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Title: Combined Effects of Fe(III)-Bearing Clay Minerals and Organic Ligands on U(VI) Bioreduction and U(IV) Speciation

Abstract

Reduction of U(VI) to U(IV) drastically reduces its solubility and has been proposed as a method for remediation of uranium contamination. However, much is still unknown about the kinetics, mechanisms, and products of U(VI) bioreduction in complex systems. In this work, U(VI) bioreduction experiments were conducted with Shewanella putrefaciens strain CN32 in the presence of clay minerals and two organic ligands: citrate and EDTA. In reactors with U and Fe(III)-clay minerals, the rate of U(VI) bioreduction was enhanced due to the presence of ligands, likely because soluble Fe3+- and Fe2+-ligand complexes served as electron shuttles. In the presence of citrate, bioreduced U(IV) formed a soluble U(IV)-citrate complex in experiments with either Fe-rich or Fe-poor clay mineral. In the presence of EDTA, U(IV) occurred as a soluble U(IV)-EDTA complex in Fe-poor montmorillonite experiments. However, U(IV) remained associated with the solid phase in Fe-rich nontronite experiments through the formation of a ternary U(IV)-EDTA-surface complex, as suggested by the EXAFS analysis. Our study indicates that organic ligands and Fe(III)-bearing clays can significantly affect the microbial reduction of U(VI) and the stability of the resulting U(IV) phase.

Authors:
 [1];  [2];  [2];  [3];  [3]; ORCiD logo [3];  [4];  [5];  [6]; ORCiD logo [2];  [7]
+ Show Author Affiliations
  1. China Univ. of Geosciences, Beijing (China); Chinese Academy of Sciences (CAS), Beijing (China)
  2. China Univ. of Geosciences, Beijing (China)
  3. Argonne National Lab. (ANL), Argonne, IL (United States)
  4. Ecole Polytechnique Federale Lausanne (Switzerland)
  5. Fudan Univ., Shanghai (China)
  6. Chinese Academy of Sciences (CAS), Beijing (China)
  7. Argonne National Lab. (ANL), Argonne, IL (United States); Bulgarian Academy of Sciences, Sofia (Bulgaria)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Biological and Environmental Research (BER); National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1798054
Grant/Contract Number:  
AC02-06CH11357; 41630103
Resource Type:
Accepted Manuscript
Journal Name:
Environmental Science and Technology
Additional Journal Information:
Journal Volume: 55; Journal Issue: 9; 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; redox reactions; uranium; ligands; minerals; clay

Citation Formats

Zhang, Limin, Chen, Yu, Xia, Qingyin, Kemner, Kenneth M., Shen, Yanghao, O’Loughlin, Edward J., Pan, Zezhen, Wang, Qihuang, Huang, Ying, Dong, Hailiang, and Boyanov, Maxim I. Combined Effects of Fe(III)-Bearing Clay Minerals and Organic Ligands on U(VI) Bioreduction and U(IV) Speciation. United States: N. p., 2021. Web. doi:10.1021/acs.est.0c08645.
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Zhang, Limin, Chen, Yu, Xia, Qingyin, Kemner, Kenneth M., Shen, Yanghao, O’Loughlin, Edward J., Pan, Zezhen, Wang, Qihuang, Huang, Ying, Dong, Hailiang, & Boyanov, Maxim I. Combined Effects of Fe(III)-Bearing Clay Minerals and Organic Ligands on U(VI) Bioreduction and U(IV) Speciation. United States. https://doi.org/10.1021/acs.est.0c08645
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Zhang, Limin, Chen, Yu, Xia, Qingyin, Kemner, Kenneth M., Shen, Yanghao, O’Loughlin, Edward J., Pan, Zezhen, Wang, Qihuang, Huang, Ying, Dong, Hailiang, and Boyanov, Maxim I. Tue . "Combined Effects of Fe(III)-Bearing Clay Minerals and Organic Ligands on U(VI) Bioreduction and U(IV) Speciation". United States. https://doi.org/10.1021/acs.est.0c08645. https://www.osti.gov/servlets/purl/1798054.
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@article{osti_1798054,
title = {Combined Effects of Fe(III)-Bearing Clay Minerals and Organic Ligands on U(VI) Bioreduction and U(IV) Speciation},
author = {Zhang, Limin and Chen, Yu and Xia, Qingyin and Kemner, Kenneth M. and Shen, Yanghao and O’Loughlin, Edward J. and Pan, Zezhen and Wang, Qihuang and Huang, Ying and Dong, Hailiang and Boyanov, Maxim I.},
abstractNote = {Reduction of U(VI) to U(IV) drastically reduces its solubility and has been proposed as a method for remediation of uranium contamination. However, much is still unknown about the kinetics, mechanisms, and products of U(VI) bioreduction in complex systems. In this work, U(VI) bioreduction experiments were conducted with Shewanella putrefaciens strain CN32 in the presence of clay minerals and two organic ligands: citrate and EDTA. In reactors with U and Fe(III)-clay minerals, the rate of U(VI) bioreduction was enhanced due to the presence of ligands, likely because soluble Fe3+- and Fe2+-ligand complexes served as electron shuttles. In the presence of citrate, bioreduced U(IV) formed a soluble U(IV)-citrate complex in experiments with either Fe-rich or Fe-poor clay mineral. In the presence of EDTA, U(IV) occurred as a soluble U(IV)-EDTA complex in Fe-poor montmorillonite experiments. However, U(IV) remained associated with the solid phase in Fe-rich nontronite experiments through the formation of a ternary U(IV)-EDTA-surface complex, as suggested by the EXAFS analysis. Our study indicates that organic ligands and Fe(III)-bearing clays can significantly affect the microbial reduction of U(VI) and the stability of the resulting U(IV) phase.},
doi = {10.1021/acs.est.0c08645},
journal = {Environmental Science and Technology},
number = 9,
volume = 55,
place = {United States},
year = {Tue Apr 06 00:00:00 EDT 2021},
month = {Tue Apr 06 00:00:00 EDT 2021}
}
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Works referenced in this record:

Bioremediation of uranium-contaminated groundwater: a systems approach to subsurface biogeochemistry
journal, June 2013

  • Williams, Kenneth H.; Bargar, John R.; Lloyd, Jonathan R.
  • Current Opinion in Biotechnology, Vol. 24, Issue 3
  • DOI: 10.1016/j.copbio.2012.10.008

Thermodynamic Controls on the Microbial Reduction of Iron-Bearing Nontronite and Uranium
journal, February 2014

  • Luan, Fubo; Gorski, Christopher A.; Burgos, William D.
  • Environmental Science & Technology, Vol. 48, Issue 5
  • DOI: 10.1021/es404885e

Bicarbonate impact on U(VI) bioreduction in a shallow alluvial aquifer
journal, February 2015

  • Long, Philip E.; Williams, Kenneth H.; Davis, James A.
  • Geochimica et Cosmochimica Acta, Vol. 150
  • DOI: 10.1016/j.gca.2014.11.013

Uranium Reduction by Fe(II) in the Presence of Montmorillonite and Nontronite
journal, July 2016

  • Tsarev, Sergey; Waite, T. David; Collins, Richard N.
  • Environmental Science & Technology, Vol. 50, Issue 15
  • DOI: 10.1021/acs.est.6b02000

Cathodic Action of the Uranyl-Lactate Complex at the Dropping Mercury Electrode.
journal, June 1963

  • Lai, Tsai-Teh.; Wang, Bi-Cheng.
  • Analytical Chemistry, Vol. 35, Issue 7
  • DOI: 10.1021/ac60200a040

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

  • Stookey, Lawrence L.
  • Analytical Chemistry, Vol. 42, Issue 7, p. 779-781
  • DOI: 10.1021/ac60289a016

Anoxic storage regenerates reactive Fe(II) in reduced nontronite with short-term oxidation
journal, July 2019

The biogeochemistry and bioremediation of uranium and other priority radionuclides
journal, January 2014

Mechanisms of electron transfer from structrual Fe(II) in reduced nontronite to oxygen for production of hydroxyl radicals
journal, February 2018

Effects of Citrate, NTA, and EDTA on the Reduction of U(VI) by Shewanella putrefaciens
journal, April 2010

Biological Redox Cycling of Iron in Nontronite and Its Potential Application in Nitrate Removal
journal, April 2015

  • Zhao, Linduo; Dong, Hailiang; Kukkadapu, Ravi K.
  • Environmental Science & Technology, Vol. 49, Issue 9
  • DOI: 10.1021/acs.est.5b00131

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

  • O’Loughlin, Edward J.; Kelly, Shelly D.; Kemner, Kenneth M.
  • Environmental Science & Technology, Vol. 44, Issue 5
  • DOI: 10.1021/es9027953

U(VI) Reduction to Mononuclear U(IV) by Desulfitobacterium Species
journal, June 2010

  • Fletcher, Kelly E.; Boyanov, Maxim I.; Thomas, Sara H.
  • Environmental Science & Technology, Vol. 44, Issue 12
  • DOI: 10.1021/es903636c

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

  • Latta, Drew E.; Mishra, Bhoopesh; Cook, Russell E.
  • Environmental Science & Technology, Vol. 48, Issue 3
  • DOI: 10.1021/es4047389

Uranium(VI) Interactions with Mackinawite in the Presence and Absence of Bicarbonate and Oxygen
journal, June 2013

  • Gallegos, Tanya J.; Fuller, Christopher C.; Webb, Samuel M.
  • Environmental Science & Technology, Vol. 47, Issue 13
  • DOI: 10.1021/es400450z

U(VI) Sorption and Reduction Kinetics on the Magnetite (111) Surface
journal, March 2012

  • Singer, David M.; Chatman, Shawn M.; Ilton, Eugene S.
  • Environmental Science & Technology, Vol. 46, Issue 7
  • DOI: 10.1021/es203878c

Enhancing uranium solubilization in soils by citrate, EDTA, and EDDS chelating amendments
journal, December 2011

Microbial reduction of uranium
journal, April 1991

  • Lovley, Derek R.; Phillips, Elizabeth J. P.; Gorby, Yuri A.
  • Nature, Vol. 350, Issue 6317
  • DOI: 10.1038/350413a0

Determination of Stability Constants of U(VI)−Fe(III)−Citrate Complexes
journal, April 2005

  • Kantar, Cetin; Gillow, Jeff B.; Harper-Arabie, Ruth
  • Environmental Science & Technology, Vol. 39, Issue 7
  • DOI: 10.1021/es048852c

Direct detection of trace levels of uranium by laser-induced kinetic phosphorimetry
journal, July 1992

  • Brina, Rossella.; Miller, Allan G.
  • Analytical Chemistry, Vol. 64, Issue 13
  • DOI: 10.1021/ac00037a020

Aqueous speciation and pH effect on the sorption behavior of uranium by montmorillonite
journal, November 1998

  • Akçay, H.
  • Journal of Radioanalytical and Nuclear Chemistry, Vol. 237, Issue 1-2
  • DOI: 10.1007/BF02386676

Uranium Redox Transformations after U(VI) Coprecipitation with Magnetite Nanoparticles
journal, February 2017

  • Pidchenko, Ivan; Kvashnina, Kristina O.; Yokosawa, Tadahiro
  • Environmental Science & Technology, Vol. 51, Issue 4
  • DOI: 10.1021/acs.est.6b04035

Influence of Chelating Agents on Biogenic Uraninite Reoxidation by Fe(III) (Hydr)oxides
journal, August 2012

  • Stewart, Brandy D.; Girardot, Crystal; Spycher, Nicolas
  • Environmental Science & Technology, Vol. 47, Issue 1
  • DOI: 10.1021/es303022p

Spectroscopic Confirmation of Uranium(VI)−Carbonato Adsorption Complexes on Hematite
journal, July 1999

  • Bargar, John R.; Reitmeyer, Rebecca; Davis, James A.
  • Environmental Science & Technology, Vol. 33, Issue 14
  • DOI: 10.1021/es990048g

In Situ Bioremediation of Uranium with Emulsified Vegetable Oil as the Electron Donor
journal, May 2013

  • Watson, David B.; Wu, Wei-Min; Mehlhorn, Tonia
  • Environmental Science & Technology, Vol. 47, Issue 12
  • DOI: 10.1021/es3033555

Bioreduction of Uranium(VI) Complexed with Citric Acid by Clostridia Affects Its Structure and Solubility
journal, November 2008

  • Francis, A. J.; Dodge, C. J.
  • Environmental Science & Technology, Vol. 42, Issue 22
  • DOI: 10.1021/es801045m

Microbial Reduction of Structural Fe(III) in Illite and Goethite
journal, April 2003

  • Dong, Hailiang; Kukkadapu, Ravi K.; Fredrickson, James K.
  • Environmental Science & Technology, Vol. 37, Issue 7
  • DOI: 10.1021/es020919d

Mobile uranium(IV)-bearing colloids in a mining-impacted wetland
journal, December 2013

  • Wang, Yuheng; Frutschi, Manon; Suvorova, Elena
  • Nature Communications, Vol. 4, Issue 1
  • DOI: 10.1038/ncomms3942

Potential for Nonenzymatic Reduction of Fe(III) via Electron Shuttling in Subsurface Sediments
journal, June 2000

  • Nevin, Kelly P.; Lovley, Derek R.
  • Environmental Science & Technology, Vol. 34, Issue 12
  • DOI: 10.1021/es991181b

Fe(II)–Fe(III) Electron Transfer in a Clay Mineral with Low Fe Content
journal, May 2017

Uranium(VI) Reduction by Anaeromyxobacter dehalogenans Strain 2CP-C
journal, May 2006

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

  • Alessi, Daniel S.; Uster, Benjamin; Veeramani, Harish
  • Environmental Science & Technology, Vol. 46, Issue 11
  • DOI: 10.1021/es204123z

Reduction of Actinides and Fission Products by Fe(III)-Reducing Bacteria
journal, January 2002

Soil Humic Acid Decreases Biological Uranium(VI) Reduction by Shewanella putrefaciens CN32
journal, July 2007

  • Burgos, William D.; Senko, John M.; Dempsey, Brian A.
  • Environmental Engineering Science, Vol. 24, Issue 6
  • DOI: 10.1089/ees.2006.0009

Spectroscopic Evidence for Fe(II)–Fe(III) Electron Transfer at Clay Mineral Edge and Basal Sites
journal, March 2013

  • Neumann, Anke; Olson, Tyler L.; Scherer, Michelle M.
  • Environmental Science & Technology, Vol. 47, Issue 13
  • DOI: 10.1021/es304744v

Effect of ligands on the production of oxidants from oxygenation of reduced Fe-bearing clay mineral nontronite
journal, April 2019

Effects of redox cycling of iron in nontronite on reduction of technetium
journal, January 2012

Acetate Availability and its Influence on Sustainable Bioremediation of Uranium-Contaminated Groundwater
journal, June 2011

Physicochemical and Mineralogical Characterization of Uranium-Contaminated Soils
journal, September 2000

Redox Interactions of Tc(VII), U(VI), and Np(V) with Microbially Reduced Biotite and Chlorite
journal, November 2015

  • Brookshaw, Diana R.; Pattrick, Richard A. D.; Bots, Pieter
  • Environmental Science & Technology, Vol. 49, Issue 22
  • DOI: 10.1021/acs.est.5b03463

XPS and XANES Studies of Uranium Reduction by Clostridium sp
journal, April 1994

  • Francis, Arokiasamy J.; Dodge, Cleveland J.; Lu, Fulong.
  • Environmental Science & Technology, Vol. 28, Issue 4
  • DOI: 10.1021/es00053a016

Multiple Lines of Evidence Identify U(V) as a Key Intermediate during U(VI) Reduction by Shewanella oneidensis MR1
journal, January 2020

  • Vettese, Gianni F.; Morris, Katherine; Natrajan, Louise S.
  • Environmental Science & Technology, Vol. 54, Issue 4
  • DOI: 10.1021/acs.est.9b05285

The influence of citric acid, EDTA, and fulvic acid on U(VI) sorption onto kaolinite
journal, June 2011

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

  • O'Loughlin, Edward J.; Kelly, Shelly D.; Cook, Russell E.
  • Environmental Science & Technology, Vol. 37, Issue 4
  • DOI: 10.1021/es0208409

Bioleaching of rare earth elements from bastnaesite-bearing rock by actinobacteria
journal, April 2018

Speciation of An(IV) (Pu, Np, U and Th) in citrate media
journal, January 2008

Respiration and Dissolution of Iron(III)-Containing Clay Minerals by Bacteria
journal, September 1999

  • Kostka, Joel E.; Haefele, Eberhard; Viehweger, Ralf
  • Environmental Science & Technology, Vol. 33, Issue 18
  • DOI: 10.1021/es990021x

Metaschoepite Dissolution in Sediment Column Systems—Implications for Uranium Speciation and Transport
journal, July 2019

  • Bower, William R.; Morris, Katherine; Livens, Francis R.
  • Environmental Science & Technology, Vol. 53, Issue 16
  • DOI: 10.1021/acs.est.9b02292

Microbe-clay mineral interactions
journal, November 2009

  • Dong, H.; Jaisi, D. P.; Kim, J.
  • American Mineralogist, Vol. 94, Issue 11-12
  • DOI: 10.2138/am.2009.3246

Rapid immobilisation of U(VI) by Eucalyptus bark: Adsorption without reduction
journal, September 2018

Degradation of 1, 4-dioxane by hydroxyl radicals produced from clay minerals
journal, June 2017

Surface catalysis of uranium(VI) reduction by iron(II)
journal, October 1999

  • Liger, Emmanuelle; Charlet, Laurent; Van Cappellen, Philippe
  • Geochimica et Cosmochimica Acta, Vol. 63, Issue 19-20
  • DOI: 10.1016/S0016-7037(99)00265-3

U(VI) Sorption and Reduction by Fe(II) Sorbed on Montmorillonite
journal, May 2010

  • Chakraborty, Sudipta; Favre, Fabienne; Banerjee, Dipanjan
  • Environmental Science & Technology, Vol. 44, Issue 10
  • DOI: 10.1021/es903493n

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

  • Boyanov, Maxim I.; Fletcher, Kelly E.; Kwon, Man Jae
  • Environmental Science & Technology, Vol. 45, Issue 19
  • DOI: 10.1021/es2014049

The effect of U(VI) bioreduction kinetics on subsequent reoxidation of biogenic U(IV)
journal, October 2007

  • Senko, John M.; Kelly, Shelly D.; Dohnalkova, Alice C.
  • Geochimica et Cosmochimica Acta, Vol. 71, Issue 19
  • DOI: 10.1016/j.gca.2007.07.021

Dissolution of Uranium-Bearing Minerals and Mobilization of Uranium by Organic Ligands in a Biologically Reduced Sediment
journal, April 2011

  • Luo, Wensui; Gu, Baohua
  • Environmental Science & Technology, Vol. 45, Issue 7
  • DOI: 10.1021/es103073u

Organic complexation of U(VI) in reducing soils at a natural analogue site: Implications for uranium transport
journal, September 2020

Characterization of U(VI)-carbonato ternary complexes on hematite: EXAFS and electrophoretic mobility measurements
journal, August 2000

Iron and Manganese in Anaerobic Respiration: Environmental Significance, Physiology, and Regulation
journal, October 1994

Adsorption of U(VI) ions on biotite from aqueous solutions
journal, November 2009

Bioreduction of Fe-bearing clay minerals and their reactivity toward pertechnetate (Tc-99)
journal, September 2011

  • Bishop, Michael E.; Dong, Hailiang; Kukkadapu, Ravi K.
  • Geochimica et Cosmochimica Acta, Vol. 75, Issue 18
  • DOI: 10.1016/j.gca.2011.06.034

Complexation by Organic Matter Controls Uranium Mobility in Anoxic Sediments
journal, December 2019

  • Bone, Sharon E.; Cliff, John; Weaver, Karrie
  • Environmental Science & Technology, Vol. 54, Issue 3
  • DOI: 10.1021/acs.est.9b04741

ADesulfovibrio sp. capable of growing by reducing U(VI)
journal, December 1999

Effects of citrate on hexavalent chromium reduction by structural Fe(II) in nontronite
journal, February 2018

Spectroscopic Evidence for Interfacial Fe(II)−Fe(III) Electron Transfer in a Clay Mineral
journal, January 2011

  • Schaefer, Michael V.; Gorski, Christopher A.; Scherer, Michelle M.
  • Environmental Science & Technology, Vol. 45, Issue 2
  • DOI: 10.1021/es102560m

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

Composition and Stability of Iron and Copper Citrate Complexes in Aqueous Solution
journal, September 1974

  • Field, Terrence B.; McCourt, Janet L.; McBryde, W. A. E.
  • Canadian Journal of Chemistry, Vol. 52, Issue 17
  • DOI: 10.1139/v74-458

Microbial reduction of chlorite and uranium followed by air oxidation
journal, April 2011

Natural Humics Impact Uranium Bioreduction and Oxidation
journal, July 2005

  • Gu, Baohua; Yan, Hui; Zhou, Ping
  • Environmental Science & Technology, Vol. 39, Issue 14
  • DOI: 10.1021/es050350r

Microbial reduction of iron(III)-rich nontronite and uranium(VI)
journal, June 2009

  • Zhang, Gengxin; Senko, John M.; Kelly, Shelly D.
  • Geochimica et Cosmochimica Acta, Vol. 73, Issue 12, p. 3523-3538
  • DOI: 10.1016/j.gca.2009.03.030

Uranium in geologic fluids: Estimates of standard partial molal properties, oxidation potentials, and hydrolysis constants at high temperatures and pressures
journal, October 1997

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

  • O’Loughlin, Edward J.; Gorski, Christopher A.; Flynn, Theodore M.
  • Minerals, Vol. 9, Issue 7
  • DOI: 10.3390/min9070434

Geochemical controls of the microbially mediated redox cycling of uranium and iron
journal, August 2018

Polymerization of Uranyl-Citrate, -Malate, -Tartrate and -Lactate Complexes 1
journal, September 1954

  • Feldman, Isaac; Havill, Jean R.; Neuman, W. F.
  • Journal of the American Chemical Society, Vol. 76, Issue 18
  • DOI: 10.1021/ja01647a070

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

  • Bargar, J. R.; Williams, K. H.; Campbell, K. M.
  • Proceedings of the National Academy of Sciences, Vol. 110, Issue 12
  • DOI: 10.1073/pnas.1219198110

The New MRCAT (Sector 10) Bending Magnet Beamline at the Advanced Photon Source
conference, January 2010

  • Kropf, A. J.; Katsoudas, J.; Chattopadhyay, S.
  • SRI 2009, 10TH INTERNATIONAL CONFERENCE ON RADIATION INSTRUMENTATION, AIP Conference Proceedings
  • DOI: 10.1063/1.3463194
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