon; D007501:Iron