Biogenic non-crystalline U(IV) revealed as major component in uranium ore deposits

Bhattacharyya, Amrita; Campbell, Kate M.; Kelly, Shelly D.; Roebbert, Yvonne; Weyer, Stefan; Bernier-Latmani, Rizlan; Borch, Thomas

doi:10.1038/ncomms15538

Title: Biogenic non-crystalline U^(IV) revealed as major component in uranium ore deposits

Abstract

Historically, it is believed that crystalline uraninite, produced via the abiotic reduction of hexavalent uranium (U^(VI)) is the dominant reduced U species formed in low-temperature uranium roll-front ore deposits. Here we show that non-crystalline U^(IV) generated through biologically mediated U^(VI) reduction is the predominant U^(IV) species in an undisturbed U roll-front ore deposit in Wyoming, USA. Characterization of U species revealed that the majority (~58-89%) of U is bound as U^(IV) to C-containing organic functional groups or inorganic carbonate, while uraninite and U^(VI) represent only minor components. The uranium deposit exhibited mostly 238U-enriched isotope signatures, consistent with largely biotic reduction of U^(VI) to U^(IV). This finding implies that biogenic processes are more important to uranium ore genesis than previously understood. The predominance of a relatively labile form of U^(IV) also provides an opportunity for a more economical and environmentally benign mining process, as well as the design of more effective post-mining restoration strategies and human health-risk assessment.

Authors:

Bhattacharyya, Amrita ^[1]; Campbell, Kate M. ^[2]; Kelly, Shelly D. ^[3]; Roebbert, Yvonne ^[4]; Weyer, Stefan ^[4]; Bernier-Latmani, Rizlan ^[5];

^[6]

Colorado State Univ., Fort Collins, CO (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
U.S. Geological Survey, Boulder, CO (United States)
EXAFS Analysis, Bolingbrook, IL (United States)
Leibniz Univ. Hannover, Hannover (Germany)
Ecole Polytechnique Federale de Lausanne, Lausanne (Switzerland)
Colorado State Univ., Fort Collins, CO (United States)

Publication Date:: Thu Jun 01 00:00:00 EDT 2017

Research Org.:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1379874

Grant/Contract Number:: AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: Nature Communications

Additional Journal Information:: Journal Volume: 8; Journal ID: ISSN 2041-1723

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 58 GEOSCIENCES; Element cycles; Geochemistry; Microbial ecology; Nuclear waste

Citation Formats


                    Bhattacharyya, Amrita, Campbell, Kate M., Kelly, Shelly D., Roebbert, Yvonne, Weyer, Stefan, Bernier-Latmani, Rizlan, and Borch, Thomas. Biogenic non-crystalline U(IV) revealed as major component in uranium ore deposits.  United States: N. p., 2017. 
Web.  doi:10.1038/ncomms15538.

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                    Bhattacharyya, Amrita, Campbell, Kate M., Kelly, Shelly D., Roebbert, Yvonne, Weyer, Stefan, Bernier-Latmani, Rizlan, & Borch, Thomas. Biogenic non-crystalline U(IV) revealed as major component in uranium ore deposits.  United States.  https://doi.org/10.1038/ncomms15538

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                    Bhattacharyya, Amrita, Campbell, Kate M., Kelly, Shelly D., Roebbert, Yvonne, Weyer, Stefan, Bernier-Latmani, Rizlan, and Borch, Thomas. Thu .  
"Biogenic non-crystalline U(IV) revealed as major component in uranium ore deposits".  United States.  https://doi.org/10.1038/ncomms15538.  https://www.osti.gov/servlets/purl/1379874.

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@article{osti_1379874,

  title        = {Biogenic non-crystalline U(IV) revealed as major component in uranium ore deposits},

  author       = {Bhattacharyya, Amrita and Campbell, Kate M. and Kelly, Shelly D. and Roebbert, Yvonne and Weyer, Stefan and Bernier-Latmani, Rizlan and Borch, Thomas},

  abstractNote = {Historically, it is believed that crystalline uraninite, produced via the abiotic reduction of hexavalent uranium (U(VI)) is the dominant reduced U species formed in low-temperature uranium roll-front ore deposits. Here we show that non-crystalline U(IV) generated through biologically mediated U(VI) reduction is the predominant U(IV) species in an undisturbed U roll-front ore deposit in Wyoming, USA. Characterization of U species revealed that the majority (~58-89%) of U is bound as U(IV) to C-containing organic functional groups or inorganic carbonate, while uraninite and U(VI) represent only minor components. The uranium deposit exhibited mostly 238U-enriched isotope signatures, consistent with largely biotic reduction of U(VI) to U(IV). This finding implies that biogenic processes are more important to uranium ore genesis than previously understood. The predominance of a relatively labile form of U(IV) also provides an opportunity for a more economical and environmentally benign mining process, as well as the design of more effective post-mining restoration strategies and human health-risk assessment.},

  doi          = {10.1038/ncomms15538},

  journal      = {Nature Communications},

  number       = ,

  volume       = 8,

  place        = {United States},

  year         = {Thu Jun 01 00:00:00 EDT 2017},

  month        = {Thu Jun 01 00:00:00 EDT 2017}

}

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McMahon, Sean; Ivarsson, Magnus
BioEssays, Vol. 41, Issue 8
DOI: 10.1002/bies.201900052

The Role of Organic Matter on Uranium Precipitation in Zoovch Ovoo, Mongolia
journal, May 2019

Rallakis, Dimitrios; Michels, Raymond; Brouand, Marc
Minerals, Vol. 9, Issue 5
DOI: 10.3390/min9050310

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© 2014. In-situ recovery (ISR) of uranium (U) from sandstone-type roll-front deposits is a technology that involves the injection of solutions that consist of ground water fortified with oxygen and carbonate to promote the oxidative dissolution of U, which is pumped to recovery facilities located at the surface that capture the dissolved U and recycle the treated water. The ISR process alters the geochemical conditions in the subsurface creating conditions that are more favorable to the migration of uranium and other metals associated with the uranium deposit. There is a lack of clear understanding of the impact of ISR miningmore »« less
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Title: Biogenic non-crystalline U(IV) revealed as major component in uranium ore deposits

Abstract

Citation Formats

Extracellular reduction of uranium via Geobacter conductive pili as a protective cellular mechanism journal, September 2011

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

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

Low-temperature isotopic fractionation of uranium journal, December 2007

Aqueous uptake of uranium onto pyrite surfaces; reactivity of fresh versus weathered material journal, November 2007

Fractionation studies of trace elements in contaminated soils and sediments: a review of sequential extraction procedures journal, June 2002

Uranium isotopic compositions of the crust and ocean: Age corrections, U budget and global extent of modern anoxia journal, October 2015

The UWXAFS analysis package: philosophy and details journal, March 1995

Three examples illustrating the analysis of organic matter associated with uranium ores journal, January 1990

Spectroscopic Evidence of Uranium Immobilization in Acidic Wetlands by Natural Organic Matter and Plant Roots journal, February 2015

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

Spectroscopic Evidence of Uranium Immobilization in Acidic Wetlands by Natural Organic Matter and Plant Roots journal, February 2015

Non-uraninite Products of Microbial U(VI) Reduction journal, December 2010

Uranium isotopic compositions of the crust and ocean: Age corrections, U budget and global extent of modern anoxia journal, October 2015

Iron disulfide minerals and the genesis of roll-type uranium deposits journal, February 1983

Microbial reduction of uranium journal, April 1991

Isotopic Evidence for Reductive Immobilization of Uranium Across a Roll-Front Mineral Deposit journal, June 2016

Reduction of uranium by cytochrome c3 of Desulfovibrio vulgaris. journal, January 1993

Uranium Transformations in Static Microcosms journal, January 2010

Hydrogeochemical evolution and C isotope study of groundwaters from “Mina Fe” U deposit (Salamanca, Spain): implications for processes in radwaste disposal journal, March 2005

Long-term solid-phase fate of co-precipitated U(VI)-Fe(III) following biological iron reduction by Thermoanaerobacter journal, September 2012

Biogenic and petroleum-related ore-forming processes in Dongsheng uranium deposit, NW China journal, September 2007

Uranium Uptake from Aqueous Solution by Interaction with Goethite, Lepidocrocite, Muscovite, and Mackinawite: An X-ray Absorption Spectroscopy Study journal, March 2000

SIXPack a Graphical User Interface for XAS Analysis Using IFEFFIT journal, January 2005

An ab initio molecular orbital study of the nuclear volume effects in uranium isotope fractionations journal, October 2008

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

Non-uraninite Products of Microbial U(VI) Reduction journal, December 2010

Three examples illustrating the analysis of organic matter associated with uranium ores journal, January 1990

Kinetics of Uranium(VI) Reduction by Hydrogen Sulfide in Anoxic Aqueous Systems journal, August 2006

Persistent U(IV) and U(VI) following in-situ recovery (ISR) mining of a sandstone uranium deposit, Wyoming, USA journal, December 2015

238 U/ 235 U isotope ratios of crustal material, rivers and products of hydrothermal alteration: new insights on the oceanic U isotope mass balance journal, February 2015

Isotopic Evidence for Reductive Immobilization of Uranium Across a Roll-Front Mineral Deposit journal, June 2016

238U/235U isotope ratios of crustal material, rivers and products of hydrothermal alteration: new insights on the oceanic U isotope mass balance text, January 2015

Uranium Reduction journal, October 2006

Uranium mobility in organic matter-rich sediments: A review of geological and geochemical processes journal, August 2016

Sequential extraction procedure for the speciation of particulate trace metals journal, June 1979

Relative Reactivity of Biogenic and Chemogenic Uraninite and Biogenic Noncrystalline U(IV) journal, August 2013

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

Mechanism of Uranium Reduction and Immobilization in Desulfovibrio vulgaris Biofilms journal, August 2015

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

Uranium Isotope Fractionation journal, January 2017

Structure of Biogenic Uraninite Produced by Shewanella oneidensis Strain MR-1 journal, November 2008

Structure of Biogenic Uraninite Produced by Shewanella oneidensis Strain MR-1 journal, November 2008

Enhanced Uranium Immobilization and Reduction by Geobacter sulfurreducens Biofilms journal, August 2014

The SILVA ribosomal RNA gene database project: improved data processing and web-based tools journal, November 2012

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

QIIME allows analysis of high-throughput community sequencing data journal, April 2010

Natural fractionation of 238U/235U journal, January 2008

Interaction between aqueous uranium (VI) and sulfide minerals: Spectroscopic evidence for sorption and reduction journal, July 1994

The role of anaerobic respiration in the immobilization of uranium through biomineralization of phosphate minerals journal, April 2013

Relationship between the hydrogeochemical environment and sandstone-type uranium mineralization in the Ili basin, China journal, January 2011

The SILVA ribosomal RNA gene database project: improved data processing and web-based tools journal, November 2012

Multiple mechanisms of uranium immobilization by Cellulomonas sp. strain ES6 journal, October 2010

Kinetics of Uranium(VI) Reduction by Hydrogen Sulfide in Anoxic Aqueous Systems journal, August 2006

Reduction of Uranium(VI) to Uranium(IV) by Clostridia journal, May 2008

The effect of pH and natural microbial phosphatase activity on the speciation of uranium in subsurface soils journal, October 2011

Natural variations in uranium isotope ratios of uranium ore concentrates: Understanding the 238U/235U fractionation mechanism journal, March 2010

Characterization of cores from an in-situ recovery mined uranium deposit in Wyoming: Implications for post-mining restoration journal, December 2014

Multiple mechanisms of uranium immobilization by Cellulomonas sp. strain ES6 journal, October 2010

Sandstone hosted uranium deposits of the Great Divide Basin, Wyoming, USA journal, June 2012

Relative Reactivity of Biogenic and Chemogenic Uraninite and Biogenic Noncrystalline U(IV) journal, August 2013

Mechanism of Uranium Reduction and Immobilization in Desulfovibrio vulgaris Biofilms journal, August 2015

Age of uranium mineralization at the Highland Mine, Powder River basin, Wyoming, as indicated by U-Pb isotope analyses journal, May 1983

Reduction of uranium by Desulfovibrio desulfuricans. journal, January 1992

Fractionation of 238U/235U by reduction during low temperature uranium mineralisation processes journal, February 2014

QIIME allows analysis of high-throughput community sequencing data journal, April 2010

Uranium Isotope Fractionation during Adsorption, (Co)precipitation, and Biotic Reduction journal, November 2016

Uranium isotopic fractionation factors during U(VI) reduction by bacterial isolates journal, July 2014

Uranium isotopes fingerprint biotic reduction journal, April 2015

Coexisting coffinite and uraninite in some sandstone-host uranium ores of Wyoming journal, April 1980

Uranium isotopes fingerprint biotic reduction journal, April 2015

Unstable sulfur compounds and the origin of roll-type uranium deposits journal, April 1969

Hydrothermal alteration of organic matter in uranium ores, Elliot Lake, Canada: Implications for selected organic-rich deposits journal, July 1993

Microbial reduction of uranium journal, April 1991

Uranium mobility in organic matter-rich sediments: A review of geological and geochemical processes journal, August 2016

Isotope fractionation during oxidation of tetravalent uranium by dissolved oxygen journal, February 2015

Variations in 238U/235U in uranium ore deposits: Isotopic signatures of the U reduction process? journal, July 2009

Title: Biogenic non-crystalline U^(IV) revealed as major component in uranium ore deposits

Extracellular reduction of uranium via Geobacter conductive pili as a protective cellular mechanism
journal, September 2011

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

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

Low-temperature isotopic fractionation of uranium
journal, December 2007

Aqueous uptake of uranium onto pyrite surfaces; reactivity of fresh versus weathered material
journal, November 2007

Fractionation studies of trace elements in contaminated soils and sediments: a review of sequential extraction procedures
journal, June 2002

Uranium isotopic compositions of the crust and ocean: Age corrections, U budget and global extent of modern anoxia
journal, October 2015

The UWXAFS analysis package: philosophy and details
journal, March 1995

Three examples illustrating the analysis of organic matter associated with uranium ores
journal, January 1990

Spectroscopic Evidence of Uranium Immobilization in Acidic Wetlands by Natural Organic Matter and Plant Roots
journal, February 2015

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

Spectroscopic Evidence of Uranium Immobilization in Acidic Wetlands by Natural Organic Matter and Plant Roots
journal, February 2015

Non-uraninite Products of Microbial U(VI) Reduction
journal, December 2010

Uranium isotopic compositions of the crust and ocean: Age corrections, U budget and global extent of modern anoxia
journal, October 2015

Iron disulfide minerals and the genesis of roll-type uranium deposits
journal, February 1983

Microbial reduction of uranium
journal, April 1991

Isotopic Evidence for Reductive Immobilization of Uranium Across a Roll-Front Mineral Deposit
journal, June 2016

Reduction of uranium by cytochrome c3 of Desulfovibrio vulgaris.
journal, January 1993

Uranium Transformations in Static Microcosms
journal, January 2010

Hydrogeochemical evolution and C isotope study of groundwaters from “Mina Fe” U deposit (Salamanca, Spain): implications for processes in radwaste disposal
journal, March 2005

Long-term solid-phase fate of co-precipitated U(VI)-Fe(III) following biological iron reduction by Thermoanaerobacter
journal, September 2012

Biogenic and petroleum-related ore-forming processes in Dongsheng uranium deposit, NW China
journal, September 2007

Uranium Uptake from Aqueous Solution by Interaction with Goethite, Lepidocrocite, Muscovite, and Mackinawite: An X-ray Absorption Spectroscopy Study
journal, March 2000

SIXPack a Graphical User Interface for XAS Analysis Using IFEFFIT
journal, January 2005

An ab initio molecular orbital study of the nuclear volume effects in uranium isotope fractionations
journal, October 2008

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

Non-uraninite Products of Microbial U(VI) Reduction
journal, December 2010

Three examples illustrating the analysis of organic matter associated with uranium ores
journal, January 1990

Kinetics of Uranium(VI) Reduction by Hydrogen Sulfide in Anoxic Aqueous Systems
journal, August 2006

Persistent U(IV) and U(VI) following in-situ recovery (ISR) mining of a sandstone uranium deposit, Wyoming, USA
journal, December 2015

²³⁸ U/ ²³⁵ U isotope ratios of crustal material, rivers and products of hydrothermal alteration: new insights on the oceanic U isotope mass balance
journal, February 2015

Isotopic Evidence for Reductive Immobilization of Uranium Across a Roll-Front Mineral Deposit
journal, June 2016

²³⁸U/²³⁵U isotope ratios of crustal material, rivers and products of hydrothermal alteration: new insights on the oceanic U isotope mass balance
text, January 2015

Uranium Reduction
journal, October 2006

Uranium mobility in organic matter-rich sediments: A review of geological and geochemical processes
journal, August 2016

Sequential extraction procedure for the speciation of particulate trace metals
journal, June 1979

Relative Reactivity of Biogenic and Chemogenic Uraninite and Biogenic Noncrystalline U(IV)
journal, August 2013

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

Mechanism of Uranium Reduction and Immobilization in Desulfovibrio vulgaris Biofilms
journal, August 2015

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

Uranium Isotope Fractionation
journal, January 2017

Structure of Biogenic Uraninite Produced by Shewanella oneidensis Strain MR-1
journal, November 2008

Structure of Biogenic Uraninite Produced by Shewanella oneidensis Strain MR-1
journal, November 2008

Enhanced Uranium Immobilization and Reduction by Geobacter sulfurreducens Biofilms
journal, August 2014

The SILVA ribosomal RNA gene database project: improved data processing and web-based tools
journal, November 2012

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

QIIME allows analysis of high-throughput community sequencing data
journal, April 2010

Natural fractionation of 238U/235U
journal, January 2008

Interaction between aqueous uranium (VI) and sulfide minerals: Spectroscopic evidence for sorption and reduction
journal, July 1994

The role of anaerobic respiration in the immobilization of uranium through biomineralization of phosphate minerals
journal, April 2013

Relationship between the hydrogeochemical environment and sandstone-type uranium mineralization in the Ili basin, China
journal, January 2011

The SILVA ribosomal RNA gene database project: improved data processing and web-based tools
journal, November 2012

Multiple mechanisms of uranium immobilization by Cellulomonas sp. strain ES6
journal, October 2010

Kinetics of Uranium(VI) Reduction by Hydrogen Sulfide in Anoxic Aqueous Systems
journal, August 2006

Reduction of Uranium(VI) to Uranium(IV) by Clostridia
journal, May 2008

The effect of pH and natural microbial phosphatase activity on the speciation of uranium in subsurface soils
journal, October 2011

Natural variations in uranium isotope ratios of uranium ore concentrates: Understanding the 238U/235U fractionation mechanism
journal, March 2010

Characterization of cores from an in-situ recovery mined uranium deposit in Wyoming: Implications for post-mining restoration
journal, December 2014

Multiple mechanisms of uranium immobilization by Cellulomonas sp. strain ES6
journal, October 2010

Sandstone hosted uranium deposits of the Great Divide Basin, Wyoming, USA
journal, June 2012

Relative Reactivity of Biogenic and Chemogenic Uraninite and Biogenic Noncrystalline U(IV)
journal, August 2013

Mechanism of Uranium Reduction and Immobilization in Desulfovibrio vulgaris Biofilms
journal, August 2015

Age of uranium mineralization at the Highland Mine, Powder River basin, Wyoming, as indicated by U-Pb isotope analyses
journal, May 1983

Reduction of uranium by Desulfovibrio desulfuricans.
journal, January 1992

Fractionation of 238U/235U by reduction during low temperature uranium mineralisation processes
journal, February 2014

QIIME allows analysis of high-throughput community sequencing data
journal, April 2010

Uranium Isotope Fractionation during Adsorption, (Co)precipitation, and Biotic Reduction
journal, November 2016

Uranium isotopic fractionation factors during U(VI) reduction by bacterial isolates
journal, July 2014

Uranium isotopes fingerprint biotic reduction
journal, April 2015

Coexisting coffinite and uraninite in some sandstone-host uranium ores of Wyoming
journal, April 1980

Uranium isotopes fingerprint biotic reduction
journal, April 2015

Unstable sulfur compounds and the origin of roll-type uranium deposits
journal, April 1969

Hydrothermal alteration of organic matter in uranium ores, Elliot Lake, Canada: Implications for selected organic-rich deposits
journal, July 1993

Microbial reduction of uranium
journal, April 1991

Uranium mobility in organic matter-rich sediments: A review of geological and geochemical processes
journal, August 2016

Isotope fractionation during oxidation of tetravalent uranium by dissolved oxygen
journal, February 2015

Variations in 238U/235U in uranium ore deposits: Isotopic signatures of the U reduction process?
journal, July 2009

New average values for the n(238U)/n(235U) isotope ratios of natural uranium standards
journal, July 2010

An ab initio molecular orbital study of the nuclear volume effects in uranium isotope fractionations
journal, October 2008