U(VI) Reduction by Biogenic and Abiotic Hydroxycarbonate Green Rusts: Impacts on U(IV) Speciation and Stability Over Time

Yan, Sen; Boyanov, Maxim I.; Mishra, Bhoopesh; Kemner, Kenneth M.; O'Loughlin, Edward J.

doi:10.1021/acs.est.7b06405

U(VI) Reduction by Biogenic and Abiotic Hydroxycarbonate Green Rusts: Impacts on U(IV) Speciation and Stability Over Time

Journal Article · Mon Apr 09 00:00:00 EDT 2018 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.7b06405· OSTI ID:1437378

Yan, Sen ^[1]; ^[2]; Mishra, Bhoopesh ^[3]; Kemner, Kenneth M. ^[4]; ^[4]

China Univ. of Geosciences, Wuhan (China); Argonne National Lab. (ANL), Argonne, IL (United States)
Argonne National Lab. (ANL), Argonne, IL (United States); Bulgarian Academy of Sciences, Sofia (Bulgaria)
Argonne National Lab. (ANL), Argonne, IL (United States); Univ. of Leeds, Leeds (United Kingdom)
Argonne National Lab. (ANL), Argonne, IL (United States)

Green rusts (GRs) are redox active Fe^II-Fe^III minerals that form in the environment via various biotic and abiotic processes. Although both biogenic (BioGR) and abiotic (ChemGR) GRs have been shown to reduce U^VI, the dynamics of the transformations and the speciation and stability of the resulting U^IV phases are poorly understood. We used carbonate extraction and XAFS spectroscopy to investigate the products of U^VI reduction by BioGR and ChemGR. The results show that both GRs can rapidly remove U^VI from synthetic groundwater via reduction to U^IV. The initial products in the ChemGR system are solids-associated U^IV-carbonate complexes that gradually transform to nanocrystalline uraninite over time, leading to a decrease in the proportion of carbonate-extractable U from ~95% to ~10%. In contrast, solid-phase U^IV atoms in the BioGR system remain relatively extractable, non-uraninite U^IV species over the same reaction period. The presence of calcium and carbonate in groundwater significantly increase the extractability of U^IV in the BioGR system. Furthermore, these data provide new insights into the transformations of U under anoxic conditions in groundwater that contains calcium and carbonate, and have major implications for predicting uranium stability within redox dynamic environments and designing approaches for the remediation of uranium-contaminated groundwater.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Biological and Environmental Research (BER) (SC-23)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1437378

Journal Information:: Environmental Science and Technology, Journal Name: Environmental Science and Technology Journal Issue: 8 Vol. 52; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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