Se Isotopes as groundwater redox indicators: Detecting natural attenuation of Se at an in situ recovery U mine
Abstract
One of the major ecological concerns associated with the in situ recovery (ISR) of uranium (U) is the environmental release of soluble, toxic selenium (Se) oxyanions generated by mining. Post-mining natural attenuation by the residual reductants in the ore body and reduced down-gradient sediments should mitigate the risk of Se contamination in groundwater. In this work, we investigate the Se concentrations and Se isotope systematics of groundwater and of U ore bearing sediments from an ISR site at Rosita, TX, USA. Our results show that selenate (Se(VI)) is the dominant Se species in Rosita groundwater, and while several up-gradient wells have elevated Se(VI), the majority of the ore zone and down-gradient wells have little or no Se oxyanions. In addition, the δ 82 Se VI of Rosita groundwater is generally elevated relative to the U ore up to +6.14‰, with the most enriched values observed in the ore-zone wells. Increasing δ 82 Se with decreasing Se(VI) conforms to a Rayleigh type distillation model with an ϵ of -2.25‰ ± 0.61‰, suggesting natural Se(VI) reduction occurring along the hydraulic gradient at the Rosita ISR site. Furthermore, our results show that Se isotopes are excellent sensors for detecting and monitoring post-mining naturalmore »
- Authors:
-
[7];
[7];
- Univ. of California, Berkeley, CA (United States). Dept. of Earth and Planetary Science
- Univ. of California, Berkeley, CA (United States). Dept. of Environmental Science, Policy and Management
- Univ. of California, Berkeley, CA (United States). Dept. of Earth and Planetary Science; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Univ. of Illinois, Urbana-Champaign, IL (United States). Dept. of Geology
- Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
- Uranium Resources, Inc., Centennial, CO (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- Contributing Org.:
- Uranium Resources, Inc., Centennial, CO (United States)
- OSTI Identifier:
- 1345152
- Alternate Identifier(s):
- OSTI ID: 1440942
- Report Number(s):
- LA-UR-16-24690
Journal ID: ISSN 0013-936X
- Grant/Contract Number:
- AC52-06NA25396; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Environmental Science and Technology
- Additional Journal Information:
- Journal Volume: 50; Journal Issue: 20; Journal ID: ISSN 0013-936X
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 54 ENVIRONMENTAL SCIENCES; 58 GEOSCIENCES; Planetary Sciences
Citation Formats
Anirban, Basu, Schilling, Kathrin, Brown, Shaun T., Johnson, Thomas M., Christensen, John N., Hartmann, Matt, Reimus, Paul William, Heikoop, Jeffrey Martin, Woldegabriel, Giday, and DePaolo, Donald J. Se Isotopes as groundwater redox indicators: Detecting natural attenuation of Se at an in situ recovery U mine. United States: N. p., 2016.
Web. doi:10.1021/acs.est.6b01464.
Anirban, Basu, Schilling, Kathrin, Brown, Shaun T., Johnson, Thomas M., Christensen, John N., Hartmann, Matt, Reimus, Paul William, Heikoop, Jeffrey Martin, Woldegabriel, Giday, & DePaolo, Donald J. Se Isotopes as groundwater redox indicators: Detecting natural attenuation of Se at an in situ recovery U mine. United States. https://doi.org/10.1021/acs.est.6b01464
Anirban, Basu, Schilling, Kathrin, Brown, Shaun T., Johnson, Thomas M., Christensen, John N., Hartmann, Matt, Reimus, Paul William, Heikoop, Jeffrey Martin, Woldegabriel, Giday, and DePaolo, Donald J. Mon .
"Se Isotopes as groundwater redox indicators: Detecting natural attenuation of Se at an in situ recovery U mine". United States. https://doi.org/10.1021/acs.est.6b01464. https://www.osti.gov/servlets/purl/1345152.
@article{osti_1345152,
title = {Se Isotopes as groundwater redox indicators: Detecting natural attenuation of Se at an in situ recovery U mine},
author = {Anirban, Basu and Schilling, Kathrin and Brown, Shaun T. and Johnson, Thomas M. and Christensen, John N. and Hartmann, Matt and Reimus, Paul William and Heikoop, Jeffrey Martin and Woldegabriel, Giday and DePaolo, Donald J.},
abstractNote = {One of the major ecological concerns associated with the in situ recovery (ISR) of uranium (U) is the environmental release of soluble, toxic selenium (Se) oxyanions generated by mining. Post-mining natural attenuation by the residual reductants in the ore body and reduced down-gradient sediments should mitigate the risk of Se contamination in groundwater. In this work, we investigate the Se concentrations and Se isotope systematics of groundwater and of U ore bearing sediments from an ISR site at Rosita, TX, USA. Our results show that selenate (Se(VI)) is the dominant Se species in Rosita groundwater, and while several up-gradient wells have elevated Se(VI), the majority of the ore zone and down-gradient wells have little or no Se oxyanions. In addition, the δ 82 Se VI of Rosita groundwater is generally elevated relative to the U ore up to +6.14‰, with the most enriched values observed in the ore-zone wells. Increasing δ 82 Se with decreasing Se(VI) conforms to a Rayleigh type distillation model with an ϵ of -2.25‰ ± 0.61‰, suggesting natural Se(VI) reduction occurring along the hydraulic gradient at the Rosita ISR site. Furthermore, our results show that Se isotopes are excellent sensors for detecting and monitoring post-mining natural attenuation of Se oxyanions at ISR sites.},
doi = {10.1021/acs.est.6b01464},
journal = {Environmental Science and Technology},
number = 20,
volume = 50,
place = {United States},
year = {Mon Aug 22 00:00:00 EDT 2016},
month = {Mon Aug 22 00:00:00 EDT 2016}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 11 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Geochemistry of selenium: formation of ferroselite and selenium behavior in the vicinity of oxidizing sulfide and uranium deposits
journal, November 1977
- Hatten Howard, J.
- Geochimica et Cosmochimica Acta, Vol. 41, Issue 11
Unstable sulfur compounds and the origin of roll-type uranium deposits
journal, April 1969
- Granger, H. C.; Warren, C. G.
- Economic Geology, Vol. 64, Issue 2
Predicted equilibrium constants for solid and aqueous selenium species to 300 °C: applications to selenium-rich mineral deposits
journal, October 2003
- Xiong, Yongliang
- Ore Geology Reviews, Vol. 23, Issue 3-4
Environmental Speciation of Actinides
journal, June 2012
- Maher, Kate; Bargar, John R.; Brown, Gordon E.
- Inorganic Chemistry, Vol. 52, Issue 7
A critical review of thermodynamic data for selenium species at 25°C
journal, January 2001
- Séby, F.; Potin-Gautier, M.; Giffaut, E.
- Chemical Geology, Vol. 171, Issue 3-4
Accumulation of selenium in aquatic systems downstream of a uranium mining operation in northern Saskatchewan, Canada
journal, November 2008
- Muscatello, J. R.; Belknap, A. M.; Janz, D. M.
- Environmental Pollution, Vol. 156, Issue 2
Larval Deformities Associated with Selenium Accumulation in Northern Pike ( Esox lucius ) Exposed to Metal Mining Effluent
journal, October 2006
- Muscatello, Jorgelina R.; Bennett, Pamela M.; Himbeault, Kevin T.
- Environmental Science & Technology, Vol. 40, Issue 20
Effects of uranium mining discharges on water quality in the Puerco River basin, Arizona and New Mexico
journal, October 1992
- Van Metre, Peter C.; Gray, John R.
- Hydrological Sciences Journal, Vol. 37, Issue 5
Field evidence of selenium bioreduction in a uranium-contaminated aquifer: Field evidence of selenium bioreduction
journal, February 2013
- Williams, Kenneth H.; Wilkins, Michael J.; N'Guessan, A. Lucie
- Environmental Microbiology Reports, Vol. 5, Issue 3
Selenium in a Wyoming Grassland Community Receiving Wastewater from an In Situ Uranium Mine
journal, May 2002
- Ramirez, Jr., P.; Rogers, B. P.
- Archives of Environmental Contamination and Toxicology, Vol. 42, Issue 4
Isotopic and Geochemical Tracers for U(VI) Reduction and U Mobility at an in Situ Recovery U Mine
journal, May 2015
- Basu, Anirban; Brown, Shaun T.; Christensen, John N.
- Environmental Science & Technology, Vol. 49, Issue 10
Isotopic Evidence for Reductive Immobilization of Uranium Across a Roll-Front Mineral Deposit
journal, June 2016
- Brown, Shaun T.; Basu, Anirban; Christensen, John N.
- Environmental Science & Technology, Vol. 50, Issue 12
Mass-Dependent Fractionation of Selenium and Chromium Isotopes in Low-Temperature Environments
journal, January 2004
- Johnson, T. M.; Bullen, T. D.
- Reviews in Mineralogy and Geochemistry, Vol. 55, Issue 1
Selenium isotope fractionation during reduction by Fe(II)-Fe(III) hydroxide-sulfate (green rust)
journal, February 2003
- Johnson, Thomas M.; Bullen, Thomas D.
- Geochimica et Cosmochimica Acta, Vol. 67, Issue 3
Stable isotope fractionation of selenium by natural microbial consortia
journal, April 2003
- Ellis, Andre S.; Johnson, Thomas M.; Herbel, Mitchell J.
- Chemical Geology, Vol. 195, Issue 1-4
Fractionation of selenium isotopes during bacterial respiratory reduction of selenium oxyanions
journal, November 2000
- Herbel, Mitchell J.; Johnson, Thomas M.; Oremland, Ronald S.
- Geochimica et Cosmochimica Acta, Vol. 64, Issue 21
Selenium sorption and isotope fractionation: Iron(III) oxides versus iron(II) sulfides
journal, March 2013
- Mitchell, Kristen; Couture, Raoul-Marie; Johnson, Thomas M.
- Chemical Geology, Vol. 342
Selenium isotope ratios as indicators of selenium sources and oxyanion reduction
journal, September 1999
- Johnson, Thomas M.; Herbel, Mitchell J.; Bullen, Thomas D.
- Geochimica et Cosmochimica Acta, Vol. 63, Issue 18
A sequential extraction technique for mass-balanced stable selenium isotope analysis of soil samples
journal, August 2014
- Schilling, Kathrin; Johnson, Thomas M.; Mason, Paul R. D.
- Chemical Geology, Vol. 381
Fate of Selenium in Soils at a Seleniferous Site Recorded by High Precision Se Isotope Measurements
journal, August 2015
- Schilling, Kathrin; Johnson, Thomas M.; Dhillon, Karaj S.
- Environmental Science & Technology, Vol. 49, Issue 16
Effective Isotopic Fractionation Factors for Solute Removal by Reactive Sediments: A Laboratory Microcosm and Slurry Study
journal, October 2008
- Clark, Scott K.; Johnson, Thomas M.
- Environmental Science & Technology, Vol. 42, Issue 21
Scaling NIST SRM 3149 for Se isotope analysis and isotopic variations of natural samples
journal, August 2007
- Carignan, Jean; Wen, Hanjie
- Chemical Geology, Vol. 242, Issue 3-4
Estimating Precision Using Duplicate Measurements
journal, September 2009
- Hyslop, Nicole Pauly; White, Warren H.
- Journal of the Air & Waste Management Association, Vol. 59, Issue 9
Optimal methods for estimating kinetic isotope effects from different forms of the Rayleigh distillation equation
journal, February 2004
- Scott, K. M.; Lu, X.; Cavanaugh, C. M.
- Geochimica et Cosmochimica Acta, Vol. 68, Issue 3
Iron disulfide minerals and the genesis of roll-type uranium deposits
journal, February 1983
- Reynolds, Richard L.; Goldhaber, Martin B.
- Economic Geology, Vol. 78, Issue 1
Origin of a South Texas roll-type uranium deposit; I, Alteration of iron-titanium oxide minerals
journal, December 1978
- Reynolds, R. L.; Goldhaber, M. B.
- Economic Geology, Vol. 73, Issue 8
Low temperature equilibrium isotope fractionation and isotope exchange kinetics between U(IV) and U(VI)
journal, June 2015
- Wang, Xiangli; Johnson, Thomas M.; Lundstrom, Craig C.
- Geochimica et Cosmochimica Acta, Vol. 158
Groundwater contamination at the Kesterson Reservoir, California: 2. Geochemical parameters influencing selenium mobility
journal, June 1991
- White, Art F.; Benson, Sally M.; Yee, Andrew W.
- Water Resources Research, Vol. 27, Issue 6
Redox Processes and Water Quality of Selected Principal Aquifer Systems
journal, March 2008
- McMahon, P. B.; Chapelle, F. H.
- Ground Water, Vol. 46, Issue 2
Reduction of Uranium(VI) by Soluble Iron(II) Conforms with Thermodynamic Predictions
journal, June 2011
- Du, Xin; Boonchayaanant, Benjaporn; Wu, Wei-Min
- Environmental Science & Technology, Vol. 45, Issue 11
An experimental and ab initio study on the abiotic reduction of uranyl by ferrous iron
journal, May 2015
- Taylor, S. D.; Marcano, M. C.; Rosso, K. M.
- Geochimica et Cosmochimica Acta, Vol. 156
Influence of Magnetite Stoichiometry on U VI Reduction
journal, December 2011
- Latta, Drew E.; Gorski, Christopher A.; Boyanov, Maxim I.
- Environmental Science & Technology, Vol. 46, Issue 2
Uranium reduction on magnetite: Probing for pentavalent uranium using electrochemical methods
journal, May 2015
- Yuan, Ke; Renock, Devon; Ewing, Rodney C.
- Geochimica et Cosmochimica Acta, Vol. 156
Reaction of U VI with Titanium-Substituted Magnetite: Influence of Ti on U IV Speciation
journal, April 2013
- Latta, Drew E.; Pearce, Carolyn I.; Rosso, Kevin M.
- Environmental Science & Technology, Vol. 47, Issue 9
Abiotic Reductive Immobilization of U(VI) by Biogenic Mackinawite
journal, February 2013
- Veeramani, Harish; Scheinost, Andreas C.; Monsegue, Niven
- Environmental Science & Technology, Vol. 47, Issue 5
Simultaneous Reduction of Arsenic(V) and Uranium(VI) by Mackinawite: Role of Uranyl Arsenate Precipitate Formation
journal, November 2014
- Troyer, Lyndsay D.; Tang, Yuanzhi; Borch, Thomas
- Environmental Science & Technology, Vol. 48, Issue 24
Abiotic Selenium Redox Transformations in the Presence of Fe(II,III) Oxides
journal, November 1997
- Myneni, S. C.
- Science, Vol. 278, Issue 5340
Selenite Reduction by Mackinawite, Magnetite and Siderite: XAS Characterization of Nanosized Redox Products
journal, March 2008
- Scheinost, Andreas C.; Charlet, Laurent
- Environmental Science & Technology, Vol. 42, Issue 6
Electron transfer at the mineral/water interface: Selenium reduction by ferrous iron sorbed on clay
journal, December 2007
- Charlet, L.; Scheinost, A. C.; Tournassat, C.
- Geochimica et Cosmochimica Acta, Vol. 71, Issue 23
Sorption and reduction of selenite on chlorite surfaces in the presence of Fe(II) ions
journal, December 2013
- Baik, Min Hoon; Lee, Seung Yeop; Jeong, Jongtae
- Journal of Environmental Radioactivity, Vol. 126
Works referencing / citing this record:
Isolation of selenate from selenite, carbonate, phosphate, and arsenate solutions for δ 18 O-selenate determination
journal, March 2020
- Xia, Lichao; Schellenger, Alexandra E. P.; Onnis-Hayden, Annalisa
- Isotopes in Environmental and Health Studies, Vol. 56, Issue 3
Precise measurement of selenium isotopes by HG-MC-ICPMS using a 76–78 double-spike
journal, January 2020
- Pons, Marie-Laure; Millet, Marc-Alban; Nowell, Geoff N.
- Journal of Analytical Atomic Spectrometry, Vol. 35, Issue 2
Precise measurement of selenium isotopes by HG-MC-ICPMS using a 76-78 double-spike
journalarticle, January 2020
- Pons, Ml; Millet, Ma; Nowell, Gn
- Royal Society of Chemistry (RSC)
Isolation of selenate from selenite, carbonate, phosphate, and arsenate solutions for δ18O-selenate determination
text, January 2020
- Xia, Lichao; Schellenger, Alexandra E. P.; Onnis-Hayden, Annalisa
- Taylor & Francis