Uranium transport in acidic brines under reducing conditions
Abstract
The behavior of uranium in environments, ranging from those of natural systems responsible for the formation of uranium deposits to those of nuclear reactors providing 11% of the world’s electricity, is governed by processes involving high-temperature aqueous solutions. It has been well documented that uranium is mobile in aqueous solutions in its oxidized, U6+ state, whereas in its reduced, U4+ state, uranium has been assumed to be immobile. Here, we present experimental evidence from high temperature (>100 °C) acidic brines that invalidates this assumption. Our experiments have identified a new uranium chloride species (UCl4°) that is more stable under reducing than oxidized conditions. Furthermore, these results indicate that uranium is mobile under reducing conditions and necessitate a re-evaluation of the mobility of uranium, particularly in ore deposit models involving this metal. Regardless of the scenario considered, reducing conditions can no longer be considered a guarantee of uranium immobility.
- Authors:
-
[2];
[1];
[2];
[2];
[2]
- McGill Univ., Montreal, QC (Canada)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Nuclear Energy (NE)
- OSTI Identifier:
- 1484636
- Report Number(s):
- LA-UR-17-29029
Journal ID: ISSN 2041-1723
- Grant/Contract Number:
- 89233218CNA000001
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; uranium; hydrothermal; redox; mobility
Citation Formats
Timofeev, Alexander, Migdisov, Artaches A., Williams-Jones, Anthony E., Roback, Robert, Nelson, Andrew Thomas, and Xu, Hongwu. Uranium transport in acidic brines under reducing conditions. United States: N. p., 2018.
Web. doi:10.1038/s41467-018-03564-7.
Timofeev, Alexander, Migdisov, Artaches A., Williams-Jones, Anthony E., Roback, Robert, Nelson, Andrew Thomas, & Xu, Hongwu. Uranium transport in acidic brines under reducing conditions. United States. https://doi.org/10.1038/s41467-018-03564-7
Timofeev, Alexander, Migdisov, Artaches A., Williams-Jones, Anthony E., Roback, Robert, Nelson, Andrew Thomas, and Xu, Hongwu. Mon .
"Uranium transport in acidic brines under reducing conditions". United States. https://doi.org/10.1038/s41467-018-03564-7. https://www.osti.gov/servlets/purl/1484636.
@article{osti_1484636,
title = {Uranium transport in acidic brines under reducing conditions},
author = {Timofeev, Alexander and Migdisov, Artaches A. and Williams-Jones, Anthony E. and Roback, Robert and Nelson, Andrew Thomas and Xu, Hongwu},
abstractNote = {The behavior of uranium in environments, ranging from those of natural systems responsible for the formation of uranium deposits to those of nuclear reactors providing 11% of the world’s electricity, is governed by processes involving high-temperature aqueous solutions. It has been well documented that uranium is mobile in aqueous solutions in its oxidized, U6+ state, whereas in its reduced, U4+ state, uranium has been assumed to be immobile. Here, we present experimental evidence from high temperature (>100 °C) acidic brines that invalidates this assumption. Our experiments have identified a new uranium chloride species (UCl4°) that is more stable under reducing than oxidized conditions. Furthermore, these results indicate that uranium is mobile under reducing conditions and necessitate a re-evaluation of the mobility of uranium, particularly in ore deposit models involving this metal. Regardless of the scenario considered, reducing conditions can no longer be considered a guarantee of uranium immobility.},
doi = {10.1038/s41467-018-03564-7},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {Mon Apr 16 00:00:00 EDT 2018},
month = {Mon Apr 16 00:00:00 EDT 2018}
}
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Synchrotron XRF and XANES investigation of uranium speciation and element distribution in fluid inclusions from unconformity-related uranium deposits
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An internally consistent thermodynamic data set for phases of petrological interest: AN INTERNALLY CONSISTENT THERMODYNAMIC DATA SET
journal, May 1998
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Nuclear Fuel in a Reactor Accident
journal, March 2012
- Burns, Peter C.; Ewing, Rodney C.; Navrotsky, Alexandra
- Science, Vol. 335, Issue 6073
Magmatic and Metamorphic Uraninite Mineralization in the Western Margin of the Trans-Hudson Orogen (Saskatchewan, Canada): A Uranium Source for Unconformity-Related Uranium Deposits?
journal, June 2013
- Mercadier, J.; Annesley, I. R.; McKechnie, C. L.
- Economic Geology, Vol. 108, Issue 5
On the genesis of Rabbit Lake and other unconformity-type uranium deposits in northern Saskatchewan, Canada
journal, December 1978
- Hoeve, J.; Sibbald, T. I. I.
- Economic Geology, Vol. 73, Issue 8
The Lightning Creek Sill Complex, Cloncurry District,
Northwest Queensland: A Source of Fluids for Fe Oxide Cu-Au Mineralization
and Sodic-Calcic Alteration
journal, August 2000
- Perring, C. S.; Pollard, P. J.; Dong, G.
- Economic Geology, Vol. 95, Issue 5
Geological Disposal of Radioactive Waste in Clay
journal, July 2016
- Grambow, Bernd
- Elements, Vol. 12, Issue 4
Crystalline Rock as a Repository for Swedish Spent Nuclear Fuel
journal, July 2016
- Hedin, Allan; Olsson, Olle
- Elements, Vol. 12, Issue 4
Salt as a Host Rock for the Geological Repository for Nuclear Waste
journal, July 2016
- von Berlepsch, Thilo; Haverkamp, Bernt
- Elements, Vol. 12, Issue 4
Geological Disposal of Nuclear Waste in Tuff: Yucca Mountain (USA)
journal, July 2016
- Swift, Peter N.; Bonano, Evaristo J.
- Elements, Vol. 12, Issue 4
Interactions between Nuclear Fuel and Water at the Fukushima Daiichi Reactors
journal, June 2012
- Grambow, B.; Poinssot, C.
- Elements, Vol. 8, Issue 3
Theoretical prediction of the thermodynamic behavior of aqueous electrolytes by high pressures and temperatures; IV, Calculation of activity coefficients, osmotic coefficients, and apparent molal and standard and relative partial molal properties to 600 degrees C and 5kb
journal, December 1981
- Helgeson, H. C.; Kirkham, D. H.; Flowers, G. C.
- American Journal of Science, Vol. 281, Issue 10
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Cretaceous–Neogene basin control on the formation of uranium deposits in South China: evidence from geology, mineralization ages, and H–O isotopes
text, January 2019
- Zhang, Chuang; Cai, Yu-Qi; Dong, Qian
- Taylor & Francis