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Title: 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, U 6+ state, whereas in its reduced, U 4+ 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 (UCl 4°) 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:
 [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]
  1. McGill Univ., Montreal, QC (Canada)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Los Alamos National Lab. (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. doi: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. doi: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 = {2018},
month = {4}
}

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Cited by: 11 works
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