Speciation of Uranium in Sediments before and after In situ Biostimulation

Shelly D. Kelly, Kenneth M. Kemner, Jack Carley, Craig Criddle, Phillip M. Jardine, Terence L. Marsh, Debra Phillips, David Watson, Wei-Min Wu

    Research output: Contribution to journalArticlepeer-review

    102 Citations (Scopus)

    Abstract

    The success of sequestration-based remediation strategies will depend on detailed information, including the predominant U species present as sources before biostimulation and the products produced during and after in situ biostimulation. We used X-ray absorption spectroscopy to determine the valence state and chemical speciation of U in sediment samples collected at a variety of depths through the contaminant plume at the Field Research Center at Oak Ridge, TN, before and after approximately 400 days of in situ biostimulation, as well as in duplicate bioreduced sediments after 363 days of resting conditions. The results indicate that U(VI) in subsurface sediments was partially reduced to 10–40% U(IV) during biostimulation. After biostimulation, U was no longer bound to carbon ligands and was adsorbed to Fe/Mn minerals. Reduction of U(VI) to U(IV) continued in sediment samples stored under anaerobic condition at <4 °C for 12 months, with the fraction of U(IV) in sediments more than doubling and U concentrations in the aqueous phase decreasing from 0.5-0.74 to <0.1 µM. A shift of uranyl species from uranyl bound to phosphorus ligands to uranyl bound to carbon ligands and the formation of nanoparticulate uraninite occurred in the sediment samples during storage.
    Original languageEnglish
    Pages (from-to)1558-1564
    Number of pages7
    JournalEnvironmental Science and Technology
    Volume42
    Issue number5
    DOIs
    Publication statusPublished - 25 Jan 2008

    ASJC Scopus subject areas

    • Environmental Engineering
    • Environmental Science(all)
    • Environmental Chemistry

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