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Title: 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(SO 4) 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:
ORCiD logo [1]; ORCiD logo [2];  [3]; ORCiD logo [2];  [3]; ORCiD logo [2]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); McGill Univ., Montreal, QC (Canada)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  3. McGill Univ., Montreal, QC (Canada)
Publication Date:
Research Org.:
Los Alamos National Lab. (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. doi: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. doi: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 = {2019},
month = {11}
}

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