Challenging the thorium-immobility paradigm
Abstract
Thorium is the most abundant actinide in the Earth’s crust and has universally been considered one of the most immobile elements in natural aqueous systems. This view, however, is based almost exclusively on solubility data obtained at low temperature and their theoretical extrapolation to elevated temperature. The occurrence of hydrothermal deposits with high concentrations of Th challenges the Th immobility paradigm and strongly suggests that Th may be mobilized by some aqueous fluids. Here, we demonstrate experimentally that Th, indeed, is highly mobile at temperatures between 175 and 250°C in sulfate-bearing aqueous fluids due to the formation of the highly stable Th(SO4)2 aqueous complex. The results of this study indicate that current models grossly underestimate the mobility of Th in hydrothermal fluids, and thus the behavior of Th in ore-forming systems and the nuclear fuel cycle needs to be re-evaluated.
- Authors:
-
[1];
[2];
[2];
[2]
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); McGill Univ., Montreal, QC (Canada)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- McGill Univ., Montreal, QC (Canada)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA)
- OSTI Identifier:
- 1597339
- Report Number(s):
- LA-UR-19-20286
Journal ID: ISSN 2045-2322
- Grant/Contract Number:
- 89233218CNA000001; 20180007DR; 20180475DR
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 58 GEOSCIENCES; thorium; solubility; sulfate; hydrothermal; economic geology; geochemistry
Citation Formats
Nisbet, Haylea Dawn, Migdissov, Artaches A., Williams-Jones, Anthony E., Xu, Hongwu, van Hinsberg, Vincent J., and Roback, Robert Clifford. Challenging the thorium-immobility paradigm. United States: N. p., 2019.
Web. doi:10.1038/s41598-019-53571-x.
Nisbet, Haylea Dawn, Migdissov, Artaches A., Williams-Jones, Anthony E., Xu, Hongwu, van Hinsberg, Vincent J., & Roback, Robert Clifford. Challenging the thorium-immobility paradigm. United States. https://doi.org/10.1038/s41598-019-53571-x
Nisbet, Haylea Dawn, Migdissov, Artaches A., Williams-Jones, Anthony E., Xu, Hongwu, van Hinsberg, Vincent J., and Roback, Robert Clifford. Tue .
"Challenging the thorium-immobility paradigm". United States. https://doi.org/10.1038/s41598-019-53571-x. https://www.osti.gov/servlets/purl/1597339.
@article{osti_1597339,
title = {Challenging the thorium-immobility paradigm},
author = {Nisbet, Haylea Dawn and Migdissov, Artaches A. and Williams-Jones, Anthony E. and Xu, Hongwu and van Hinsberg, Vincent J. and Roback, Robert Clifford},
abstractNote = {Thorium is the most abundant actinide in the Earth’s crust and has universally been considered one of the most immobile elements in natural aqueous systems. This view, however, is based almost exclusively on solubility data obtained at low temperature and their theoretical extrapolation to elevated temperature. The occurrence of hydrothermal deposits with high concentrations of Th challenges the Th immobility paradigm and strongly suggests that Th may be mobilized by some aqueous fluids. Here, we demonstrate experimentally that Th, indeed, is highly mobile at temperatures between 175 and 250°C in sulfate-bearing aqueous fluids due to the formation of the highly stable Th(SO4)2 aqueous complex. The results of this study indicate that current models grossly underestimate the mobility of Th in hydrothermal fluids, and thus the behavior of Th in ore-forming systems and the nuclear fuel cycle needs to be re-evaluated.},
doi = {10.1038/s41598-019-53571-x},
journal = {Scientific Reports},
number = 1,
volume = 9,
place = {United States},
year = {Tue Nov 19 00:00:00 EST 2019},
month = {Tue Nov 19 00:00:00 EST 2019}
}
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