Microbial Reduction of U(VI) under Alkaline Conditions: Implications for Radioactive Waste Geodisposal.

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Title: Microbial Reduction of U(VI) under Alkaline Conditions: Implications for Radioactive Waste Geodisposal.
Authors: Williamson, Adam J.1, Morris, Katherine1, Law, Gareth T. W.2, Rizoulis, Athanasios1, Charnock, John M.1, Lloyd, Jonathan R.1 jon.lloyd@manchester.ac.uk
Source: Environmental Science & Technology. 11/18/2014, Vol. 48 Issue 22, p13549-13556. 8p.
Subjects: Radioactive waste disposal, Chemical reduction, Microorganisms, Uranium, Chemical speciation, Biogeochemistry, Nitrates, Iron
Abstract: Although there is consensus that microorganisms significantly influence uranium speciation and mobility in the subsurface under circumneutral conditions, microbiologically mediated U(VI) redox cycling under alkaline conditions relevant to the geological disposal of cementitious intermediate level radioactive waste, remains unexplored. Here, we describe microcosm experiments that investigate the biogeochemical fate of U(VI) at pH 10-10.5, using sediments from a legacy lime working site, stimulated with an added electron donor, and incubated in the presence and absence of added Fe(III) as ferrihydrite. In systems without added Fe(III), partial U(VI) reduction occurred, forming a U(IV)-bearing non-uraninite phase which underwent reoxidation in the presence of air (O2) and to some extent nitrate. By contrast, in the presence of added Fe(III), U(VI) was first removed from solution by sorption to the Fe(III) mineral, followed by bioreduction and (bio)magnetite formation coupled to formation of a complex U(IV)-bearing phase with uraninite present, which also underwent air (O2) and partial nitrate reoxidation. 16S rRNA gene pyrosequencing showed that Gram-positive bacteria affiliated with the Firmicutes and Bacteroidetes dominated in the post-reduction sediments. These data provide the first insights into uranium biogeochemistry at high pH and have significant implications for the long-term fate of uranium in geological disposal in both engineered barrier systems and the alkaline, chemically disturbed geosphere. [ABSTRACT FROM AUTHOR]
Copyright of Environmental Science & Technology is the property of American Chemical Society and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract. (Copyright applies to all Abstracts.)
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  Data: Microbial Reduction of U(VI) under Alkaline Conditions: Implications for Radioactive Waste Geodisposal.
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  Data: <searchLink fieldCode="AR" term="%22Williamson%2C+Adam+J%2E%22">Williamson, Adam J.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Morris%2C+Katherine%22">Morris, Katherine</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Law%2C+Gareth+T%2E+W%2E%22">Law, Gareth T. W.</searchLink><relatesTo>2</relatesTo><br /><searchLink fieldCode="AR" term="%22Rizoulis%2C+Athanasios%22">Rizoulis, Athanasios</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Charnock%2C+John+M%2E%22">Charnock, John M.</searchLink><relatesTo>1</relatesTo><br /><searchLink fieldCode="AR" term="%22Lloyd%2C+Jonathan+R%2E%22">Lloyd, Jonathan R.</searchLink><relatesTo>1</relatesTo><i> jon.lloyd@manchester.ac.uk</i>
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  Data: <searchLink fieldCode="JN" term="%22Environmental+Science+%26+Technology%22">Environmental Science & Technology</searchLink>. 11/18/2014, Vol. 48 Issue 22, p13549-13556. 8p.
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  Data: <searchLink fieldCode="DE" term="%22Radioactive+waste+disposal%22">Radioactive waste disposal</searchLink><br /><searchLink fieldCode="DE" term="%22Chemical+reduction%22">Chemical reduction</searchLink><br /><searchLink fieldCode="DE" term="%22Microorganisms%22">Microorganisms</searchLink><br /><searchLink fieldCode="DE" term="%22Uranium%22">Uranium</searchLink><br /><searchLink fieldCode="DE" term="%22Chemical+speciation%22">Chemical speciation</searchLink><br /><searchLink fieldCode="DE" term="%22Biogeochemistry%22">Biogeochemistry</searchLink><br /><searchLink fieldCode="DE" term="%22Nitrates%22">Nitrates</searchLink><br /><searchLink fieldCode="DE" term="%22Iron%22">Iron</searchLink>
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  Data: Although there is consensus that microorganisms significantly influence uranium speciation and mobility in the subsurface under circumneutral conditions, microbiologically mediated U(VI) redox cycling under alkaline conditions relevant to the geological disposal of cementitious intermediate level radioactive waste, remains unexplored. Here, we describe microcosm experiments that investigate the biogeochemical fate of U(VI) at pH 10-10.5, using sediments from a legacy lime working site, stimulated with an added electron donor, and incubated in the presence and absence of added Fe(III) as ferrihydrite. In systems without added Fe(III), partial U(VI) reduction occurred, forming a U(IV)-bearing non-uraninite phase which underwent reoxidation in the presence of air (O2) and to some extent nitrate. By contrast, in the presence of added Fe(III), U(VI) was first removed from solution by sorption to the Fe(III) mineral, followed by bioreduction and (bio)magnetite formation coupled to formation of a complex U(IV)-bearing phase with uraninite present, which also underwent air (O2) and partial nitrate reoxidation. 16S rRNA gene pyrosequencing showed that Gram-positive bacteria affiliated with the Firmicutes and Bacteroidetes dominated in the post-reduction sediments. These data provide the first insights into uranium biogeochemistry at high pH and have significant implications for the long-term fate of uranium in geological disposal in both engineered barrier systems and the alkaline, chemically disturbed geosphere. [ABSTRACT FROM AUTHOR]
– Name: AbstractSuppliedCopyright
  Label:
  Group: Ab
  Data: <i>Copyright of Environmental Science & Technology is the property of American Chemical Society and its content may not be copied or emailed to multiple sites without the copyright holder's express written permission. Additionally, content may not be used with any artificial intelligence tools or machine learning technologies. However, users may print, download, or email articles for individual use. This abstract may be abridged. No warranty is given about the accuracy of the copy. Users should refer to the original published version of the material for the full abstract.</i> (Copyright applies to all Abstracts.)
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        Value: 10.1021/es5017125
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      – Code: eng
        Text: English
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        StartPage: 13549
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      – SubjectFull: Radioactive waste disposal
        Type: general
      – SubjectFull: Chemical reduction
        Type: general
      – SubjectFull: Microorganisms
        Type: general
      – SubjectFull: Uranium
        Type: general
      – SubjectFull: Chemical speciation
        Type: general
      – SubjectFull: Biogeochemistry
        Type: general
      – SubjectFull: Nitrates
        Type: general
      – SubjectFull: Iron
        Type: general
    Titles:
      – TitleFull: Microbial Reduction of U(VI) under Alkaline Conditions: Implications for Radioactive Waste Geodisposal.
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              Text: 11/18/2014
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              Y: 2014
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