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

Abstract

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.

Authors:

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)

Publication Date:: 2018-04-09

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

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

OSTI Identifier:: 1437378

Grant/Contract Number:: AC02-06CH11357

Resource Type:: Accepted Manuscript

Journal Name:: Environmental Science and Technology

Additional Journal Information:: Journal Volume: 52; Journal Issue: 8; Journal ID: ISSN 0013-936X

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats


                    Yan, Sen, Boyanov, Maxim I., Mishra, Bhoopesh, Kemner, Kenneth M., and O'Loughlin, Edward J. U(VI) Reduction by Biogenic and Abiotic Hydroxycarbonate Green Rusts: Impacts on U(IV) Speciation and Stability Over Time.  United States: N. p., 2018. 
Web.  doi:10.1021/acs.est.7b06405.

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                    Yan, Sen, Boyanov, Maxim I., Mishra, Bhoopesh, Kemner, Kenneth M., & O'Loughlin, Edward J. U(VI) Reduction by Biogenic and Abiotic Hydroxycarbonate Green Rusts: Impacts on U(IV) Speciation and Stability Over Time.  United States.  https://doi.org/10.1021/acs.est.7b06405

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                    Yan, Sen, Boyanov, Maxim I., Mishra, Bhoopesh, Kemner, Kenneth M., and O'Loughlin, Edward J. Mon .  
"U(VI) Reduction by Biogenic and Abiotic Hydroxycarbonate Green Rusts: Impacts on U(IV) Speciation and Stability Over Time".  United States.  https://doi.org/10.1021/acs.est.7b06405.  https://www.osti.gov/servlets/purl/1437378.

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@article{osti_1437378,

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

  author       = {Yan, Sen and Boyanov, Maxim I. and Mishra, Bhoopesh and Kemner, Kenneth M. and O'Loughlin, Edward J.},

  abstractNote = {Green rusts (GRs) are redox active FeII-FeIII 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 UVI, the dynamics of the transformations and the speciation and stability of the resulting UIV phases are poorly understood. We used carbonate extraction and XAFS spectroscopy to investigate the products of UVI reduction by BioGR and ChemGR. The results show that both GRs can rapidly remove UVI from synthetic groundwater via reduction to UIV. The initial products in the ChemGR system are solids-associated UIV-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 UIV atoms in the BioGR system remain relatively extractable, non-uraninite UIV species over the same reaction period. The presence of calcium and carbonate in groundwater significantly increase the extractability of UIV 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.},

  doi          = {10.1021/acs.est.7b06405},

  journal      = {Environmental Science and Technology},

  number       = 8,

  volume       = 52,

  place        = {United States},

  year         = {2018},

  month        = {4}

}

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

Abstract

Citation Formats

Speciation of Uranium in Sediments before and after In situ Biostimulation journal, March 2008

Uranium redox transition pathways in acetate-amended sediments journal, March 2013

Evaluating Chemical Extraction Techniques for the Determination of Uranium Oxidation State in Reduced Aquifer Sediments journal, August 2013

Solution and Microbial Controls on the Formation of Reduced U(IV) Species journal, October 2011

Effects of calcium and phosphate on uranium(IV) oxidation: Comparison between nanoparticulate uraninite and amorphous UIV–phosphate journal, February 2016

Surface area effects on the reduction of UVI in the presence of synthetic montmorillonite journal, August 2017

Green rust formation controls nutrient availability in a ferruginous water column journal, July 2012

Identification of Green Rust in Groundwater journal, May 2009

Observations and assessment of iron oxide and green rust nanoparticles in metal-polluted mine drainage within a steep redox gradient journal, January 2014

Identification of a green rust mineral in a reductomorphic soil by Mossbauer and Raman spectroscopies 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 journal, April 1998

In situ Mössbauer spectroscopy: Evidence for green rust (fougerite) in a gleysol and its mineralogical transformations with time and depth journal, September 2005

Identification of green rust in an ochre sludge journal, December 1991

Fe(II)/Fe(III) ‘green rust’ developed within ochreous coal mine drainage sediment in South Wales, UK journal, December 2006

Arsenic sequestration by sorption processes in high-iron sediments journal, December 2007

Abiotic Transformation of Hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) by Green Rusts journal, June 2008

Reduction of Halogenated Ethanes by Green rust journal, January 2004

Kinetics of Cr(VI) Reduction by Carbonate Green Rust journal, September 2001

Reduction of AgI, AuIII, CuII, and HgII by FeII/FeIII hydroxysulfate green rust journal, November 2003

Nitrite Reduction by Biogenic Hydroxycarbonate Green Rusts: Evidence for Hydroxy-nitrite Green Rust Formation as an Intermediate Reaction Product 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 journal, October 2014

Fougerite: From field experiment to the homologation of the mineral journal, December 2006

Bioreduction of ferric species and biogenesis of green rusts in soils journal, June 2006

Biogenic Magnetite Formation through Anaerobic Biooxidation of Fe(II) journal, June 2001

Green Rust Formation during Fe(II) Oxidation by the Nitrate-Reducing Acidovorax sp. Strain BoFeN1 journal, January 2012

Formation of green rust via mineralogical transformation of ferric oxides (ferrihydrite, goethite and hematite) journal, August 2012

Abiotic Process for Fe(II) Oxidation and Green Rust Mineralization Driven by a Heterotrophic Nitrate Reducing Bacteria ( Klebsiella mobilis ) journal, March 2014

Effects of Phosphate on Secondary Mineral Formation During the Bioreduction of Akaganeite (.β-FeOOH): Green Rust Versus Framboidal Magnetite journal, July 2015

Magnetite as a precursor for green rust through the hydrogenotrophic activity of the iron-reducing bacteria Shewanella putrefaciens journal, December 2015

Origin of the Differential Nanoscale Reactivity of Biologically and Chemically Formed Green Rust Crystals Investigated by Chemical Force Spectroscopy 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) journal, March 2015

Reduction of Uranium(VI) by Mixed Iron(II)/Iron(III) Hydroxide (Green Rust): Formation of UO 2 Nanoparticles journal, February 2003

XAFS Investigation of the Interactions of U VI with Secondary Mineralization Products from the Bioreduction of Fe III Oxides journal, March 2010

Reaction of Uranium(VI) with Green Rusts: Effect of Interlayer Anion journal, July 2015

Inhibition of Bacterial U(VI) Reduction by Calcium 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. journal, April 2014

The anionic species competition in iron aqueous corrosion: Role of various green rust compounds journal, September 1997

Mechanisms of formation and structure of green rust one in aqueous corrosion of iron in the presence of chloride ions journal, September 1998

Microbial Reductive Transformation of Phyllosilicate Fe(III) and U(VI) in Fluvial Subsurface Sediments journal, March 2012

Ferrozine---a new spectrophotometric reagent for iron journal, June 1970

The effect of sample matrix quenching on the measurement of trace uranium concentrations in aqueous solutions using kinetic phosphorimetry 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 journal, August 2006

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT journal, June 2005

Abiotic Reductive Immobilization of U(VI) by Biogenic Mackinawite journal, February 2013

Products of abiotic U(VI) reduction by biogenic magnetite and vivianite journal, May 2011

Reductive Precipitation of Uranium(VI) by Zero-Valent Iron journal, November 1998

Uranium(VI) Removal by Nanoscale Zerovalent Iron in Anoxic Batch Systems journal, October 2010

Quantitative Separation of Monomeric U(IV) from UO 2 in Products of U(VI) Reduction journal, May 2012

Stable U(IV) Complexes Form at High-Affinity Mineral Surface Sites journal, January 2014

U(VI) Reduction to Mononuclear U(IV) by Desulfitobacterium Species 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] 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 journal, April 2007

Uranium(IV) adsorption by natural organic matter in anoxic sediments journal, January 2017

Formation of Ferrihydrite and Associated Iron Corrosion Products in Permeable Reactive Barriers of Zero-Valent Iron journal, December 2002

Mineralogical Characteristics and Transformations during Long‐Term Operation of a Zerovalent Iron Reactive Barrier journal, November 2003

Quantifying Constraints Imposed by Calcium and Iron on Bacterial Reduction of Uranium(VI) journal, January 2007

Electron Donor Utilization and Secondary Mineral Formation during the Bioreduction of Lepidocrocite by Shewanella putrefaciens CN32 journal, July 2019

Speciation of Uranium in Sediments before and after In situ Biostimulation
journal, March 2008

Uranium redox transition pathways in acetate-amended sediments
journal, March 2013

Evaluating Chemical Extraction Techniques for the Determination of Uranium Oxidation State in Reduced Aquifer Sediments
journal, August 2013

Solution and Microbial Controls on the Formation of Reduced U(IV) Species
journal, October 2011

Effects of calcium and phosphate on uranium(IV) oxidation: Comparison between nanoparticulate uraninite and amorphous UIV–phosphate
journal, February 2016

Surface area effects on the reduction of UVI in the presence of synthetic montmorillonite
journal, August 2017

Green rust formation controls nutrient availability in a ferruginous water column
journal, July 2012

Identification of Green Rust in Groundwater
journal, May 2009

Observations and assessment of iron oxide and green rust nanoparticles in metal-polluted mine drainage within a steep redox gradient
journal, January 2014

Identification of a green rust mineral in a reductomorphic soil by Mossbauer and Raman spectroscopies
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
journal, April 1998

In situ Mössbauer spectroscopy: Evidence for green rust (fougerite) in a gleysol and its mineralogical transformations with time and depth
journal, September 2005

Identification of green rust in an ochre sludge
journal, December 1991

Fe(II)/Fe(III) ‘green rust’ developed within ochreous coal mine drainage sediment in South Wales, UK
journal, December 2006

Arsenic sequestration by sorption processes in high-iron sediments
journal, December 2007

Abiotic Transformation of Hexahydro-1,3,5-trinitro-1,3,5-triazine (RDX) by Green Rusts
journal, June 2008

Reduction of Halogenated Ethanes by Green rust
journal, January 2004

Kinetics of Cr(VI) Reduction by Carbonate Green Rust
journal, September 2001

Reduction of AgI, AuIII, CuII, and HgII by FeII/FeIII hydroxysulfate green rust
journal, November 2003

Nitrite Reduction by Biogenic Hydroxycarbonate Green Rusts: Evidence for Hydroxy-nitrite Green Rust Formation as an Intermediate Reaction Product
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
journal, October 2014

Fougerite: From field experiment to the homologation of the mineral
journal, December 2006

Bioreduction of ferric species and biogenesis of green rusts in soils
journal, June 2006

Biogenic Magnetite Formation through Anaerobic Biooxidation of Fe(II)
journal, June 2001

Green Rust Formation during Fe(II) Oxidation by the Nitrate-Reducing Acidovorax sp. Strain BoFeN1
journal, January 2012

Formation of green rust via mineralogical transformation of ferric oxides (ferrihydrite, goethite and hematite)
journal, August 2012

Abiotic Process for Fe(II) Oxidation and Green Rust Mineralization Driven by a Heterotrophic Nitrate Reducing Bacteria ( Klebsiella mobilis )
journal, March 2014

Effects of Phosphate on Secondary Mineral Formation During the Bioreduction of Akaganeite (.β-FeOOH): Green Rust Versus Framboidal Magnetite
journal, July 2015

Magnetite as a precursor for green rust through the hydrogenotrophic activity of the iron-reducing bacteria Shewanella putrefaciens
journal, December 2015

Origin of the Differential Nanoscale Reactivity of Biologically and Chemically Formed Green Rust Crystals Investigated by Chemical Force Spectroscopy
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)
journal, March 2015

Reduction of Uranium(VI) by Mixed Iron(II)/Iron(III) Hydroxide (Green Rust): Formation of UO ₂ Nanoparticles
journal, February 2003

XAFS Investigation of the Interactions of U ^VI with Secondary Mineralization Products from the Bioreduction of Fe ^III Oxides
journal, March 2010

Reaction of Uranium(VI) with Green Rusts: Effect of Interlayer Anion
journal, July 2015

Inhibition of Bacterial U(VI) Reduction by Calcium
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.
journal, April 2014

The anionic species competition in iron aqueous corrosion: Role of various green rust compounds
journal, September 1997

Mechanisms of formation and structure of green rust one in aqueous corrosion of iron in the presence of chloride ions
journal, September 1998

Microbial Reductive Transformation of Phyllosilicate Fe(III) and U(VI) in Fluvial Subsurface Sediments
journal, March 2012

Ferrozine---a new spectrophotometric reagent for iron
journal, June 1970

The effect of sample matrix quenching on the measurement of trace uranium concentrations in aqueous solutions using kinetic phosphorimetry
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
journal, August 2006

ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT
journal, June 2005

Abiotic Reductive Immobilization of U(VI) by Biogenic Mackinawite
journal, February 2013

Products of abiotic U(VI) reduction by biogenic magnetite and vivianite
journal, May 2011

Reductive Precipitation of Uranium(VI) by Zero-Valent Iron
journal, November 1998

Uranium(VI) Removal by Nanoscale Zerovalent Iron in Anoxic Batch Systems
journal, October 2010

Quantitative Separation of Monomeric U(IV) from UO ₂ in Products of U(VI) Reduction
journal, May 2012

Stable U(IV) Complexes Form at High-Affinity Mineral Surface Sites
journal, January 2014

U(VI) Reduction to Mononuclear U(IV) by Desulfitobacterium Species
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]
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
journal, April 2007

Uranium(IV) adsorption by natural organic matter in anoxic sediments
journal, January 2017

Formation of Ferrihydrite and Associated Iron Corrosion Products in Permeable Reactive Barriers of Zero-Valent Iron
journal, December 2002

Mineralogical Characteristics and Transformations during Long‐Term Operation of a Zerovalent Iron Reactive Barrier
journal, November 2003

Quantifying Constraints Imposed by Calcium and Iron on Bacterial Reduction of Uranium(VI)
journal, January 2007

Electron Donor Utilization and Secondary Mineral Formation during the Bioreduction of Lepidocrocite by Shewanella putrefaciens CN32
journal, July 2019