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Title: Redox Fluctuations and Organic Complexation Govern Uranium Redistribution from U(IV)-Phosphate Minerals in a Mining-Polluted Wetland Soil, Brittany, France

Abstract

Wetlands have been proposed to naturally attenuate U transfers in the environment via U complexation by organic matter and potential U reduction. However, U mobility may depend on the identity of particulate/dissolved uranium source materials and their redox sensitivity. Here, we examined the fate of uranium in a highly contaminated wetland (up to 4500 mg·kg–1 U) impacted by former mine water discharges. Bulk U LIII-EXAFS and (micro-)XANES combined with SEM-EDXS analyses of undisturbed soil cores show a sharp U redox boundary at the water table, together with a major U redistribution from U(IV)-minerals to U(VI)-organic matter complexes. Above the water table, U is fully oxidized into mono- and bidentate U(VI)-carboxyl and monodentate U(VI)-phosphoryl complexes. Minute amounts of U(VI)-phosphate minerals are also observed. Below the water table, U is fully reduced and is partitioned between U(IV)-phosphate minerals (i.e., ningyoite and a lermontovite-like phase), and bidentate U(IV)-phosphoryl and monodentate U(IV)-carboxyl complexes. Such a U redistribution from U-minerals inherited from mine water discharge deposits could result from redox cycling nearby the water table fluctuation zone. In conclusion, oxidative dissolution of U(IV)-phosphate minerals could have led to U(VI)-organic matter complexation, followed by subsequent reduction into U(IV)-organic complexes. However, uranium(IV) minerals could have been preservedmore » in permanently waterlogged soil.« less

Authors:
 [1];  [2]; ORCiD logo [2];  [3];  [3];  [3];  [3];  [2];  [4];  [5]; ORCiD logo [5];  [2]; ORCiD logo [3]
+ Show Author Affiliations
  1. CNRS-Sorbonne Univ.-IRD-MNHN, Paris Cedex (France); Institut de Radioprotection et de Surete Nucleaire, Fontenay-aux-Roses (France)
  2. Institut de Radioprotection et de Surete Nucleaire, Fontenay-aux-Roses (France)
  3. CNRS-Sorbonne Univ.-IRD-MNHN, Paris Cedex (France)
  4. Univ. Grenoble Alpes, Grenoble (France); BM30B/CRG-FAME, ESRF, Grenoble (France)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States)
Publication Date:
Research Org.:
SLAC National Accelerator Lab., Menlo Park, CA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1490871
Grant/Contract Number:  
AC02-76SF00515
Resource Type:
Accepted Manuscript
Journal Name:
Environmental Science and Technology
Additional Journal Information:
Journal Volume: 52; Journal Issue: 22; Journal ID: ISSN 0013-936X
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
54 ENVIRONMENTAL SCIENCES

Citation Formats

Stetten, Lucie, Blanchart, Pascale, Mangeret, Arnaud, Lefebvre, Pierre, Le Pape, Pierre, Brest, Jessica, Merrot, Pauline, Julien, Anthony, Proux, Olivier, Webb, Samuel M., Bargar, John R., Cazala, Charlotte, and Morin, Guillaume. Redox Fluctuations and Organic Complexation Govern Uranium Redistribution from U(IV)-Phosphate Minerals in a Mining-Polluted Wetland Soil, Brittany, France. United States: N. p., 2018. Web. doi:10.1021/acs.est.8b03031.
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Stetten, Lucie, Blanchart, Pascale, Mangeret, Arnaud, Lefebvre, Pierre, Le Pape, Pierre, Brest, Jessica, Merrot, Pauline, Julien, Anthony, Proux, Olivier, Webb, Samuel M., Bargar, John R., Cazala, Charlotte, & Morin, Guillaume. Redox Fluctuations and Organic Complexation Govern Uranium Redistribution from U(IV)-Phosphate Minerals in a Mining-Polluted Wetland Soil, Brittany, France. United States. https://doi.org/10.1021/acs.est.8b03031
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Stetten, Lucie, Blanchart, Pascale, Mangeret, Arnaud, Lefebvre, Pierre, Le Pape, Pierre, Brest, Jessica, Merrot, Pauline, Julien, Anthony, Proux, Olivier, Webb, Samuel M., Bargar, John R., Cazala, Charlotte, and Morin, Guillaume. Fri . "Redox Fluctuations and Organic Complexation Govern Uranium Redistribution from U(IV)-Phosphate Minerals in a Mining-Polluted Wetland Soil, Brittany, France". United States. https://doi.org/10.1021/acs.est.8b03031. https://www.osti.gov/servlets/purl/1490871.
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@article{osti_1490871,
title = {Redox Fluctuations and Organic Complexation Govern Uranium Redistribution from U(IV)-Phosphate Minerals in a Mining-Polluted Wetland Soil, Brittany, France},
author = {Stetten, Lucie and Blanchart, Pascale and Mangeret, Arnaud and Lefebvre, Pierre and Le Pape, Pierre and Brest, Jessica and Merrot, Pauline and Julien, Anthony and Proux, Olivier and Webb, Samuel M. and Bargar, John R. and Cazala, Charlotte and Morin, Guillaume},
abstractNote = {Wetlands have been proposed to naturally attenuate U transfers in the environment via U complexation by organic matter and potential U reduction. However, U mobility may depend on the identity of particulate/dissolved uranium source materials and their redox sensitivity. Here, we examined the fate of uranium in a highly contaminated wetland (up to 4500 mg·kg–1 U) impacted by former mine water discharges. Bulk U LIII-EXAFS and (micro-)XANES combined with SEM-EDXS analyses of undisturbed soil cores show a sharp U redox boundary at the water table, together with a major U redistribution from U(IV)-minerals to U(VI)-organic matter complexes. Above the water table, U is fully oxidized into mono- and bidentate U(VI)-carboxyl and monodentate U(VI)-phosphoryl complexes. Minute amounts of U(VI)-phosphate minerals are also observed. Below the water table, U is fully reduced and is partitioned between U(IV)-phosphate minerals (i.e., ningyoite and a lermontovite-like phase), and bidentate U(IV)-phosphoryl and monodentate U(IV)-carboxyl complexes. Such a U redistribution from U-minerals inherited from mine water discharge deposits could result from redox cycling nearby the water table fluctuation zone. In conclusion, oxidative dissolution of U(IV)-phosphate minerals could have led to U(VI)-organic matter complexation, followed by subsequent reduction into U(IV)-organic complexes. However, uranium(IV) minerals could have been preserved in permanently waterlogged soil.},
doi = {10.1021/acs.est.8b03031},
journal = {Environmental Science and Technology},
number = 22,
volume = 52,
place = {United States},
year = {Fri Oct 19 00:00:00 EDT 2018},
month = {Fri Oct 19 00:00:00 EDT 2018}
}
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Journal Article:
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https://doi.org/10.1021/acs.est.8b03031
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Cited by: 23 works
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Figures / Tables:

Figure 1 Figure 1: Vertical distribution of bulk uranium concentrations and redox state, and pedo-lithology of the soil cores C2 and C6 sampled in the contaminated wetland. From left to right: picture of the cores, pedo-lithological interpretation based on chemistry and mineralogy data ( see Table SI-1; Figure S1-2a and text) andmore » red curve displaying the total bulk uranium concentrations in the solid phase in mg·kg-1 (see Table SI-1) with bar diagrams displaying the proportions ofU(VI) in orange and U(N) in green obtained from LCF analysis of the U LⅢ-edge XANES data (see Table SI-2 and Figure SI-4), normalized to bulk U. The water table level at the sampling date is indicated in light blue and dash line. The water table level was observed on the field for the C6 core and inferred from the position of the iron-oxide layer for the C2 core (see text).« less
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