Persistence of Uranium in Old and Cold Subpermafrost Groundwater Indicated by Linking 234 U- 235 U- 238 U, Groundwater Ages, and Hydrogeochemistry
Uranium (U) contamination in groundwater from geogenic sources affects water quality globally. Here, we use a multifaceted isotopic and geochemical approach to elucidate U sources and controls on geogenic U release to groundwater and surface water at a prospective subarctic gold deposit in Yukon, Ca...
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ftsmithonian:oai:figshare.com:article/17108660 2023-05-15T17:57:29+02:00 Persistence of Uranium in Old and Cold Subpermafrost Groundwater Indicated by Linking 234 U- 235 U- 238 U, Groundwater Ages, and Hydrogeochemistry Elliott K. Skierszkan (6681497) John W. Dockrey (6681506) Jordi Helsen (11778998) Laura-Lee Findlater (11779001) Clément P. Bataille (11779004) Ghislain de Laplante (11779007) Joyce M. McBeth (2328241) K. Ulrich Mayer (2237767) Roger D. Beckie (6681512) 2021-12-01T00:00:00Z https://doi.org/10.1021/acsearthspacechem.1c00307.s001 unknown https://figshare.com/articles/journal_contribution/Persistence_of_Uranium_in_Old_and_Cold_Subpermafrost_Groundwater_Indicated_by_Linking_sup_234_sup_U-_sup_235_sup_U-_sup_238_sup_U_Groundwater_Ages_and_Hydrogeochemistry/17108660 doi:10.1021/acsearthspacechem.1c00307.s001 CC BY-NC 4.0 CC-BY-NC Biophysics Biochemistry Genetics Ecology Space Science Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified study provides insight sorption – desorption ray absorption spectroscopy mineralized structures around median 38 μg hydrogeochemical changes may 3 </ sup 238 </ sup 235 </ sup 234 </ sup 14 </ sup fe ( iii u isotope fractionation phase u present geogenic u release elucidate u sources u /< sup u -< sup rich groundwater produced cold groundwater conditions groundwater u concentrations groundwater ages inferred u ( vi ( vi groundwater ages u transport u mobilization subarctic groundwater groundwater indicates time scales surface water sequential extractions range 1 pivotal time oxidative weathering multifaceted isotopic mobile form main driver geochemical approach fractured bedrock Text Journal contribution 2021 ftsmithonian https://doi.org/10.1021/acsearthspacechem.1c00307.s001 2021-12-19T20:24:46Z Uranium (U) contamination in groundwater from geogenic sources affects water quality globally. Here, we use a multifaceted isotopic and geochemical approach to elucidate U sources and controls on geogenic U release to groundwater and surface water at a prospective subarctic gold deposit in Yukon, Canada, that is characterized by permafrost, fractured bedrock, and cold (<2 °C) groundwater. X-ray absorption spectroscopy, sequential extractions, and micro X-ray fluorescence mapping show extensive subsurface oxidation and solid-phase U present in its hexavalent and mobile form. Limited 238 U/ 235 U isotope fractionation and predominance of U(VI) in rocks suggest U(VI) sorption–desorption is the main driver of U mobilization. Groundwater U concentrations are appreciable (median 38 μg/L, range 1.2–535 μg/L) and are explained by high-alkalinity, Ca-rich groundwater produced from oxidative weathering of sulfide and carbonate-mineralized structures around the deposit. Minor 238 U/ 235 U isotope fractionation in groundwater indicates that limited U(VI) reduction occurs beneath permafrost despite groundwater redox conditions below Fe(III) and S(VI) reduction, and groundwater ages inferred from 3 H and 14 C to be on the order of thousands of years. The complexation of U as uranyl–calcium–carbonate complexes and the resilience of these complexes to U(VI) reduction contributes to high U(VI) mobility under cold groundwater conditions. This study provides insight into processes and time scales of U transport in subarctic groundwater at a pivotal time when hydrogeochemical changes may be anticipated in cold regions worldwide due to permafrost degradation. Other Non-Article Part of Journal/Newspaper permafrost Subarctic Yukon Unknown Yukon Canada |
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Open Polar |
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Unknown |
op_collection_id |
ftsmithonian |
language |
unknown |
topic |
Biophysics Biochemistry Genetics Ecology Space Science Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified study provides insight sorption – desorption ray absorption spectroscopy mineralized structures around median 38 μg hydrogeochemical changes may 3 </ sup 238 </ sup 235 </ sup 234 </ sup 14 </ sup fe ( iii u isotope fractionation phase u present geogenic u release elucidate u sources u /< sup u -< sup rich groundwater produced cold groundwater conditions groundwater u concentrations groundwater ages inferred u ( vi ( vi groundwater ages u transport u mobilization subarctic groundwater groundwater indicates time scales surface water sequential extractions range 1 pivotal time oxidative weathering multifaceted isotopic mobile form main driver geochemical approach fractured bedrock |
spellingShingle |
Biophysics Biochemistry Genetics Ecology Space Science Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified study provides insight sorption – desorption ray absorption spectroscopy mineralized structures around median 38 μg hydrogeochemical changes may 3 </ sup 238 </ sup 235 </ sup 234 </ sup 14 </ sup fe ( iii u isotope fractionation phase u present geogenic u release elucidate u sources u /< sup u -< sup rich groundwater produced cold groundwater conditions groundwater u concentrations groundwater ages inferred u ( vi ( vi groundwater ages u transport u mobilization subarctic groundwater groundwater indicates time scales surface water sequential extractions range 1 pivotal time oxidative weathering multifaceted isotopic mobile form main driver geochemical approach fractured bedrock Elliott K. Skierszkan (6681497) John W. Dockrey (6681506) Jordi Helsen (11778998) Laura-Lee Findlater (11779001) Clément P. Bataille (11779004) Ghislain de Laplante (11779007) Joyce M. McBeth (2328241) K. Ulrich Mayer (2237767) Roger D. Beckie (6681512) Persistence of Uranium in Old and Cold Subpermafrost Groundwater Indicated by Linking 234 U- 235 U- 238 U, Groundwater Ages, and Hydrogeochemistry |
topic_facet |
Biophysics Biochemistry Genetics Ecology Space Science Environmental Sciences not elsewhere classified Chemical Sciences not elsewhere classified study provides insight sorption – desorption ray absorption spectroscopy mineralized structures around median 38 μg hydrogeochemical changes may 3 </ sup 238 </ sup 235 </ sup 234 </ sup 14 </ sup fe ( iii u isotope fractionation phase u present geogenic u release elucidate u sources u /< sup u -< sup rich groundwater produced cold groundwater conditions groundwater u concentrations groundwater ages inferred u ( vi ( vi groundwater ages u transport u mobilization subarctic groundwater groundwater indicates time scales surface water sequential extractions range 1 pivotal time oxidative weathering multifaceted isotopic mobile form main driver geochemical approach fractured bedrock |
description |
Uranium (U) contamination in groundwater from geogenic sources affects water quality globally. Here, we use a multifaceted isotopic and geochemical approach to elucidate U sources and controls on geogenic U release to groundwater and surface water at a prospective subarctic gold deposit in Yukon, Canada, that is characterized by permafrost, fractured bedrock, and cold (<2 °C) groundwater. X-ray absorption spectroscopy, sequential extractions, and micro X-ray fluorescence mapping show extensive subsurface oxidation and solid-phase U present in its hexavalent and mobile form. Limited 238 U/ 235 U isotope fractionation and predominance of U(VI) in rocks suggest U(VI) sorption–desorption is the main driver of U mobilization. Groundwater U concentrations are appreciable (median 38 μg/L, range 1.2–535 μg/L) and are explained by high-alkalinity, Ca-rich groundwater produced from oxidative weathering of sulfide and carbonate-mineralized structures around the deposit. Minor 238 U/ 235 U isotope fractionation in groundwater indicates that limited U(VI) reduction occurs beneath permafrost despite groundwater redox conditions below Fe(III) and S(VI) reduction, and groundwater ages inferred from 3 H and 14 C to be on the order of thousands of years. The complexation of U as uranyl–calcium–carbonate complexes and the resilience of these complexes to U(VI) reduction contributes to high U(VI) mobility under cold groundwater conditions. This study provides insight into processes and time scales of U transport in subarctic groundwater at a pivotal time when hydrogeochemical changes may be anticipated in cold regions worldwide due to permafrost degradation. |
format |
Other Non-Article Part of Journal/Newspaper |
author |
Elliott K. Skierszkan (6681497) John W. Dockrey (6681506) Jordi Helsen (11778998) Laura-Lee Findlater (11779001) Clément P. Bataille (11779004) Ghislain de Laplante (11779007) Joyce M. McBeth (2328241) K. Ulrich Mayer (2237767) Roger D. Beckie (6681512) |
author_facet |
Elliott K. Skierszkan (6681497) John W. Dockrey (6681506) Jordi Helsen (11778998) Laura-Lee Findlater (11779001) Clément P. Bataille (11779004) Ghislain de Laplante (11779007) Joyce M. McBeth (2328241) K. Ulrich Mayer (2237767) Roger D. Beckie (6681512) |
author_sort |
Elliott K. Skierszkan (6681497) |
title |
Persistence of Uranium in Old and Cold Subpermafrost Groundwater Indicated by Linking 234 U- 235 U- 238 U, Groundwater Ages, and Hydrogeochemistry |
title_short |
Persistence of Uranium in Old and Cold Subpermafrost Groundwater Indicated by Linking 234 U- 235 U- 238 U, Groundwater Ages, and Hydrogeochemistry |
title_full |
Persistence of Uranium in Old and Cold Subpermafrost Groundwater Indicated by Linking 234 U- 235 U- 238 U, Groundwater Ages, and Hydrogeochemistry |
title_fullStr |
Persistence of Uranium in Old and Cold Subpermafrost Groundwater Indicated by Linking 234 U- 235 U- 238 U, Groundwater Ages, and Hydrogeochemistry |
title_full_unstemmed |
Persistence of Uranium in Old and Cold Subpermafrost Groundwater Indicated by Linking 234 U- 235 U- 238 U, Groundwater Ages, and Hydrogeochemistry |
title_sort |
persistence of uranium in old and cold subpermafrost groundwater indicated by linking 234 u- 235 u- 238 u, groundwater ages, and hydrogeochemistry |
publishDate |
2021 |
url |
https://doi.org/10.1021/acsearthspacechem.1c00307.s001 |
geographic |
Yukon Canada |
geographic_facet |
Yukon Canada |
genre |
permafrost Subarctic Yukon |
genre_facet |
permafrost Subarctic Yukon |
op_relation |
https://figshare.com/articles/journal_contribution/Persistence_of_Uranium_in_Old_and_Cold_Subpermafrost_Groundwater_Indicated_by_Linking_sup_234_sup_U-_sup_235_sup_U-_sup_238_sup_U_Groundwater_Ages_and_Hydrogeochemistry/17108660 doi:10.1021/acsearthspacechem.1c00307.s001 |
op_rights |
CC BY-NC 4.0 |
op_rightsnorm |
CC-BY-NC |
op_doi |
https://doi.org/10.1021/acsearthspacechem.1c00307.s001 |
_version_ |
1766165922354036736 |