Isotopic and geochemical tracers for U(VI) reduction and U mobility at an in situ recovery U mine

Basu, Anirban; Brown, Shaun T.; Christensen, John N.; DePaolo, Donald J.; Reimus, Paul W.; Heikoop, Jeffrey M.; Woldegabriel, Giday; Simmons, Ardyth M.; House, Brian M.; Hartmann, Matt; Maher, Kate

doi:10.1021/acs.est.5b00701

Title: Isotopic and geochemical tracers for U(VI) reduction and U mobility at an in situ recovery U mine

Abstract

In situ recovery (ISR) uranium (U) mining mobilizes U in its oxidized hexavalent form (U(VI)) by oxidative dissolution of U from the roll-front U deposits. Post-mining natural attenuation of residual U(VI) at ISR mines is a potential remediation strategy. Detection and monitoring of naturally occurring reducing subsurface environments are important for successful implementation of this remediation scheme. We used the isotopic tracers ²³⁸U/²³⁵U (δ²³⁸U), ²³⁴U/²³⁸U activity ratio, and ³⁴S/³²S (δ³⁴S), and geochemical measurements of U ore and groundwater collected from 32 wells located within, upgradient, and downgradient of a roll-front U deposit to detect U(VI) reduction and U mobility at an ISR mining site at Rosita, TX, USA. The δ²³⁸U in Rosita groundwater varies from 0.61‰ to -2.49‰, with a trend toward lower δ²³⁸U in downgradient wells. The concurrent decrease in U(VI) concentration and δ²³⁸U with an ε of 0.48‰ ± 0.08‰ is indicative of naturally occurring reducing environments conducive to U(VI) reduction. Additionally, characteristic ²³⁴U/²³⁸U activity ratio and δ³⁴S values may also be used to trace the mobility of the ore zone groundwater after mining has ended. These results support the use of U isotope-based detection of natural attenuation of U(VI) at Rosita and other similar ISR mining sites.

Authors:

Basu, Anirban ^[1]; Brown, Shaun T. ^[2]; Christensen, John N. ^[3]; DePaolo, Donald J. ^[2]; Reimus, Paul W. ^[4]; Heikoop, Jeffrey M. ^[4]; Woldegabriel, Giday ^[4]; Simmons, Ardyth M. ^[4]; House, Brian M. ^[5]; Hartmann, Matt ^[6]; Maher, Kate ^[7]

Univ. of California, Berkeley, CA (United States)
Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of California, San Diego, La Jolla, CA (United States)
Uranium Resources, Inc., Centennial, CO (United States)
Stanford Univ., Stanford, CA (United States)

Publication Date:: Tue May 19 00:00:00 EDT 2015

Research Org.:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Org.:: USDOE

OSTI Identifier:: 1193681

Report Number(s):: LA-UR-15-21333
Journal ID: ISSN 0013-936X

Grant/Contract Number:: AC52-06NA25396

Resource Type:: Accepted Manuscript

Journal Name:: Environmental Science and Technology

Additional Journal Information:: Journal Volume: 49; Journal Issue: 10; Journal ID: ISSN 0013-936X

Country of Publication:: United States

Language:: English

Subject:: 54 ENVIRONMENTAL SCIENCES; 58 GEOSCIENCES; Planetary Sciences

Citation Formats


                    Basu, Anirban, Brown, Shaun T., Christensen, John N., DePaolo, Donald J., Reimus, Paul W., Heikoop, Jeffrey M., Woldegabriel, Giday, Simmons, Ardyth M., House, Brian M., Hartmann, Matt, and Maher, Kate. Isotopic and geochemical tracers for U(VI) reduction and U mobility at an in situ recovery U mine.  United States: N. p., 2015. 
Web.  doi:10.1021/acs.est.5b00701.

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                    Basu, Anirban, Brown, Shaun T., Christensen, John N., DePaolo, Donald J., Reimus, Paul W., Heikoop, Jeffrey M., Woldegabriel, Giday, Simmons, Ardyth M., House, Brian M., Hartmann, Matt, & Maher, Kate. Isotopic and geochemical tracers for U(VI) reduction and U mobility at an in situ recovery U mine.  United States.  https://doi.org/10.1021/acs.est.5b00701

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                    Basu, Anirban, Brown, Shaun T., Christensen, John N., DePaolo, Donald J., Reimus, Paul W., Heikoop, Jeffrey M., Woldegabriel, Giday, Simmons, Ardyth M., House, Brian M., Hartmann, Matt, and Maher, Kate. Tue .  
"Isotopic and geochemical tracers for U(VI) reduction and U mobility at an in situ recovery U mine".  United States.  https://doi.org/10.1021/acs.est.5b00701.  https://www.osti.gov/servlets/purl/1193681.

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@article{osti_1193681,

  title        = {Isotopic and geochemical tracers for U(VI) reduction and U mobility at an in situ recovery U mine},

  author       = {Basu, Anirban and Brown, Shaun T. and Christensen, John N. and DePaolo, Donald J. and Reimus, Paul W. and Heikoop, Jeffrey M. and Woldegabriel, Giday and Simmons, Ardyth M. and House, Brian M. and Hartmann, Matt and Maher, Kate},

  abstractNote = {In situ recovery (ISR) uranium (U) mining mobilizes U in its oxidized hexavalent form (U(VI)) by oxidative dissolution of U from the roll-front U deposits. Post-mining natural attenuation of residual U(VI) at ISR mines is a potential remediation strategy. Detection and monitoring of naturally occurring reducing subsurface environments are important for successful implementation of this remediation scheme. We used the isotopic tracers ²³⁸U/²³⁵U (δ²³⁸U), ²³⁴U/²³⁸U activity ratio, and ³⁴S/³²S (δ³⁴S), and geochemical measurements of U ore and groundwater collected from 32 wells located within, upgradient, and downgradient of a roll-front U deposit to detect U(VI) reduction and U mobility at an ISR mining site at Rosita, TX, USA. The δ²³⁸U in Rosita groundwater varies from 0.61‰ to -2.49‰, with a trend toward lower δ²³⁸U in downgradient wells. The concurrent decrease in U(VI) concentration and δ²³⁸U with an ε of 0.48‰ ± 0.08‰ is indicative of naturally occurring reducing environments conducive to U(VI) reduction. Additionally, characteristic ²³⁴U/²³⁸U activity ratio and δ³⁴S values may also be used to trace the mobility of the ore zone groundwater after mining has ended. These results support the use of U isotope-based detection of natural attenuation of U(VI) at Rosita and other similar ISR mining sites.},

  doi          = {10.1021/acs.est.5b00701},

  journal      = {Environmental Science and Technology},

  number       = 10,

  volume       = 49,

  place        = {United States},

  year         = {Tue May 19 00:00:00 EDT 2015},

  month        = {Tue May 19 00:00:00 EDT 2015}

}

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Journal Article Bhattacharyya, Amrita ; Campbell, Kate M. ; Kelly, Shelly D. ; ... - Nature Communications

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 reductionmore »« less
Cited by 43
https://doi.org/10.1038/ncomms15538

Full Text Available
Reduction and potential remediation of U(VI) by dithionite at an in-situ recovery mine: Insights gained by δ²³⁸U

Journal Article Jemison, Noah Edward ; Reimus, Paul William ; Harris, Rose Janina ; ... - Applied Geochemistry

In-situ recovery is a common method of mining U ore. This technique involves injecting an oxidant to oxidize U deposited as insoluble U(IV) to soluble U(VI) and a complexing agent to form mobile U(VI) compounds, which are extracted from mining waters. Unfortunately, U concentrations often remain elevated in groundwater following this mining process. One promising technique to decrease U concentrations to acceptable levels is in-situ remediation where a reductant is injected into the mined area to reduce U(VI) back to insoluble U(IV). Here we assess the efficacy of the chemical reductant dithionite to reduce U(VI) concentrations. While dithionite can reducemore »« less
Cited by 5
https://doi.org/10.1016/j.apgeochem.2020.104560

Full Text Available

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Title: Isotopic and geochemical tracers for U(VI) reduction and U mobility at an in situ recovery U mine

Abstract

Citation Formats

Critical review of acid in situ leach uranium mining: 1. USA and Australia journal, December 2001

The future of Yellowcake: A global assessment of uranium resources and mining journal, February 2014

Sustainability of Uranium Mining and Milling: Toward Quantifying Resources and Eco-Efficiency journal, March 2008

A top-down assessment of energy, water and land use in uranium mining, milling, and refining journal, November 2013

Evolution of uranium and thorium minerals journal, October 2009

Uranium Deposits of the World: Asia reference-book, January 2009

Uranium ore rolls; an analysis journal, March 1965

Groundwater processes and sedimentary uranium deposits journal, February 1999

Role of nuclear volume in driving equilibrium stable isotope fractionation of mercury, thallium, and other very heavy elements journal, May 2007

Nuclear Size and Shape Effects in Chemical Reactions. Isotope Chemistry of the Heavy Elements journal, January 1996

Nuclear field shift in natural environments journal, March 2013

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

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

Low-temperature isotopic fractionation of uranium journal, December 2007

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

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

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

Uranium 238 U/ 235 U Isotope Ratios as Indicators of Reduction: Results from an in situ Biostimulation Experiment at Rifle, Colorado, U.S.A. journal, August 2010

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

No Measurable Changes in 238 U/ 235 U due to Desorption–Adsorption of U(VI) from Groundwater at the Rifle, Colorado, Integrated Field Research Challenge Site journal, February 2013

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

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

Similarities, differences, and some genetic problems of the wyoming and colorado plateau types of uranium deposits in sandstone journal, November 1970

Sulfur isotopes and the origin of sandstone-type uranium deposits [Colorado Plateau and Wyoming] journal, August 1958

Geochemistry of selenium: formation of ferroselite and selenium behavior in the vicinity of oxidizing sulfide and uranium deposits journal, November 1977

12. Biogeochemistry of Sulfur Isotopes book, January 2001

The kinetic isotope effect in the chemical reduction of sulphate journal, January 1957

8. The Behavior of U- and Th-series Nuclides in Groundwater book, December 2003

The mineral dissolution rate conundrum: Insights from reactive transport modeling of U isotopes and pore fluid chemistry in marine sediments journal, January 2006

U–Sr isotopic speedometer: Fluid flow and chemical weathering rates in aquifers journal, September 2006

Alpha-Recoil Thorium-234: Dissolution into Water and the Uranium-234/Uranium-238 Disequilibrium in Nature journal, July 1971

Sediment transport time measured with U-series isotopes: Results from ODP North Atlantic drift site 984 journal, August 2006

Experimental evidence for 234U–238U fractionation during granite weathering with implications for 234U/238U in natural waters journal, July 2009

Identifying the Sources of Subsurface Contamination at the Hanford Site in Washington using High-Precision Uranium Isotopic Measurements journal, June 2004

A large column analog experiment of stable isotope variations during reactive transport: I. A comprehensive model of sulfur cycling and δ34S fractionation journal, January 2014

A Bacterial Method for the Nitrogen Isotopic Analysis of Nitrate in Seawater and Freshwater journal, September 2001

Measurement of the Oxygen Isotopic Composition of Nitrate in Seawater and Freshwater Using the Denitrifier Method journal, October 2002

Environmental Speciation of Actinides journal, June 2012

The effect of calcium on aqueous uranium(VI) speciation and adsorption to ferrihydrite and quartz journal, March 2006

Uranyl(VI) carbonate complex formation: Validation of the Ca2UO2(CO3)3(aq.) species journal, January 2001

Adsorption of uranyl onto ferric oxyhydroxides: Application of the surface complexation site-binding model journal, September 1985

Uranium(VI) adsorption to ferrihydrite: Application of a surface complexation model journal, December 1994

Sorption of uranyl ions on hydrous titanium dioxide journal, January 1988

Approaches to surface complexation modeling of Uranium(VI) adsorption on aquifer sediments journal, September 2004

Interactions of aqueous U(VI) with soil minerals in slightly alkaline natural systems journal, August 2008

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

Speciation-Dependent Kinetics of Uranium(VI) Bioreduction journal, June 2011

Redox Processes and Water Quality of Selected Principal Aquifer Systems journal, March 2008

The thermodynamic ladder in geomicrobiology journal, March 2011

Using isotope fractionation of nitrate-nitrogen and nitrate-oxygen for evaluation of microbial denitrification in a sandy aquifer journal, May 1990

Stable Isotopes of Oxygen and Nitrogen in Source Identification of Nitrate from Septic Systems journal, March 1993

Multiple Geochemical and Isotopic Approaches for Assessing Ground Water NO3- Elimination in a Riparian Zone journal, May 1999

Role of the riparian zone in controlling the distribution and fate of agricultural nitrogen near a small stream in southern Ontario journal, April 1999

Modelling nitrogen and oxygen isotope fractionation during denitrification in a lacustrine redox-transition zone journal, July 2003

A dual isotope approach to identify denitrification in groundwater at a river-bank infiltration site journal, July 2003

Does the Rayleigh Equation Apply to Evaluate Field Isotope Data in Contaminant Hydrogeology? journal, March 2006

Effective Isotopic Fractionation Factors for Solute Removal by Reactive Sediments: A Laboratory Microcosm and Slurry Study journal, October 2008

Cr Stable Isotopes As Indicators of Cr(VI) Reduction in Groundwater: A Detailed Time-Series Study of a Point-Source Plume journal, February 2010

Uranium Isotope Fractionation during Adsorption to Mn-Oxyhydroxides journal, February 2011

Uranium comminution ages: Sediment transport and deposition time scales journal, November 2012

Uranium-series comminution ages of continental sediments: Case study of a Pleistocene alluvial fan journal, August 2010

The transport of U- and Th-series nuclides in a sandy unconfined aquifer journal, April 2001

The transport of U- and Th-series nuclides in sandy confined aquifers journal, June 2003

Identifying natural and anthropogenic variability of uranium at the well scale, Homestake Superfund site, near Milan, New Mexico, USA journal, February 2019

Di- μ -acetato Diuranyl(VI) Complexes with N -(2-pyridyl)- N′ -(5-R-salicylidene)hydrazines: Syntheses, Structures, Properties and Extraction Studies journal, May 2018

Differentiating anthropogenic and natural sources of uranium by geochemical fingerprinting of groundwater at the Homestake uranium mill, Milan, New Mexico, USA journal, June 2019

Uranium isotope fractionation by abiotic reductive precipitation journal, August 2018

Critical review of acid in situ leach uranium mining: 1. USA and Australia
journal, December 2001

The future of Yellowcake: A global assessment of uranium resources and mining
journal, February 2014

Sustainability of Uranium Mining and Milling: Toward Quantifying Resources and Eco-Efficiency
journal, March 2008

A top-down assessment of energy, water and land use in uranium mining, milling, and refining
journal, November 2013

Evolution of uranium and thorium minerals
journal, October 2009

Uranium Deposits of the World: Asia
reference-book, January 2009

Uranium ore rolls; an analysis
journal, March 1965

Groundwater processes and sedimentary uranium deposits
journal, February 1999

Role of nuclear volume in driving equilibrium stable isotope fractionation of mercury, thallium, and other very heavy elements
journal, May 2007

Nuclear Size and Shape Effects in Chemical Reactions. Isotope Chemistry of the Heavy Elements
journal, January 1996

Nuclear field shift in natural environments
journal, March 2013

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

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

Low-temperature isotopic fractionation of uranium
journal, December 2007

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

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

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

Uranium ²³⁸ U/ ²³⁵ U Isotope Ratios as Indicators of Reduction: Results from an in situ Biostimulation Experiment at Rifle, Colorado, U.S.A.
journal, August 2010

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

No Measurable Changes in ²³⁸ U/ ²³⁵ U due to Desorption–Adsorption of U(VI) from Groundwater at the Rifle, Colorado, Integrated Field Research Challenge Site
journal, February 2013

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

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

Similarities, differences, and some genetic problems of the wyoming and colorado plateau types of uranium deposits in sandstone
journal, November 1970

Sulfur isotopes and the origin of sandstone-type uranium deposits [Colorado Plateau and Wyoming]
journal, August 1958

Geochemistry of selenium: formation of ferroselite and selenium behavior in the vicinity of oxidizing sulfide and uranium deposits
journal, November 1977

12. Biogeochemistry of Sulfur Isotopes
book, January 2001

The kinetic isotope effect in the chemical reduction of sulphate
journal, January 1957

8. The Behavior of U- and Th-series Nuclides in Groundwater
book, December 2003

The mineral dissolution rate conundrum: Insights from reactive transport modeling of U isotopes and pore fluid chemistry in marine sediments
journal, January 2006

U–Sr isotopic speedometer: Fluid flow and chemical weathering rates in aquifers
journal, September 2006

Alpha-Recoil Thorium-234: Dissolution into Water and the Uranium-234/Uranium-238 Disequilibrium in Nature
journal, July 1971

Sediment transport time measured with U-series isotopes: Results from ODP North Atlantic drift site 984
journal, August 2006

Experimental evidence for 234U–238U fractionation during granite weathering with implications for 234U/238U in natural waters
journal, July 2009

Identifying the Sources of Subsurface Contamination at the Hanford Site in Washington using High-Precision Uranium Isotopic Measurements
journal, June 2004

A large column analog experiment of stable isotope variations during reactive transport: I. A comprehensive model of sulfur cycling and δ34S fractionation
journal, January 2014

A Bacterial Method for the Nitrogen Isotopic Analysis of Nitrate in Seawater and Freshwater
journal, September 2001

Measurement of the Oxygen Isotopic Composition of Nitrate in Seawater and Freshwater Using the Denitrifier Method
journal, October 2002

Environmental Speciation of Actinides
journal, June 2012

The effect of calcium on aqueous uranium(VI) speciation and adsorption to ferrihydrite and quartz
journal, March 2006

Uranyl(VI) carbonate complex formation: Validation of the Ca2UO2(CO3)3(aq.) species
journal, January 2001

Adsorption of uranyl onto ferric oxyhydroxides: Application of the surface complexation site-binding model
journal, September 1985

Uranium(VI) adsorption to ferrihydrite: Application of a surface complexation model
journal, December 1994

Sorption of uranyl ions on hydrous titanium dioxide
journal, January 1988

Approaches to surface complexation modeling of Uranium(VI) adsorption on aquifer sediments
journal, September 2004

Interactions of aqueous U(VI) with soil minerals in slightly alkaline natural systems
journal, August 2008

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

Speciation-Dependent Kinetics of Uranium(VI) Bioreduction
journal, June 2011

Redox Processes and Water Quality of Selected Principal Aquifer Systems
journal, March 2008

The thermodynamic ladder in geomicrobiology
journal, March 2011

Using isotope fractionation of nitrate-nitrogen and nitrate-oxygen for evaluation of microbial denitrification in a sandy aquifer
journal, May 1990

Stable Isotopes of Oxygen and Nitrogen in Source Identification of Nitrate from Septic Systems
journal, March 1993

Multiple Geochemical and Isotopic Approaches for Assessing Ground Water NO3- Elimination in a Riparian Zone
journal, May 1999

Role of the riparian zone in controlling the distribution and fate of agricultural nitrogen near a small stream in southern Ontario
journal, April 1999

Modelling nitrogen and oxygen isotope fractionation during denitrification in a lacustrine redox-transition zone
journal, July 2003

A dual isotope approach to identify denitrification in groundwater at a river-bank infiltration site
journal, July 2003

Does the Rayleigh Equation Apply to Evaluate Field Isotope Data in Contaminant Hydrogeology?
journal, March 2006

Effective Isotopic Fractionation Factors for Solute Removal by Reactive Sediments: A Laboratory Microcosm and Slurry Study
journal, October 2008

Cr Stable Isotopes As Indicators of Cr(VI) Reduction in Groundwater: A Detailed Time-Series Study of a Point-Source Plume
journal, February 2010

Uranium Isotope Fractionation during Adsorption to Mn-Oxyhydroxides
journal, February 2011

Uranium comminution ages: Sediment transport and deposition time scales
journal, November 2012

Uranium-series comminution ages of continental sediments: Case study of a Pleistocene alluvial fan
journal, August 2010

The transport of U- and Th-series nuclides in a sandy unconfined aquifer
journal, April 2001

The transport of U- and Th-series nuclides in sandy confined aquifers
journal, June 2003

Identifying natural and anthropogenic variability of uranium at the well scale, Homestake Superfund site, near Milan, New Mexico, USA
journal, February 2019

Di- μ -acetato Diuranyl(VI) Complexes with N -(2-pyridyl)- N′ -(5-R-salicylidene)hydrazines: Syntheses, Structures, Properties and Extraction Studies
journal, May 2018

Differentiating anthropogenic and natural sources of uranium by geochemical fingerprinting of groundwater at the Homestake uranium mill, Milan, New Mexico, USA
journal, June 2019

Uranium isotope fractionation by abiotic reductive precipitation
journal, August 2018