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

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

doi:10.1021/acs.est.8b03031

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

Journal Article · 19 October 2018 · Environmental Science and Technology

DOI: https://doi.org/10.1021/acs.est.8b03031 · OSTI ID:1490871

Stetten, Lucie ^[1]; Blanchart, Pascale ^[2];

^[2]; Lefebvre, Pierre ^[3]; Le Pape, Pierre ^[3]; Brest, Jessica ^[3]; Merrot, Pauline ^[3]; Julien, Anthony ^[2]; Proux, Olivier ^[4]; Webb, Samuel M. ^[5];

^[5]; Cazala, Charlotte ^[2];

^[3]

CNRS-Sorbonne Univ.-IRD-MNHN, Paris Cedex (France); Institut de Radioprotection et de Surete Nucleaire, Fontenay-aux-Roses (France)
Institut de Radioprotection et de Surete Nucleaire, Fontenay-aux-Roses (France)
CNRS-Sorbonne Univ.-IRD-MNHN, Paris Cedex (France)
Univ. Grenoble Alpes, Grenoble (France); BM30B/CRG-FAME, ESRF, Grenoble (France)
SLAC National Accelerator Lab., Menlo Park, CA (United States)

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 L_III-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.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States)

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC02-76SF00515

OSTI ID:: 1490871

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 22 Vol. 52; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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