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

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

Journal Article · 09 April 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.

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

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

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1437378

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

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 18 works

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References (56)

Speciation of Uranium in Sediments before and after In situ Biostimulation Kelly, Shelly D.; Kemner, Kenneth M.; Carley, Jack Environmental Science & Technology, Vol. 42, Issue 5 https://doi.org/10.1021/es071764i	journal	March 2008
Uranium redox transition pathways in acetate-amended sediments Bargar, J. R.; Williams, K. H.; Campbell, K. M. Proceedings of the National Academy of Sciences, Vol. 110, Issue 12 https://doi.org/10.1073/pnas.1219198110	journal	March 2013
Evaluating Chemical Extraction Techniques for the Determination of Uranium Oxidation State in Reduced Aquifer Sediments Stoliker, Deborah L.; Campbell, Kate M.; Fox, Patricia M. Environmental Science & Technology, Vol. 47, Issue 16 https://doi.org/10.1021/es401450v	journal	August 2013
Solution and Microbial Controls on the Formation of Reduced U(IV) Species Boyanov, Maxim I.; Fletcher, Kelly E.; Kwon, Man Jae Environmental Science & Technology, Vol. 45, Issue 19 https://doi.org/10.1021/es2014049	journal	October 2011
Effects of calcium and phosphate on uranium(IV) oxidation: Comparison between nanoparticulate uraninite and amorphous UIV–phosphate Latta, Drew E.; Kemner, Kenneth M.; Mishra, Bhoopesh Geochimica et Cosmochimica Acta, Vol. 174 https://doi.org/10.1016/j.gca.2015.11.010	journal	February 2016
Surface area effects on the reduction of UVI in the presence of synthetic montmorillonite Boyanov, Maxim I.; Latta, Drew E.; Scherer, Michelle M. Chemical Geology, Vol. 464 https://doi.org/10.1016/j.chemgeo.2016.12.016	journal	August 2017
Green rust formation controls nutrient availability in a ferruginous water column Zegeye, Asfaw; Bonneville, Steeve; Benning, Liane G. Geology, Vol. 40, Issue 7 https://doi.org/10.1130/G32959.1	journal	July 2012
Identification of Green Rust in Groundwater Christiansen, B. C.; Balic-Zunic, T.; Dideriksen, K. Environmental Science & Technology, Vol. 43, Issue 10 https://doi.org/10.1021/es8011047	journal	May 2009
Observations and assessment of iron oxide and green rust nanoparticles in metal-polluted mine drainage within a steep redox gradient Johnson, Carol A.; Freyer, Gina; Fabisch, Maria Environmental Chemistry, Vol. 11, Issue 4 https://doi.org/10.1071/EN13184	journal	January 2014
Identification of a green rust mineral in a reductomorphic soil by Mossbauer and Raman spectroscopies Trolard, F.; Génin, J. -M. R.; Abdelmoula, M. Geochimica et Cosmochimica Acta, Vol. 61, Issue 5 https://doi.org/10.1016/S0016-7037(96)00381-X	journal	March 1997
Thermodynamic Equilibria in Aqueous Suspensions of Synthetic and Natural Fe(II)−Fe(III) Green Rusts: Occurrences of the Mineral in Hydromorphic Soils Génin, Jean-Marie R.; Bourrié, Guilhem; Trolard, Fabienne Environmental Science & Technology, Vol. 32, Issue 8 https://doi.org/10.1021/es970547m	journal	April 1998
In situ Mössbauer spectroscopy: Evidence for green rust (fougerite) in a gleysol and its mineralogical transformations with time and depth Feder, Frédéric; Trolard, Fabienne; Klingelhöfer, Göstar Geochimica et Cosmochimica Acta, Vol. 69, Issue 18 https://doi.org/10.1016/j.gca.2005.03.042	journal	September 2005
Identification of green rust in an ochre sludge Bender Koch, C.; Mørup, S. Clay Minerals, Vol. 26, Issue 4 https://doi.org/10.1180/claymin.1991.026.4.12	journal	December 1991
Fe(II)/Fe(III) ‘green rust’ developed within ochreous coal mine drainage sediment in South Wales, UK Bearcock, J. M.; Perkins, W. T.; Dinelli, E. Mineralogical Magazine, Vol. 70, Issue 6 https://doi.org/10.1180/0026461067060360	journal	December 2006
Arsenic sequestration by sorption processes in high-iron sediments Root, Robert A.; Dixit, Suvasis; Campbell, Kate M. Geochimica et Cosmochimica Acta, Vol. 71, Issue 23 https://doi.org/10.1016/j.gca.2007.04.038	journal	December 2007
Abiotic Transformation of Hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) by Green Rusts Larese-Casanova, Philip; Scherer, Michelle M. Environmental Science & Technology, Vol. 42, Issue 11 https://doi.org/10.1021/es702390b	journal	June 2008
Reduction of Halogenated Ethanes by Green rust O'Loughlin, Edward J.; Burris, David R. Environmental Toxicology and Chemistry, Vol. 23, Issue 1 https://doi.org/10.1897/03-45	journal	January 2004
Kinetics of Cr(VI) Reduction by Carbonate Green Rust Williams, Aaron G. B.; Scherer, Michelle M. Environmental Science & Technology, Vol. 35, Issue 17 https://doi.org/10.1021/es010579g	journal	September 2001
Reduction of AgI, AuIII, CuII, and HgII by FeII/FeIII hydroxysulfate green rust O’Loughlin, Edward J.; Kelly, Shelly D.; Kemner, Kenneth M. Chemosphere, Vol. 53, Issue 5 https://doi.org/10.1016/S0045-6535(03)00545-9	journal	November 2003
Nitrite Reduction by Biogenic Hydroxycarbonate Green Rusts: Evidence for Hydroxy-nitrite Green Rust Formation as an Intermediate Reaction Product Guerbois, Delphine; Ona-Nguema, Georges; Morin, Guillaume Environmental Science & Technology, Vol. 48, Issue 8 https://doi.org/10.1021/es404009k	journal	March 2014
Nitrate reduction by mixed iron(II-III) hydroxycarbonate green rust in the presence of phosphate anions: The key parameters influencing the ammonium selectivity Etique, Marjorie; Zegeye, Asfaw; Grégoire, Brian Water Research, Vol. 62 https://doi.org/10.1016/j.watres.2014.05.028	journal	October 2014
Fougerite: From field experiment to the homologation of the mineral Trolard, Fabienne Comptes Rendus Geoscience, Vol. 338, Issue 16 https://doi.org/10.1016/j.crte.2006.08.003	journal	December 2006
Bioreduction of ferric species and biogenesis of green rusts in soils Berthelin, Jacques; Ona-Nguema, Georges; Stemmler, Sébastien Comptes Rendus Geoscience, Vol. 338, Issue 6-7 https://doi.org/10.1016/j.crte.2006.04.013	journal	June 2006
Green Rust Formation during Fe(II) Oxidation by the Nitrate-Reducing Acidovorax sp. Strain BoFeN1 Pantke, Claudia; Obst, Martin; Benzerara, Karim Environmental Science & Technology, Vol. 46, Issue 3 https://doi.org/10.1021/es2016457	journal	January 2012
Formation of green rust via mineralogical transformation of ferric oxides (ferrihydrite, goethite and hematite) Usman, M.; Hanna, K.; Abdelmoula, M. Applied Clay Science, Vol. 64 https://doi.org/10.1016/j.clay.2011.10.008	journal	August 2012
Abiotic Process for Fe(II) Oxidation and Green Rust Mineralization Driven by a Heterotrophic Nitrate Reducing Bacteria ( Klebsiella mobilis ) Etique, Marjorie; Jorand, Frédéric P. A.; Zegeye, Asfaw Environmental Science & Technology, Vol. 48, Issue 7 https://doi.org/10.1021/es403358v	journal	March 2014
Effects of Phosphate on Secondary Mineral Formation During the Bioreduction of Akaganeite (.β-FeOOH): Green Rust Versus Framboidal Magnetite O'Loughlin, Edward; Gorski, Christopher; Scherer, Michelle Current Inorganic Chemistry, Vol. 5, Issue 3 https://doi.org/10.2174/1877944105666150421001126	journal	July 2015
Magnetite as a precursor for green rust through the hydrogenotrophic activity of the iron-reducing bacteria Shewanella putrefaciens Etique, M.; Jorand, F. P. A.; Ruby, C. Geobiology, Vol. 14, Issue 3 https://doi.org/10.1111/gbi.12170	journal	December 2015
Origin of the Differential Nanoscale Reactivity of Biologically and Chemically Formed Green Rust Crystals Investigated by Chemical Force Spectroscopy Zegeye, Asfaw; Etique, Marjorie; Carteret, Cédric The Journal of Physical Chemistry C, Vol. 118, Issue 11 https://doi.org/10.1021/jp500462r	journal	March 2014
Pseudo-first-order reaction of chemically and biologically formed green rusts with HgII and C15H15N3O2: Effects of pH and stabilizing agents (phosphate, silicate, polyacrylic acid, and bacterial cells) Remy, P. -Ph.; Etique, M.; Hazotte, A. A. Water Research, Vol. 70 https://doi.org/10.1016/j.watres.2014.12.007	journal	March 2015
Reduction of Uranium(VI) by Mixed Iron(II)/Iron(III) Hydroxide (Green Rust): Formation of UO ₂ Nanoparticles O'Loughlin, Edward J.; Kelly, Shelly D.; Cook, Russell E. Environmental Science & Technology, Vol. 37, Issue 4 https://doi.org/10.1021/es0208409	journal	February 2003
XAFS Investigation of the Interactions of U ^VI with Secondary Mineralization Products from the Bioreduction of Fe ^III Oxides O’Loughlin, Edward J.; Kelly, Shelly D.; Kemner, Kenneth M. Environmental Science & Technology, Vol. 44, Issue 5 https://doi.org/10.1021/es9027953	journal	March 2010
Reaction of Uranium(VI) with Green Rusts: Effect of Interlayer Anion Latta, Drew; Boyanov, Maxim; Kemner, Kenneth Current Inorganic Chemistry, Vol. 5, Issue 3 https://doi.org/10.2174/1877944105666150420235350	journal	July 2015
Inhibition of Bacterial U(VI) Reduction by Calcium Brooks, Scott C.; Fredrickson, James K.; Carroll, Sue L. Environmental Science & Technology, Vol. 37, Issue 9 https://doi.org/10.1021/es0210042	journal	May 2003
Structure and occurrences of ≪ green rust ≫ related new minerals of the ≪ fougérite ≫ group, trébeurdenite and mössbauerite, belonging to the ≪ hydrotalcite ≫ supergroup; how Mössbauer spectroscopy helps XRD. Génin, J. -M. R.; Christy, A.; Kuzmann, E. Hyperfine Interactions, Vol. 226, Issue 1-3 https://doi.org/10.1007/s10751-014-1045-4	journal	April 2014
The anionic species competition in iron aqueous corrosion: Role of various green rust compounds Refait, Ph.; Drissi, S. H.; Pytkiewicz, J. Corrosion Science, Vol. 39, Issue 9 https://doi.org/10.1016/S0010-938X(97)00076-0	journal	September 1997
Mechanisms of formation and structure of green rust one in aqueous corrosion of iron in the presence of chloride ions Refait, Ph.; Abdelmoula, M.; GÉnin, J. -M. R. Corrosion Science, Vol. 40, Issue 9 https://doi.org/10.1016/S0010-938X(98)00066-3	journal	September 1998
Microbial Reductive Transformation of Phyllosilicate Fe(III) and U(VI) in Fluvial Subsurface Sediments Lee, Ji-Hoon; Fredrickson, James K.; Kukkadapu, Ravi K. Environmental Science & Technology, Vol. 46, Issue 7 https://doi.org/10.1021/es204528m	journal	March 2012
Ferrozine---a new spectrophotometric reagent for iron Stookey, Lawrence L. Analytical Chemistry, Vol. 42, Issue 7, p. 779-781 https://doi.org/10.1021/ac60289a016	journal	June 1970
The effect of sample matrix quenching on the measurement of trace uranium concentrations in aqueous solutions using kinetic phosphorimetry Sowder, A. G.; Clark, S. B.; Fjeld, R. A. Journal of Radioanalytical and Nuclear Chemistry, Vol. 234, Issue 1-2 https://doi.org/10.1007/BF02389781	journal	August 1998
Determination of the Formation Constants of Ternary Complexes of Uranyl and Carbonate with Alkaline Earth Metals (Mg ²⁺ , Ca ²⁺ , Sr ²⁺ , and Ba ²⁺ ) Using Anion Exchange Method Dong, Wenming; Brooks, Scott C. Environmental Science & Technology, Vol. 40, Issue 15 https://doi.org/10.1021/es0606327	journal	August 2006
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT Ravel, B.; Newville, M. Journal of Synchrotron Radiation, Vol. 12, Issue 4 https://doi.org/10.1107/S0909049505012719	journal	June 2005
Abiotic Reductive Immobilization of U(VI) by Biogenic Mackinawite Veeramani, Harish; Scheinost, Andreas C.; Monsegue, Niven Environmental Science & Technology, Vol. 47, Issue 5 https://doi.org/10.1021/es304025x	journal	February 2013
Products of abiotic U(VI) reduction by biogenic magnetite and vivianite Veeramani, Harish; Alessi, Daniel S.; Suvorova, Elena I. Geochimica et Cosmochimica Acta, Vol. 75, Issue 9 https://doi.org/10.1016/j.gca.2011.02.024	journal	May 2011
Association of Uranium with Iron Oxides Typically Formed on Corroding Steel Surfaces Dodge, C. J.; Francis, A. J.; Gillow, J. B. Environmental Science & Technology, Vol. 36, Issue 16 https://doi.org/10.1021/es011450+	journal	July 2002
Reductive Precipitation of Uranium(VI) by Zero-Valent Iron Gu, B.; Liang, L.; Dickey, M. J. Environmental Science & Technology, Vol. 32, Issue 21 https://doi.org/10.1021/es980010o	journal	November 1998
Uranium(VI) Removal by Nanoscale Zerovalent Iron in Anoxic Batch Systems Yan, Sen; Hua, Bin; Bao, Zhengyu Environmental Science & Technology, Vol. 44, Issue 20 https://doi.org/10.1021/es9036308	journal	October 2010
Quantitative Separation of Monomeric U(IV) from UO ₂ in Products of U(VI) Reduction Alessi, Daniel S.; Uster, Benjamin; Veeramani, Harish Environmental Science & Technology, Vol. 46, Issue 11 https://doi.org/10.1021/es204123z	journal	May 2012
Stable U(IV) Complexes Form at High-Affinity Mineral Surface Sites Latta, Drew E.; Mishra, Bhoopesh; Cook, Russell E. Environmental Science & Technology, Vol. 48, Issue 3 https://doi.org/10.1021/es4047389	journal	January 2014
U(VI) Reduction to Mononuclear U(IV) by Desulfitobacterium Species Fletcher, Kelly E.; Boyanov, Maxim I.; Thomas, Sara H. Environmental Science & Technology, Vol. 44, Issue 12 https://doi.org/10.1021/es903636c	journal	June 2010
Low-temperature ordered phase of CaU(PO4)2: synthesis and crystal structure [Low-temperature ordered phase of CaU(PO4)2: synthesis and crystal structure] Dusausoy, Yves; Ghermani, Nοur-Eddine; Podor, Renaud European Journal of Mineralogy, Vol. 8, Issue 4 https://doi.org/10.1127/ejm/8/4/0667	journal	July 1996
Adsorption of Fe(II) and U(VI) to carboxyl-functionalized microspheres: The influence of speciation on uranyl reduction studied by titration and XAFS Boyanov, Maxim I.; O’Loughlin, Edward J.; Roden, Eric E. Geochimica et Cosmochimica Acta, Vol. 71, Issue 8 https://doi.org/10.1016/j.gca.2007.01.025	journal	April 2007
Uranium(IV) adsorption by natural organic matter in anoxic sediments Bone, Sharon E.; Dynes, James J.; Cliff, John Proceedings of the National Academy of Sciences, Vol. 114, Issue 4 https://doi.org/10.1073/pnas.1611918114	journal	January 2017
Formation of Ferrihydrite and Associated Iron Corrosion Products in Permeable Reactive Barriers of Zero-Valent Iron Furukawa, Yoko; Kim, Jin-wook; Watkins, Janet Environmental Science & Technology, Vol. 36, Issue 24 https://doi.org/10.1021/es025533h	journal	December 2002
Mineralogical Characteristics and Transformations during Long‐Term Operation of a Zerovalent Iron Reactive Barrier Phillips, D. H.; Watson, D. B.; Roh, Y. Journal of Environmental Quality, Vol. 32, Issue 6 https://doi.org/10.2134/jeq2003.2033	journal	November 2003
Quantifying Constraints Imposed by Calcium and Iron on Bacterial Reduction of Uranium(VI) Stewart, Brandy D.; Neiss, Jim; Fendorf, Scott Journal of Environment Quality, Vol. 36, Issue 2 https://doi.org/10.2134/jeq2006.0058	journal	January 2007

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