Oxidative Uranium Release from Anoxic Sediments under Diffusion-Limited Conditions

Bone, Sharon E.; Cahill, Melanie R.; Jones, Morris E.; Fendorf, Scott; Davis, James; Williams, Kenneth H.; Bargar, John R.

doi:10.1021/acs.est.7b02241

Title: Oxidative Uranium Release from Anoxic Sediments under Diffusion-Limited Conditions

Journal Article · Wed Sep 06 00:00:00 EDT 2017 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.7b02241· OSTI ID:1463304

^[1]; Cahill, Melanie R. ^[2]; Jones, Morris E. ^[3];

^[2]; Davis, James ^[4]; Williams, Kenneth H. ^[5];

^[1]

SLAC National Accelerator Lab., Menlo Park, CA (United States)
Stanford Univ., Stanford, CA (United States)
Stanford Univ., Stanford, CA (United States); Univ. of Massachusetts, Amherst, MA (United States)
U.S. Geological Survey, Menlo Park, CA (United States)
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Uranium (U) contamination occurs as a result of mining and ore processing; often in alluvial aquifers that contain organic-rich, reduced sediments that accumulate tetravalent U, U(IV). Uranium(IV) is sparingly soluble, but may be mobilized upon exposure to nitrate (NO₃-) and oxygen (O₂), which become elevated in groundwater due to seasonal fluctuations in the water table. The extent to which oxidative U mobilization can occur depends upon the transport properties of the sediments, the rate of U(IV) oxidation, and the availability of inorganic reductants and organic electron donors that consume oxidants. We investigated the processes governing U release upon exposure of reduced sediments to artificial groundwater containing O₂ or NO₃- under diffusion-limited conditions. Little U was mobilized during the 85-day reaction, despite rapid diffusion of groundwater within the sediments and the presence of nonuraninite U(IV) species. The production of ferrous iron and sulfide in conjunction with rapid oxidant consumption suggested that the sediments harbored large concentrations of bioavailable organic carbon that fueled anaerobic microbial respiration and stabilized U(IV). Our results suggest that seasonal influxes of O₂ and NO₃- may cause only localized mobilization of U without leading to export of U from the reducing sediments when ample organic carbon is present.

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Research Organization:: SLAC National Accelerator Laboratory (SLAC), Menlo Park, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

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

Grant/Contract Number:: AC02-76SF00515; AC02-05CH11231

OSTI ID:: 1463304

Alternate ID(s):: OSTI ID: 1476550

Journal Information:: Environmental Science and Technology, Vol. 51, Issue 19; ISSN 0013-936X

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 17 works

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References (45)

Uranium Mill Tailings: Geochemistry, Mineralogy, and Environmental Impact Abdelouas, A. Elements, Vol. 2, Issue 6 https://doi.org/10.2113/gselements.2.6.335	journal	December 2006
Bioremediation of uranium-contaminated groundwater: a systems approach to subsurface biogeochemistry Williams, Kenneth H.; Bargar, John R.; Lloyd, Jonathan R. Current Opinion in Biotechnology, Vol. 24, Issue 3 https://doi.org/10.1016/j.copbio.2012.10.008	journal	June 2013
Geochemical, mineralogical and microbiological characteristics of sediment from a naturally reduced zone in a uranium-contaminated aquifer Campbell, K. M.; Kukkadapu, R. K.; Qafoku, N. P. Applied Geochemistry, Vol. 27, Issue 8 https://doi.org/10.1016/j.apgeochem.2012.04.013	journal	August 2012
Physico-Chemical Heterogeneity of Organic-Rich Sediments in the Rifle Aquifer, CO: Impact on Uranium Biogeochemistry Janot, Noémie; Lezama Pacheco, Juan S.; Pham, Don Q. Environmental Science & Technology, Vol. 50, Issue 1 https://doi.org/10.1021/acs.est.5b03208	journal	December 2015
Environmental Speciation of Actinides Maher, Kate; Bargar, John R.; Brown, Gordon E. Inorganic Chemistry, Vol. 52, Issue 7 https://doi.org/10.1021/ic301686d	journal	June 2012
Acetate Availability and its Influence on Sustainable Bioremediation of Uranium-Contaminated Groundwater Williams, Kenneth H.; Long, Philip E.; Davis, James A. Geomicrobiology Journal, Vol. 28, Issue 5-6 https://doi.org/10.1080/01490451.2010.520074	journal	June 2011
Refining the site conceptual model at a former uranium mill site in Riverton, Wyoming, USA Dam, William L.; Campbell, Sam; Johnson, Raymond H. Environmental Earth Sciences, Vol. 74, Issue 10 https://doi.org/10.1007/s12665-015-4706-y	journal	July 2015
Persistence of uranium groundwater plumes: Contrasting mechanisms at two DOE sites in the groundwater–river interaction zone Zachara, John M.; Long, Philip E.; Bargar, John Journal of Contaminant Hydrology, Vol. 147 https://doi.org/10.1016/j.jconhyd.2013.02.001	journal	April 2013
Water Table Dynamics and Biogeochemical Cycling in a Shallow, Variably-Saturated Floodplain Yabusaki, Steven B.; Wilkins, Michael J.; Fang, Yilin Environmental Science & Technology, Vol. 51, Issue 6 https://doi.org/10.1021/acs.est.6b04873	journal	March 2017
Buried organic-rich horizons: their role as nitrogen sources in stream riparian zones Hill, Alan R. Biogeochemistry, Vol. 104, Issue 1-3 https://doi.org/10.1007/s10533-010-9507-5	journal	July 2010
In - Situ Evidence for Uranium Immobilization and Remobilization Senko, John M.; Istok, Jonathan D.; Suflita, Joseph M. Environmental Science & Technology, Vol. 36, Issue 7 https://doi.org/10.1021/es011240x	journal	April 2002
Anaerobic, Nitrate-Dependent Oxidation of U(IV) Oxide Minerals by the Chemolithoautotrophic Bacterium Thiobacillus denitrificans Beller, Harry R. Applied and Environmental Microbiology, Vol. 71, Issue 4 https://doi.org/10.1128/AEM.71.4.2170-2174.2005	journal	April 2005
Geochemical Controls on Microbial Nitrate-Dependent U(IV) Oxidation Senko, John M.; Suflita, Joseph M.; Krumholz, Lee R. Geomicrobiology Journal, Vol. 22, Issue 7-8 https://doi.org/10.1080/01490450500248911	journal	October 2005
Multiple influences of nitrate on uranium solubility during bioremediation of uranium-contaminated subsurface sediments Finneran, Kevin T.; Housewright, Meghan E.; Lovley, Derek R. Environmental Microbiology, Vol. 4, Issue 9 https://doi.org/10.1046/j.1462-2920.2002.00317.x	journal	September 2002
Effects of Nitrate on the Stability of Uranium in a Bioreduced Region of the Subsurface Wu, Wei-Min; Carley, Jack; Green, Stefan J. Environmental Science & Technology, Vol. 44, Issue 13 https://doi.org/10.1021/es1000837	journal	July 2010
In Situ Bioreduction of Technetium and Uranium in a Nitrate-Contaminated Aquifer Istok, J. D.; Senko, J. M.; Krumholz, L. R. Environmental Science & Technology, Vol. 38, Issue 2 https://doi.org/10.1021/es034639p	journal	January 2004
Long-Term in Situ Oxidation of Biogenic Uraninite in an Alluvial Aquifer: Impact of Dissolved Oxygen and Calcium Lezama-Pacheco, Juan S.; Cerrato, José M.; Veeramani, Harish Environmental Science & Technology, Vol. 49, Issue 12 https://doi.org/10.1021/acs.est.5b00949	journal	June 2015
Understanding controls on redox processes in floodplain sediments of the Upper Colorado River Basin Noël, Vincent; Boye, Kristin; Kukkadapu, Ravi K. Science of The Total Environment, Vol. 603-604 https://doi.org/10.1016/j.scitotenv.2017.01.109	journal	December 2017
Comparative dissolution kinetics of biogenic and chemogenic uraninite under oxidizing conditions in the presence of carbonate Ulrich, Kai-Uwe; Ilton, Eugene S.; Veeramani, Harish Geochimica et Cosmochimica Acta, Vol. 73, Issue 20 https://doi.org/10.1016/j.gca.2009.07.012	journal	October 2009
Relative Reactivity of Biogenic and Chemogenic Uraninite and Biogenic Noncrystalline U(IV) Cerrato, José M.; Ashner, Matthew N.; Alessi, Daniel S. Environmental Science & Technology, Vol. 47, Issue 17 https://doi.org/10.1021/es401663t	journal	August 2013
Influence of Iron Sulfides on Abiotic Oxidation of UO ₂ by Nitrite and Dissolved Oxygen in Natural Sediments Carpenter, Julian; Bi, Yuqiang; Hayes, Kim F. Environmental Science & Technology, Vol. 49, Issue 2 https://doi.org/10.1021/es504481n	journal	January 2015
In situ mobility of uranium in the presence of nitrate following sulfate-reducing conditions Paradis, Charles J.; Jagadamma, Sindhu; Watson, David B. Journal of Contaminant Hydrology, Vol. 187 https://doi.org/10.1016/j.jconhyd.2016.02.002	journal	April 2016
Role for Fe(III) Minerals in Nitrate-Dependent Microbial U(IV) Oxidation Senko, John M.; Mohamed, Yasser; Dewers, Thomas A. Environmental Science & Technology, Vol. 39, Issue 8 https://doi.org/10.1021/es048906i	journal	April 2005
Postbiostimulation microbial community structure changes that control the reoxidation of uranium: Postbiostimulation microbial community structure N'Guessan, Adeola Lucie; Moon, Hee Sun; Peacock, Aaron D. FEMS Microbiology Ecology, Vol. 74, Issue 1 https://doi.org/10.1111/j.1574-6941.2010.00933.x	journal	September 2010
Degradation of natural organic matter: A thermodynamic analysis LaRowe, Douglas E.; Van Cappellen, Philippe Geochimica et Cosmochimica Acta, Vol. 75, Issue 8 https://doi.org/10.1016/j.gca.2011.01.020	journal	April 2011
Predicting the rate of microbial respiration in geochemical environments Jin, Qusheng; Bethke, Craig M. Geochimica et Cosmochimica Acta, Vol. 69, Issue 5 https://doi.org/10.1016/j.gca.2004.08.010	journal	March 2005
Thermodynamically controlled preservation of organic carbon in floodplains Boye, Kristin; Noël, Vincent; Tfaily, Malak M. Nature Geoscience, Vol. 10, Issue 6 https://doi.org/10.1038/ngeo2940	journal	May 2017
Influence of hydrological, biogeochemical and temperature transients on subsurface carbon fluxes in a flood plain environment Arora, Bhavna; Spycher, Nicolas F.; Steefel, Carl I. Biogeochemistry, Vol. 127, Issue 2-3 https://doi.org/10.1007/s10533-016-0186-8	journal	February 2016
Development of a Gold Amalgam Voltammetric Microelectrode for the Determination of Dissolved Fe, Mn, O2, and S(-II) in Porewaters of Marine and Freshwater Sediments Brendel, Paul J.; Luther, George W. III. Environmental Science & Technology, Vol. 29, Issue 3 https://doi.org/10.1021/es00003a024	journal	March 1995
ATHENA , ARTEMIS , HEPHAESTUS : data analysis for X-ray absorption spectroscopy using IFEFFIT Ravel, B.; Newville, M. Journal of Synchrotron Radiation, Vol. 12, Issue 4 https://doi.org/10.1107/S0909049505012719	journal	June 2005
Beam-induced oxidation of monomeric U(IV) species Alessi, Daniel S.; Uster, Benjamin; Borca, Camelia N. Journal of Synchrotron Radiation, Vol. 20, Issue 1 https://doi.org/10.1107/S0909049512041763	journal	November 2012
Chemistry of Iron Sulfides Rickard, David; Luther, George W. Chemical Reviews, Vol. 107, Issue 2 https://doi.org/10.1021/cr0503658	journal	February 2007
Tetra- and Hexavalent Uranium Forms Bidentate-Mononuclear Complexes with Particulate Organic Matter in a Naturally Uranium-Enriched Peatland Mikutta, Christian; Langner, Peggy; Bargar, John R. Environmental Science & Technology, Vol. 50, Issue 19 https://doi.org/10.1021/acs.est.6b03688	journal	September 2016
Quantitative Separation of Monomeric U(IV) from UO ₂ in Products of U(VI) Reduction Alessi, Daniel S.; Uster, Benjamin; Veeramani, Harish Environmental Science & Technology, Vol. 46, Issue 11 https://doi.org/10.1021/es204123z	journal	May 2012
Solution and Microbial Controls on the Formation of Reduced U(IV) Species Boyanov, Maxim I.; Fletcher, Kelly E.; Kwon, Man Jae Environmental Science & Technology, Vol. 45, Issue 19 https://doi.org/10.1021/es2014049	journal	October 2011
The product of microbial uranium reduction includes multiple species with U(IV)–phosphate coordination Alessi, Daniel S.; Lezama-Pacheco, Juan S.; Stubbs, Joanne E. Geochimica et Cosmochimica Acta, Vol. 131 https://doi.org/10.1016/j.gca.2014.01.005	journal	April 2014
Biogeochemical Controls on the Product of Microbial U(VI) Reduction Stylo, Malgorzata; Alessi, Daniel S.; Shao, Paul PaoYun Environmental Science & Technology, Vol. 47, Issue 21 https://doi.org/10.1021/es402631w	journal	October 2013
Uranium(IV) adsorption by natural organic matter in anoxic sediments Bone, Sharon E.; Dynes, James J.; Cliff, John Proceedings of the National Academy of Sciences, Vol. 114, Issue 4 https://doi.org/10.1073/pnas.1611918114	journal	January 2017
Mobile uranium(IV)-bearing colloids in a mining-impacted wetland Wang, Yuheng; Frutschi, Manon; Suvorova, Elena Nature Communications, Vol. 4, Issue 1 https://doi.org/10.1038/ncomms3942	journal	December 2013
Colloid Mobilization During Soil Iron Redox Oscillations Thompson, Aaron; Chadwick, Oliver A.; Boman, Sarah Environmental Science & Technology, Vol. 40, Issue 18 https://doi.org/10.1021/es061203b	journal	September 2006
Mobilization of colloidal carbon during iron reduction in basaltic soils Buettner, Shea W.; Kramer, Marc G.; Chadwick, Oliver A. Geoderma, Vol. 221-222 https://doi.org/10.1016/j.geoderma.2014.01.012	journal	June 2014
Oxidative Dissolution of Biogenic Uraninite in Groundwater at Old Rifle, CO Campbell, Kate M.; Veeramani, Harish; Ulrich, Kai-Uwe Environmental Science & Technology, Vol. 45, Issue 20 https://doi.org/10.1021/es200482f	journal	October 2011
Surface Passivation Limited UO ₂ Oxidative Dissolution in the Presence of FeS Bi, Yuqiang; Hayes, Kim F. Environmental Science & Technology, Vol. 48, Issue 22 https://doi.org/10.1021/es5041392	journal	October 2014
Are oxygen limitations under recognized regulators of organic carbon turnover in upland soils? Keiluweit, Marco; Nico, Peter S.; Kleber, Markus Biogeochemistry, Vol. 127, Issue 2-3 https://doi.org/10.1007/s10533-015-0180-6	journal	January 2016
Mineral protection of soil carbon counteracted by root exudates Keiluweit, Marco; Bougoure, Jeremy J.; Nico, Peter S. Nature Climate Change, Vol. 5, Issue 6 https://doi.org/10.1038/nclimate2580	journal	March 2015

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