Field Application of 238U/235U Measurements To Detect Reoxidation and Mobilization of U(IV)

Jemison, Noah E.; Shiel, Alyssa E.; Johnson, Thomas M.; Lundstrom, Craig C.; Long, Philip E.; Williams, Kenneth H.

doi:10.1021/acs.est.7b05162

Title: Field Application of ²³⁸U/²³⁵U Measurements To Detect Reoxidation and Mobilization of U(IV)

Abstract

We present that biostimulation to induce reduction of soluble U(VI) to relatively immobile U(IV) is an effective strategy for decreasing aqueous U(VI) concentrations in contaminated groundwater systems. If oxidation of U(IV) occurs following the biostimulation phase, U(VI) concentrations increase, challenging the long-term effectiveness of this technique. However, detecting U(IV) oxidation through dissolved U concentrations alone can prove difficult in locations with few groundwater wells to track the addition of U to a mass of groundwater. We propose the ²³⁸U/²³⁵U ratio of aqueous U as an independent, reliable tracer of U(IV) remobilization via oxidation or mobilization of colloids. Reduction of U(VI) produces ²³⁸U-enriched U(IV), whereas remobilization of solid U(IV) should not induce isotopic fractionation. The incorporation of remobilized U(IV) with a high ²³⁸U/²³⁵U ratio into the aqueous U(VI) pool produces an increase in ²³⁸U/²³⁵U of aqueous U(VI). Lastly, during several injections of nitrate to induce U(IV) oxidation, ²³⁸U/²³⁵U consistently increased, suggesting ²³⁸U/²³⁵U is broadly applicable for detecting mobilization of U(IV).

Authors:

^[1]; Shiel, Alyssa E. ^[2]; Johnson, Thomas M. ^[1]; Lundstrom, Craig C. ^[1]; Long, Philip E. ^[3]; Williams, Kenneth H. ^[3]

Univ. of Illinois, Urbana, IL (United States). Dept. of Geology
Oregon State Univ., Corvallis, OR (United States). College of Earth, Ocean, and Atmospheric Sciences
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Earth Sciences Division

Publication Date:: Wed Feb 21 00:00:00 EST 2018

Research Org.:: Univ. of Illinois at Urbana-Champaign, IL (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

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

OSTI Identifier:: 1460250

Alternate Identifier(s):: OSTI ID: 1477271

Grant/Contract Number:: SC0006755; AC02-05CH11231

Resource Type:: Accepted Manuscript

Journal Name:: Environmental Science and Technology

Additional Journal Information:: Journal Volume: 52; Journal Issue: 6; Journal ID: ISSN 0013-936X

Publisher:: American Chemical Society (ACS)

Country of Publication:: United States

Language:: English

Subject:: 54 ENVIRONMENTAL SCIENCES; 58 GEOSCIENCES

Citation Formats


                    Jemison, Noah E., Shiel, Alyssa E., Johnson, Thomas M., Lundstrom, Craig C., Long, Philip E., and Williams, Kenneth H. Field Application of 238U/235U Measurements To Detect Reoxidation and Mobilization of U(IV).  United States: N. p., 2018. 
Web.  doi:10.1021/acs.est.7b05162.

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                    Jemison, Noah E., Shiel, Alyssa E., Johnson, Thomas M., Lundstrom, Craig C., Long, Philip E., & Williams, Kenneth H. Field Application of 238U/235U Measurements To Detect Reoxidation and Mobilization of U(IV).  United States.  https://doi.org/10.1021/acs.est.7b05162

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                    Jemison, Noah E., Shiel, Alyssa E., Johnson, Thomas M., Lundstrom, Craig C., Long, Philip E., and Williams, Kenneth H. Wed .  
"Field Application of 238U/235U Measurements To Detect Reoxidation and Mobilization of U(IV)".  United States.  https://doi.org/10.1021/acs.est.7b05162.  https://www.osti.gov/servlets/purl/1460250.

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@article{osti_1460250,

  title        = {Field Application of 238U/235U Measurements To Detect Reoxidation and Mobilization of U(IV)},

  author       = {Jemison, Noah E. and Shiel, Alyssa E. and Johnson, Thomas M. and Lundstrom, Craig C. and Long, Philip E. and Williams, Kenneth H.},

  abstractNote = {We present that biostimulation to induce reduction of soluble U(VI) to relatively immobile U(IV) is an effective strategy for decreasing aqueous U(VI) concentrations in contaminated groundwater systems. If oxidation of U(IV) occurs following the biostimulation phase, U(VI) concentrations increase, challenging the long-term effectiveness of this technique. However, detecting U(IV) oxidation through dissolved U concentrations alone can prove difficult in locations with few groundwater wells to track the addition of U to a mass of groundwater. We propose the 238U/235U ratio of aqueous U as an independent, reliable tracer of U(IV) remobilization via oxidation or mobilization of colloids. Reduction of U(VI) produces 238U-enriched U(IV), whereas remobilization of solid U(IV) should not induce isotopic fractionation. The incorporation of remobilized U(IV) with a high 238U/235U ratio into the aqueous U(VI) pool produces an increase in 238U/235U of aqueous U(VI). Lastly, during several injections of nitrate to induce U(IV) oxidation, 238U/235U consistently increased, suggesting 238U/235U is broadly applicable for detecting mobilization of U(IV).},

  doi          = {10.1021/acs.est.7b05162},

  journal      = {Environmental Science and Technology},

  number       = 6,

  volume       = 52,

  place        = {United States},

  year         = {Wed Feb 21 00:00:00 EST 2018},

  month        = {Wed Feb 21 00:00:00 EST 2018}

}

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Works referencing / citing this record:

On the change in UO ₂ redox reactivity as a function of H ₂ O ₂ exposure
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Maier, Annika Carolin; Kegler, Philip; Klinkenberg, Martina
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Title: Field Application of 238U/235U Measurements To Detect Reoxidation and Mobilization of U(IV)

Abstract

Citation Formats

Stimulating the In Situ Activity of Geobacter Species To Remove Uranium from the Groundwater of a Uranium-Contaminated Aquifer journal, October 2003

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

Isotope fractionation of 238U and 235U during biologically-mediated uranium reduction journal, August 2015

Low-temperature isotopic fractionation of uranium journal, December 2007

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

The terrestrial uranium isotope cycle journal, January 2015

Uranium Reoxidation in Previously Bioreduced Sediment by Dissolved Oxygen and Nitrate journal, July 2007

Metatranscriptomic evidence of pervasive and diverse chemolithoautotrophy relevant to C, S, N and Fe cycling in a shallow alluvial aquifer journal, March 2016

Cr isotope fractionation factors for Cr(VI) reduction by a metabolically diverse group of bacteria journal, October 2014

Rate-limited U(VI) desorption during a small-scale tracer test in a heterogeneous uranium-contaminated aquifer: RATE-LIMITED U(VI) DESORPTION IN A U-CONTAMINATED AQUIFER journal, May 2012

Uranium isotope systematics of ferromanganese crusts in the Pacific Ocean: Implications for the marine 238 U/ 235 U isotope system journal, December 2014

Characterization and remediation of soils contaminated with uranium journal, April 2009

Uranium Mill Tailings: Geochemistry, Mineralogy, and Environmental Impact journal, December 2006

Selenium isotope fractionation during reduction by Fe(II)-Fe(III) hydroxide-sulfate (green rust) journal, February 2003

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

Uranium Bioreduction Rates across Scales: Biogeochemical Hot Moments and Hot Spots during a Biostimulation Experiment at Rifle, Colorado journal, August 2014

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

Anaerobic, Nitrate-Dependent Oxidation of U(IV) Oxide Minerals by the Chemolithoautotrophic Bacterium Thiobacillus denitrificans journal, April 2005

Biogeochemical Controls on the Product of Microbial U(VI) Reduction journal, October 2013

Uranium Reduction journal, October 2006

In Situ Bioreduction of Technetium and Uranium in a Nitrate-Contaminated Aquifer journal, January 2004

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

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

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

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

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

Oxidative dissolution of UO2 in a simulated groundwater containing synthetic nanocrystalline mackinawite journal, February 2013

Uranium isotopes distinguish two geochemically distinct stages during the later Cambrian SPICE event journal, September 2014

In situ mobility of uranium in the presence of nitrate following sulfate-reducing conditions journal, April 2016

Anaerobic, Nitrate-Dependent Oxidation of Pyrite Nanoparticles by Thiobacillus denitrificans journal, January 2012

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

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Fractionation of selenium isotopes during bacterial respiratory reduction of selenium oxyanions journal, November 2000

Chromium Isotopes and the Fate of Hexavalent Chromium in the Environment journal, March 2002

Uranium Isotopic Fractionation Induced by U(VI) Adsorption onto Common Aquifer Minerals journal, October 2016

Colloid Mobilization During Soil Iron Redox Oscillations journal, September 2006

Reactive transport of uranium in a groundwater bioreduction study: Insights from high-temporal resolution 238U/235U data journal, August 2016

On the change in UO 2 redox reactivity as a function of H 2 O 2 exposure journal, January 2020

Title: Field Application of ²³⁸U/²³⁵U Measurements To Detect Reoxidation and Mobilization of U(IV)

Stimulating the In Situ Activity of Geobacter Species To Remove Uranium from the Groundwater of a Uranium-Contaminated Aquifer
journal, October 2003

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

Isotope fractionation of 238U and 235U during biologically-mediated uranium reduction
journal, August 2015

Low-temperature isotopic fractionation of uranium
journal, December 2007

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

The terrestrial uranium isotope cycle
journal, January 2015

Uranium Reoxidation in Previously Bioreduced Sediment by Dissolved Oxygen and Nitrate
journal, July 2007

Metatranscriptomic evidence of pervasive and diverse chemolithoautotrophy relevant to C, S, N and Fe cycling in a shallow alluvial aquifer
journal, March 2016

Cr isotope fractionation factors for Cr(VI) reduction by a metabolically diverse group of bacteria
journal, October 2014

Rate-limited U(VI) desorption during a small-scale tracer test in a heterogeneous uranium-contaminated aquifer: RATE-LIMITED U(VI) DESORPTION IN A U-CONTAMINATED AQUIFER
journal, May 2012

Uranium isotope systematics of ferromanganese crusts in the Pacific Ocean: Implications for the marine 238 U/ 235 U isotope system
journal, December 2014

Characterization and remediation of soils contaminated with uranium
journal, April 2009

Uranium Mill Tailings: Geochemistry, Mineralogy, and Environmental Impact
journal, December 2006

Selenium isotope fractionation during reduction by Fe(II)-Fe(III) hydroxide-sulfate (green rust)
journal, February 2003

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

Uranium Bioreduction Rates across Scales: Biogeochemical Hot Moments and Hot Spots during a Biostimulation Experiment at Rifle, Colorado
journal, August 2014

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

Anaerobic, Nitrate-Dependent Oxidation of U(IV) Oxide Minerals by the Chemolithoautotrophic Bacterium Thiobacillus denitrificans
journal, April 2005

Biogeochemical Controls on the Product of Microbial U(VI) Reduction
journal, October 2013

Uranium Reduction
journal, October 2006

In Situ Bioreduction of Technetium and Uranium in a Nitrate-Contaminated Aquifer
journal, January 2004

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

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

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

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

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

Oxidative dissolution of UO2 in a simulated groundwater containing synthetic nanocrystalline mackinawite
journal, February 2013

Uranium isotopes distinguish two geochemically distinct stages during the later Cambrian SPICE event
journal, September 2014

In situ mobility of uranium in the presence of nitrate following sulfate-reducing conditions
journal, April 2016

Anaerobic, Nitrate-Dependent Oxidation of Pyrite Nanoparticles by Thiobacillus denitrificans
journal, January 2012

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

Speciation and Reactivity of Uranium Products Formed during in Situ Bioremediation in a Shallow Alluvial Aquifer
journal, October 2014

Uranium isotopes fingerprint biotic reduction
journal, April 2015

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

Hierarchical Bayesian method for mapping biogeochemical hot spots using induced polarization imaging
journal, January 2016

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

In - Situ Evidence for Uranium Immobilization and Remobilization
journal, April 2002

Biogenic U(IV) oxidation by dissolved oxygen and nitrate in sediment after prolonged U(VI)/Fe(III)/SO42− reduction
journal, February 2009

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

Influence of Iron Sulfides on Abiotic Oxidation of UO ₂ by Nitrite and Dissolved Oxygen in Natural Sediments
journal, January 2015

Physicochemical Heterogeneity Controls on Uranium Bioreduction Rates at the Field Scale
journal, December 2011

Nano-FeS Inhibits UO ₂ Reoxidation under Varied Oxic Conditions
journal, December 2013

Fractionation of selenium isotopes during bacterial respiratory reduction of selenium oxyanions
journal, November 2000

Chromium Isotopes and the Fate of Hexavalent Chromium in the Environment
journal, March 2002

Uranium Isotopic Fractionation Induced by U(VI) Adsorption onto Common Aquifer Minerals
journal, October 2016

Colloid Mobilization During Soil Iron Redox Oscillations
journal, September 2006

Reactive transport of uranium in a groundwater bioreduction study: Insights from high-temporal resolution 238U/235U data
journal, August 2016

On the change in UO ₂ redox reactivity as a function of H ₂ O ₂ exposure
journal, January 2020