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

Journal Article · Tue May 19 00:00:00 EDT 2015 · Environmental Science and Technology

DOI:https://doi.org/10.1021/acs.est.5b00701· OSTI ID:1193681

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)

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.

View Accepted Manuscript (DOE)

Cite

Export

Save

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

Sponsoring Organization:: USDOE

Grant/Contract Number:: AC52-06NA25396

OSTI ID:: 1193681

Report Number(s):: LA-UR-15-21333

Journal Information:: Environmental Science and Technology, Vol. 49, Issue 10; ISSN 0013-936X

Country of Publication:: United States

Language:: English

Citation Metrics:

Cited by: 39 works

Citation information provided by
Web of Science

References (63)

Critical review of acid in situ leach uranium mining: 1. USA and Australia Mudd, Gavin Environmental Geology, Vol. 41, Issue 3-4 https://doi.org/10.1007/s002540100406	journal	December 2001
The future of Yellowcake: A global assessment of uranium resources and mining Mudd, Gavin M. Science of The Total Environment, Vol. 472 https://doi.org/10.1016/j.scitotenv.2013.11.070	journal	February 2014
Sustainability of Uranium Mining and Milling: Toward Quantifying Resources and Eco-Efficiency Mudd, Gavin M.; Diesendorf, Mark Environmental Science & Technology, Vol. 42, Issue 7 https://doi.org/10.1021/es702249v	journal	March 2008
A top-down assessment of energy, water and land use in uranium mining, milling, and refining Schneider, E.; Carlsen, B.; Tavrides, E. Energy Economics, Vol. 40 https://doi.org/10.1016/j.eneco.2013.08.006	journal	November 2013
Evolution of uranium and thorium minerals Hazen, R. M.; Ewing, R. C.; Sverjensky, D. A. American Mineralogist, Vol. 94, Issue 10 https://doi.org/10.2138/am.2009.3208	journal	October 2009
Uranium Deposits of the World: Asia Dahlkamp, Franz J. https://doi.org/10.1007/978-3-540-78558-3	reference-book	January 2009
Uranium ore rolls; an analysis Shawe, D. R.; Granger, H. C. Economic Geology, Vol. 60, Issue 2 https://doi.org/10.2113/gsecongeo.60.2.240	journal	March 1965
Groundwater processes and sedimentary uranium deposits Hobday, D. K.; Galloway, W. E. Hydrogeology Journal, Vol. 7, Issue 1 https://doi.org/10.1007/s100400050184	journal	February 1999
Role of nuclear volume in driving equilibrium stable isotope fractionation of mercury, thallium, and other very heavy elements Schauble, Edwin A. Geochimica et Cosmochimica Acta, Vol. 71, Issue 9 https://doi.org/10.1016/j.gca.2007.02.004	journal	May 2007
Nuclear Size and Shape Effects in Chemical Reactions. Isotope Chemistry of the Heavy Elements Bigeleisen, Jacob Journal of the American Chemical Society, Vol. 118, Issue 15 https://doi.org/10.1021/ja954076k	journal	January 1996
Nuclear field shift in natural environments Moynier, Frédéric; Fujii, Toshiyuki; Brennecka, Gregory A. Comptes Rendus Geoscience, Vol. 345, Issue 3 https://doi.org/10.1016/j.crte.2013.01.004	journal	March 2013
An ab initio molecular orbital study of the nuclear volume effects in uranium isotope fractionations Abe, Minori; Suzuki, Tatsuya; Fujii, Yasuhiko The Journal of Chemical Physics, Vol. 129, Issue 16 https://doi.org/10.1063/1.2992616	journal	October 2008
Natural fractionation of 238U/235U Weyer, S.; Anbar, A. D.; Gerdes, A. Geochimica et Cosmochimica Acta, Vol. 72, Issue 2 https://doi.org/10.1016/j.gca.2007.11.012	journal	January 2008
Low-temperature isotopic fractionation of uranium Stirling, Claudine H.; Andersen, Morten B.; Potter, Emma-Kate Earth and Planetary Science Letters, Vol. 264, Issue 1-2 https://doi.org/10.1016/j.epsl.2007.09.019	journal	December 2007
Natural variations in uranium isotope ratios of uranium ore concentrates: Understanding the 238U/235U fractionation mechanism Brennecka, Gregory A.; Borg, Lars E.; Hutcheon, Ian D. Earth and Planetary Science Letters, Vol. 291, Issue 1-4 https://doi.org/10.1016/j.epsl.2010.01.023	journal	March 2010
Variations in 238U/235U in uranium ore deposits: Isotopic signatures of the U reduction process? Bopp, Charles John; Lundstrom, Craig C.; Johnson, Thomas M. Geology, Vol. 37, Issue 7 https://doi.org/10.1130/G25550A.1	journal	July 2009
Fractionation of 238U/235U by reduction during low temperature uranium mineralisation processes Murphy, Melissa J.; Stirling, Claudine H.; Kaltenbach, Angela Earth and Planetary Science Letters, Vol. 388 https://doi.org/10.1016/j.epsl.2013.11.034	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. Bopp, Charles John; Lundstrom, Craig C.; Johnson, Thomas M. Environmental Science & Technology, Vol. 44, Issue 15 https://doi.org/10.1021/es100643v	journal	August 2010
Uranium isotopic fractionation factors during U(VI) reduction by bacterial isolates Basu, Anirban; Sanford, Robert A.; Johnson, Thomas M. Geochimica et Cosmochimica Acta, Vol. 136 https://doi.org/10.1016/j.gca.2014.02.041	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 Shiel, Alyssa E.; Laubach, Parker G.; Johnson, Thomas M. Environmental Science & Technology, Vol. 47, Issue 6 https://doi.org/10.1021/es303913y	journal	February 2013
Unstable sulfur compounds and the origin of roll-type uranium deposits Granger, H. C.; Warren, C. G. Economic Geology, Vol. 64, Issue 2 https://doi.org/10.2113/gsecongeo.64.2.160	journal	April 1969
Iron disulfide minerals and the genesis of roll-type uranium deposits Reynolds, Richard L.; Goldhaber, Martin B. Economic Geology, Vol. 78, Issue 1 https://doi.org/10.2113/gsecongeo.78.1.105	journal	February 1983
Similarities, differences, and some genetic problems of the wyoming and colorado plateau types of uranium deposits in sandstone Fischer, R. P. Economic Geology, Vol. 65, Issue 7 https://doi.org/10.2113/gsecongeo.65.7.778	journal	November 1970
Sulfur isotopes and the origin of sandstone-type uranium deposits [Colorado Plateau and Wyoming] Jensen, Mead LeRoy Economic Geology, Vol. 53, Issue 5 https://doi.org/10.2113/gsecongeo.53.5.598	journal	August 1958
Geochemistry of selenium: formation of ferroselite and selenium behavior in the vicinity of oxidizing sulfide and uranium deposits Hatten Howard, J. Geochimica et Cosmochimica Acta, Vol. 41, Issue 11 https://doi.org/10.1016/0016-7037(77)90176-4	journal	November 1977
12. Biogeochemistry of Sulfur Isotopes Canfield, D. E. Stable Isotope Geochemistry https://doi.org/10.1515/9781501508745-015	book	January 2001
The kinetic isotope effect in the chemical reduction of sulphate Harrison, A. G.; Thode, H. G. Transactions of the Faraday Society, Vol. 53 https://doi.org/10.1039/tf9575301648	journal	January 1957
8. The Behavior of U- and Th-series Nuclides in Groundwater Porcelli, Donald; Swarzenski, Peter W. Uranium-series Geochemistry https://doi.org/10.1515/9781501509308-013	book	December 2003
The mineral dissolution rate conundrum: Insights from reactive transport modeling of U isotopes and pore fluid chemistry in marine sediments Maher, Kate; Steefel, Carl I.; DePaolo, Donald J. Geochimica et Cosmochimica Acta, Vol. 70, Issue 2 https://doi.org/10.1016/j.gca.2005.09.001	journal	January 2006
U–Sr isotopic speedometer: Fluid flow and chemical weathering rates in aquifers Maher, Kate; DePaolo, Donald J.; Christensen, John N. Geochimica et Cosmochimica Acta, Vol. 70, Issue 17 https://doi.org/10.1016/j.gca.2006.06.1559	journal	September 2006
Alpha-Recoil Thorium-234: Dissolution into Water and the Uranium-234/Uranium-238 Disequilibrium in Nature Kigoshi, K. Science, Vol. 173, Issue 3991 https://doi.org/10.1126/science.173.3991.47	journal	July 1971
Sediment transport time measured with U-series isotopes: Results from ODP North Atlantic drift site 984 DePaolo, Donald J.; Maher, Kate; Christensen, John N. Earth and Planetary Science Letters, Vol. 248, Issue 1-2 https://doi.org/10.1016/j.epsl.2006.06.004	journal	August 2006
Experimental evidence for 234U–238U fractionation during granite weathering with implications for 234U/238U in natural waters Andersen, Morten B.; Erel, Yigal; Bourdon, Bernard Geochimica et Cosmochimica Acta, Vol. 73, Issue 14 https://doi.org/10.1016/j.gca.2009.04.020	journal	July 2009
Identifying the Sources of Subsurface Contamination at the Hanford Site in Washington using High-Precision Uranium Isotopic Measurements Christensen, John N.; Dresel, P. Evan; Conrad, Mark E. Environmental Science & Technology, Vol. 38, Issue 12 https://doi.org/10.1021/es034700q	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 Druhan, Jennifer L.; Steefel, Carl I.; Conrad, Mark E. Geochimica et Cosmochimica Acta, Vol. 124 https://doi.org/10.1016/j.gca.2013.08.037	journal	January 2014
A Bacterial Method for the Nitrogen Isotopic Analysis of Nitrate in Seawater and Freshwater Sigman, D. M.; Casciotti, K. L.; Andreani, M. Analytical Chemistry, Vol. 73, Issue 17 https://doi.org/10.1021/ac010088e	journal	September 2001
Measurement of the Oxygen Isotopic Composition of Nitrate in Seawater and Freshwater Using the Denitrifier Method Casciotti, K. L.; Sigman, D. M.; Hastings, M. Galanter Analytical Chemistry, Vol. 74, Issue 19 https://doi.org/10.1021/ac020113w	journal	October 2002
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
The effect of calcium on aqueous uranium(VI) speciation and adsorption to ferrihydrite and quartz Fox, Patricia M.; Davis, James A.; Zachara, John M. Geochimica et Cosmochimica Acta, Vol. 70, Issue 6 https://doi.org/10.1016/j.gca.2005.11.027	journal	March 2006
Uranyl(VI) carbonate complex formation: Validation of the Ca2UO2(CO3)3(aq.) species Bernhard, G.; Geipel, Gerhard; Reich, T. Radiochimica Acta, Vol. 89, Issue 8 https://doi.org/10.1524/ract.2001.89.8.511	journal	January 2001
Adsorption of uranyl onto ferric oxyhydroxides: Application of the surface complexation site-binding model Hsi, Ching-kuo Daniel; Langmuir, Donald Geochimica et Cosmochimica Acta, Vol. 49, Issue 9, p. 1931-1941 https://doi.org/10.1016/0016-7037(85)90088-2	journal	September 1985
Uranium(VI) adsorption to ferrihydrite: Application of a surface complexation model Waite, T. D.; Davis, J. A.; Payne, T. E. Geochimica et Cosmochimica Acta, Vol. 58, Issue 24 https://doi.org/10.1016/0016-7037(94)90243-7	journal	December 1994
Sorption of uranyl ions on hydrous titanium dioxide Lieser, K. H.; Thybusch, B. Fresenius' Zeitschrift für analytische Chemie, Vol. 332, Issue 4 https://doi.org/10.1007/BF00468814	journal	January 1988
Approaches to surface complexation modeling of Uranium(VI) adsorption on aquifer sediments Davis, James A.; Meece, David E.; Kohler, Matthias Geochimica et Cosmochimica Acta, Vol. 68, Issue 18 https://doi.org/10.1016/j.gca.2004.03.003	journal	September 2004
Interactions of aqueous U(VI) with soil minerals in slightly alkaline natural systems Qafoku, Nikolla P.; Icenhower, Jonathan P. Reviews in Environmental Science and Bio/Technology, Vol. 7, Issue 4 https://doi.org/10.1007/s11157-008-9137-8	journal	August 2008
Bicarbonate impact on U(VI) bioreduction in a shallow alluvial aquifer Long, Philip E.; Williams, Kenneth H.; Davis, James A. Geochimica et Cosmochimica Acta, Vol. 150 https://doi.org/10.1016/j.gca.2014.11.013	journal	February 2015
Speciation-Dependent Kinetics of Uranium(VI) Bioreduction Ulrich, Kai-Uwe; Veeramani, Harish; Bernier-Latmani, Rizlan Geomicrobiology Journal, Vol. 28, Issue 5-6 https://doi.org/10.1080/01490451.2010.507640	journal	June 2011
Redox Processes and Water Quality of Selected Principal Aquifer Systems McMahon, P. B.; Chapelle, F. H. Ground Water, Vol. 46, Issue 2 https://doi.org/10.1111/j.1745-6584.2007.00385.x	journal	March 2008
The thermodynamic ladder in geomicrobiology Bethke, C. M.; Sanford, R. A.; Kirk, M. F. American Journal of Science, Vol. 311, Issue 3 https://doi.org/10.2475/03.2011.01	journal	March 2011
Using isotope fractionation of nitrate-nitrogen and nitrate-oxygen for evaluation of microbial denitrification in a sandy aquifer Böttcher, J.; Strebel, O.; Voerkelius, Susanne Journal of Hydrology, Vol. 114, Issue 3-4 https://doi.org/10.1016/0022-1694(90)90068-9	journal	May 1990
Stable Isotopes of Oxygen and Nitrogen in Source Identification of Nitrate from Septic Systems Aravena, R.; Evans, M. L.; Cherry, J. A. Ground Water, Vol. 31, Issue 2 https://doi.org/10.1111/j.1745-6584.1993.tb01809.x	journal	March 1993
Multiple Geochemical and Isotopic Approaches for Assessing Ground Water NO3- Elimination in a Riparian Zone Mengis, M.; Schif, S. L.; Harris, M. Ground Water, Vol. 37, Issue 3 https://doi.org/10.1111/j.1745-6584.1999.tb01124.x	journal	May 1999
Role of the riparian zone in controlling the distribution and fate of agricultural nitrogen near a small stream in southern Ontario Cey, Edwin E.; Rudolph, David L.; Aravena, Ramon Journal of Contaminant Hydrology, Vol. 37, Issue 1-2 https://doi.org/10.1016/S0169-7722(98)00162-4	journal	April 1999
Modelling nitrogen and oxygen isotope fractionation during denitrification in a lacustrine redox-transition zone Lehmann, Moritz F.; Reichert, Peter; Bernasconi, Stefano M. Geochimica et Cosmochimica Acta, Vol. 67, Issue 14 https://doi.org/10.1016/S0016-7037(03)00085-1	journal	July 2003
A dual isotope approach to identify denitrification in groundwater at a river-bank infiltration site Fukada, Teppei; Hiscock, Kevin M.; Dennis, Paul F. Water Research, Vol. 37, Issue 13 https://doi.org/10.1016/S0043-1354(03)00176-3	journal	July 2003
Does the Rayleigh Equation Apply to Evaluate Field Isotope Data in Contaminant Hydrogeology? Abe, Yumiko; Hunkeler, Daniel Environmental Science & Technology, Vol. 40, Issue 5 https://doi.org/10.1021/es051128p	journal	March 2006
Effective Isotopic Fractionation Factors for Solute Removal by Reactive Sediments: A Laboratory Microcosm and Slurry Study Clark, Scott K.; Johnson, Thomas M. Environmental Science & Technology, Vol. 42, Issue 21 https://doi.org/10.1021/es801814v	journal	October 2008
Cr Stable Isotopes As Indicators of Cr(VI) Reduction in Groundwater: A Detailed Time-Series Study of a Point-Source Plume Berna, Emily C.; Johnson, Thomas M.; Makdisi, Richard S. Environmental Science & Technology, Vol. 44, Issue 3 https://doi.org/10.1021/es902280s	journal	February 2010
Uranium Isotope Fractionation during Adsorption to Mn-Oxyhydroxides Brennecka, Gregory A.; Wasylenki, Laura E.; Bargar, John R. Environmental Science & Technology, Vol. 45, Issue 4 https://doi.org/10.1021/es103061v	journal	February 2011
Uranium comminution ages: Sediment transport and deposition time scales DePaolo, Donald J.; Lee, Victoria E.; Christensen, John N. Comptes Rendus Geoscience, Vol. 344, Issue 11-12 https://doi.org/10.1016/j.crte.2012.10.014	journal	November 2012
Uranium-series comminution ages of continental sediments: Case study of a Pleistocene alluvial fan Lee, Victoria E.; DePaolo, Donald J.; Christensen, John N. Earth and Planetary Science Letters, Vol. 296, Issue 3-4 https://doi.org/10.1016/j.epsl.2010.05.005	journal	August 2010
The transport of U- and Th-series nuclides in a sandy unconfined aquifer Tricca, A.; Wasserburg, G. J.; Porcelli, D. Geochimica et Cosmochimica Acta, Vol. 65, Issue 8 https://doi.org/10.1016/S0016-7037(00)00617-7	journal	April 2001
The transport of U- and Th-series nuclides in sandy confined aquifers Reynolds, B. C.; Wasserburg, G. J.; Baskaran, M. Geochimica et Cosmochimica Acta, Vol. 67, Issue 11 https://doi.org/10.1016/S0016-7037(02)01341-8	journal	June 2003

Cited By (4)

Identifying natural and anthropogenic variability of uranium at the well scale, Homestake Superfund site, near Milan, New Mexico, USA Harte, Philip T.; Blake, Johanna M.; Thomas, Jonathan Environmental Earth Sciences, Vol. 78, Issue 3 https://doi.org/10.1007/s12665-019-8049-y	journal	February 2019
Di- μ -acetato Diuranyl(VI) Complexes with N -(2-pyridyl)- N′ -(5-R-salicylidene)hydrazines: Syntheses, Structures, Properties and Extraction Studies Ghosh, Sabari; Kurapati, Sathish Kumar; Ghosh, Arpita ChemistrySelect, Vol. 3, Issue 17 https://doi.org/10.1002/slct.201800940	journal	May 2018
Differentiating anthropogenic and natural sources of uranium by geochemical fingerprinting of groundwater at the Homestake uranium mill, Milan, New Mexico, USA Blake, Johanna M.; Harte, Philip; Becher, Kent Environmental Earth Sciences, Vol. 78, Issue 13 https://doi.org/10.1007/s12665-019-8385-y	journal	June 2019
Uranium isotope fractionation by abiotic reductive precipitation Brown, Shaun T.; Basu, Anirban; Ding, Xin Proceedings of the National Academy of Sciences, Vol. 115, Issue 35 https://doi.org/10.1073/pnas.1805234115	journal	August 2018

Similar Records

Se Isotopes as groundwater redox indicators: Detecting natural attenuation of Se at an in situ recovery U mine

Journal Article · Mon Aug 22 00:00:00 EDT 2016 · Environmental Science and Technology · OSTI ID:1193681

Anirban, Basu; Schilling, Kathrin; Brown, Shaun T.; +7 more

Isotopic evidence for reductive immobilization of uranium across a roll-front mineral deposit

Journal Article · Fri May 20 00:00:00 EDT 2016 · Environmental Science and Technology · OSTI ID:1193681

Brown, Shaun T.; Basu, Anirban; Christensen, John N.; +8 more

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

Journal Article · Mon Dec 01 00:00:00 EST 2014 · Chemical Geology · OSTI ID:1193681

WoldeGabriel, G.; Boukhalfa, H.; Ware, S. D.; +13 more

Related Subjects

54 ENVIRONMENTAL SCIENCES
58 GEOSCIENCES
Planetary Sciences

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

Citation Formats

References (63)

Cited By (4)

Similar Records

Related Subjects