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The influence of microbial redox cycling on radionuclide mobility in the subsurface at a low-level radioactive waste storage site

Authors

  • M. J. WILKINS,

    1. Williamson Research Centre for Molecular Environmental Science and School of Earth, Atmospheric and Environmental Sciences, The University of Manchester, Oxford Road, Manchester M13 9PL, UK
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  • F. R. LIVENS,

    1. Williamson Research Centre for Molecular Environmental Science and School of Earth, Atmospheric and Environmental Sciences, The University of Manchester, Oxford Road, Manchester M13 9PL, UK
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  • D. J. VAUGHAN,

    1. Williamson Research Centre for Molecular Environmental Science and School of Earth, Atmospheric and Environmental Sciences, The University of Manchester, Oxford Road, Manchester M13 9PL, UK
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  • I. BEADLE,

    1. Nexia Solutions, Risley, Warrington WA3 6AS, UK
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  • J. R. LLOYD

    1. Williamson Research Centre for Molecular Environmental Science and School of Earth, Atmospheric and Environmental Sciences, The University of Manchester, Oxford Road, Manchester M13 9PL, UK
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Corresponding author: J. R. Lloyd. Tel.: +44 (0) 161 275 7155; fax: +44 (0) 161 306 9361; e-mail: jon.lloyd@manchester.ac.uk.

ABSTRACT

As anaerobic microbial metabolism can have a major impact on radionuclide speciation and mobility in the subsurface, the solubility of uranium, technetium and radium was determined in microcosms prepared from sediments adjacent to the Drigg low-level radioactive waste storage site (UK). Both uranium (as U(VI); inline image) and Tc (as Tc(VII); inline image) were removed from groundwater concurrently with microbial Fe(III) reduction, presumably through reduction to insoluble U(IV) and Tc(IV), respectively, while Ra (Ra2+) that had rapidly sorbed onto mineral surfaces was not released following Fe(III) reduction. Biogenic Fe(II) minerals in reduced Drigg sediments were unable to reduce U(VI) abiotically but could reduce Tc(VII). Following addition of the oxidant nitrate to the reduced sediments, uranium was remobilized and released into solution, whereas technetium remained associated with an insoluble phase. A close relative of Pseudomonas stutzeri dominated the microbial communities under denitrifying conditions, reducing nitrate to nitrite in the microcosms, which was able to reoxidize Fe(II) and U(IV), with release of the latter into solution as U(VI). These data suggest that microbial Fe(III) reduction in the far-field at Drigg has the potential to decrease the migration of some radionuclides in the subsurface, and the potential for reoxidation and remobilization by nitrate, a common contaminant in nuclear waste streams, is radionuclide-specific.

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