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Title: Hydrothermal transport, deposition, and fractionation of the REE: Experimental data and thermodynamic calculations

Abstract

For many years, our understanding of the behavior of the REE in hydrothermal systems was based on semi-empirical estimates involving extrapolation of thermodynamic data obtained at 25 °C. Since then, a substantial body of experimental data has accumulated on the stability of aqueous complexes of the REE. These data have shown that some of the predictions of Haas et al. (1995) are accurate, but others may be in error by several orders of magnitude. However, application of the data in modeling hydrothermal transport and deposition of the REE has been severely hampered by the lack of data on the thermodynamic properties of even the most common REE minerals. The discrepancies between the predictions and experimental determinations of the thermodynamic properties of aqueous REE species, together with the paucity of data on the stability of REE minerals, raise serious questions about the reliability of some models that have been proposed for the hydrothermal mobility of these critical metals. In this contribution, we review a body of high-temperature experimental data collected over the past 15 years on the stability of REE aqueous species and minerals. Using this new thermodynamic dataset, we re-evaluate the mechanisms responsible for hydrothermal transport and deposition of themore » REE. We also discuss the mechanisms that can result in REE fractionation during their hydrothermal transport and deposition. Here, our calculations suggest that in hydrothermal solutions, the main REE transporting ligands are chloride and sulfate, whereas fluoride, carbonate, and phosphate likely play an important role as depositional ligands. In addition to crystallographic fractionation, which is based on the differing affinity of mineral structures for the REE, our models suggest that the REE can be fractionated hydrothermally due to the differences in the stability of the LREE and HREE as aqueous chloride complexes.« less

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [1]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
  2. McGill Univ., Montreal, QC (Canada)
  3. Monash Univ., Melbourne, VIC (Australia)
Publication Date:
Research Org.:
Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
Natural Sciences and Engineering Research Council of Canada (NSERC); USDOE
OSTI Identifier:
1351190
Report Number(s):
LA-UR-16-21989
Journal ID: ISSN 0009-2541
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Chemical Geology
Additional Journal Information:
Journal Volume: 439; Journal Issue: C; Journal ID: ISSN 0009-2541
Publisher:
Elsevier
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; earth sciences; hydrothermal; REE; transport; deposition; fractionation; rare earth elements

Citation Formats

Migdisov, Artaches, Williams-Jones, A. E., Brugger, J., and Caporuscio, Florie Andre. Hydrothermal transport, deposition, and fractionation of the REE: Experimental data and thermodynamic calculations. United States: N. p., 2016. Web. doi:10.1016/j.chemgeo.2016.06.005.
Migdisov, Artaches, Williams-Jones, A. E., Brugger, J., & Caporuscio, Florie Andre. Hydrothermal transport, deposition, and fractionation of the REE: Experimental data and thermodynamic calculations. United States. doi:10.1016/j.chemgeo.2016.06.005.
Migdisov, Artaches, Williams-Jones, A. E., Brugger, J., and Caporuscio, Florie Andre. Sat . "Hydrothermal transport, deposition, and fractionation of the REE: Experimental data and thermodynamic calculations". United States. doi:10.1016/j.chemgeo.2016.06.005. https://www.osti.gov/servlets/purl/1351190.
@article{osti_1351190,
title = {Hydrothermal transport, deposition, and fractionation of the REE: Experimental data and thermodynamic calculations},
author = {Migdisov, Artaches and Williams-Jones, A. E. and Brugger, J. and Caporuscio, Florie Andre},
abstractNote = {For many years, our understanding of the behavior of the REE in hydrothermal systems was based on semi-empirical estimates involving extrapolation of thermodynamic data obtained at 25 °C. Since then, a substantial body of experimental data has accumulated on the stability of aqueous complexes of the REE. These data have shown that some of the predictions of Haas et al. (1995) are accurate, but others may be in error by several orders of magnitude. However, application of the data in modeling hydrothermal transport and deposition of the REE has been severely hampered by the lack of data on the thermodynamic properties of even the most common REE minerals. The discrepancies between the predictions and experimental determinations of the thermodynamic properties of aqueous REE species, together with the paucity of data on the stability of REE minerals, raise serious questions about the reliability of some models that have been proposed for the hydrothermal mobility of these critical metals. In this contribution, we review a body of high-temperature experimental data collected over the past 15 years on the stability of REE aqueous species and minerals. Using this new thermodynamic dataset, we re-evaluate the mechanisms responsible for hydrothermal transport and deposition of the REE. We also discuss the mechanisms that can result in REE fractionation during their hydrothermal transport and deposition. Here, our calculations suggest that in hydrothermal solutions, the main REE transporting ligands are chloride and sulfate, whereas fluoride, carbonate, and phosphate likely play an important role as depositional ligands. In addition to crystallographic fractionation, which is based on the differing affinity of mineral structures for the REE, our models suggest that the REE can be fractionated hydrothermally due to the differences in the stability of the LREE and HREE as aqueous chloride complexes.},
doi = {10.1016/j.chemgeo.2016.06.005},
journal = {Chemical Geology},
number = C,
volume = 439,
place = {United States},
year = {Sat Jun 11 00:00:00 EDT 2016},
month = {Sat Jun 11 00:00:00 EDT 2016}
}

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