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Title: Activity model for 36 elements in Fe-Ni-Si-S-C liquids with application to terrestrial planet accretion and mantle geochemistry: New data for Ru, Re, Pt, Os, Ti, Nb, and Ta

Abstract

Understanding siderophile element partitioning between metal and silicate melts under diverse conditions can be used to place important constraints on the materials and conditions of planetary accretion and core formation, as well as post core formation processes. However, the effects of Si on the partitioning and activity coefficients for these elements are not well known, despite Si likely being one of the dominant light elements in Earth’s core. To address this gap in understanding, we have undertaken a systematic study of the highly siderophile elements Re, Pt, Os, and Ru, and the refractory lithophile elements Nb, Ta and Ti at 1600 °C and 1 GPa, to derive epsilon interaction parameters for these elements in FeSi metallic liquids. Positive epsilon interaction parameters were measured for Nb, Ta, Ti, Ru, Re, Pt, and Os, indicating that dissolved Si in Fe liquids causes a decrease in their metal/silicate partition coefficients (or ‘silicophobic’ behavior). Furthermore, ε$$_{Re, Os, or Ru}^{Si}$$ > ε$$_{Re, Os, or Ru}^{S}$$ which means Si causes a larger decrease in D(metal/silicate) than S, and the chalcophile behavior expected from some elements will be completely masked by the presence of Si in a metallic liquid. The new parameters are used to update an activity model that now includes 36 siderophile elements in Fe-Ni-Si-S-C liquids (27 trace elements considered here). Systematic assessment of these 27 elements shows which have the strongest affinity for Si, C, and S, and also how activity coefficients for these elements would vary during accretion and core formation in Earth, Mars, and Mercury of widely differing fO2 and core compositional conditions. The activity model is combined with new partitioning expressions for Mo, W, Cr, Re Ru, Pt, and Os and applied to aspects of post core formation mantle geochemistry of Earth, Mars, and Mercury. Our updated expressions show that the BSE Mo/W ratio can easily be achieved with metal/silicate partitioning during growth of the Earth, whereas Re, Os and Ru become lower than and highly fractionated compared with BSE values during core formation and accretion, and thus nearly 99% of their BSE abundances are likely contributed by late accretion. Ru isotopes should be a very good indicator of the source material for the late accretion. The high Pt/Os and Re/Os developed in a deepening magma ocean during the growth of the Earth, indicates 186Os and 187Os isotopes could be coupled if this ancient material remained isolated and subsequently became entrained in mantle plumes and measured in surficial lavas. The extent to which this occurred will be limited by the low Os content of this ancient material, thus requiring mixing as a major component in plume sources. Martian mantle Hf/W ratio stays low during accretion and core formation modelling, suggesting that W isotope anomalies are more likely due to solid/liquid silicate fractionation than to core formation. Finally, Ti contents measured by MESSENGER at Mercury’s surface can be explained by segregation of either a metallic core (IW-6 to -8) or metallic core + sulfide (IW-4 to -7.5) followed by mantle melting.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [4];  [1]
+ Show Author Affiliations
  1. NASA Johnson Space Center, Houston, TX (United States)
  2. Western Washington University, Bellingham, WA (United States)
  3. Florida State Univ., Tallahassee, FL (United States)
  4. Los Alamos National Laboratory (LANL), Los Alamos, NM (United States); NASA Johnson Space Center, Houston, TX (United States)
Publication Date:
Research Org.:
Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE; National Aeronautics and Space Administration (NASA); National Science Foundation (NSF)
OSTI Identifier:
1987401
Report Number(s):
LA-UR-23-25094
Journal ID: ISSN 0016-7037; TRN: US2402773
Grant/Contract Number:  
89233218CNA000001; DMR-1644779
Resource Type:
Accepted Manuscript
Journal Name:
Geochimica et Cosmochimica Acta
Additional Journal Information:
Journal Volume: 354; Journal ID: ISSN 0016-7037
Publisher:
Elsevier; The Geochemical Society; The Meteoritical Society
Country of Publication:
United States
Language:
English
Subject:
38 RADIATION CHEMISTRY, RADIOCHEMISTRY, AND NUCLEAR CHEMISTRY; siderophile elements; core formation; metallic liquid; trace element

Citation Formats

Righter, Kevin, Boujibar, Asmaa, Humayun, Munir, Yang, Shuying, Rowland, II, Richard Lee, and Pando, Kellye. Activity model for 36 elements in Fe-Ni-Si-S-C liquids with application to terrestrial planet accretion and mantle geochemistry: New data for Ru, Re, Pt, Os, Ti, Nb, and Ta. United States: N. p., 2023. Web. doi:10.1016/j.gca.2023.06.014.
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Righter, Kevin, Boujibar, Asmaa, Humayun, Munir, Yang, Shuying, Rowland, II, Richard Lee, & Pando, Kellye. Activity model for 36 elements in Fe-Ni-Si-S-C liquids with application to terrestrial planet accretion and mantle geochemistry: New data for Ru, Re, Pt, Os, Ti, Nb, and Ta. United States. https://doi.org/10.1016/j.gca.2023.06.014
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Righter, Kevin, Boujibar, Asmaa, Humayun, Munir, Yang, Shuying, Rowland, II, Richard Lee, and Pando, Kellye. Fri . "Activity model for 36 elements in Fe-Ni-Si-S-C liquids with application to terrestrial planet accretion and mantle geochemistry: New data for Ru, Re, Pt, Os, Ti, Nb, and Ta". United States. https://doi.org/10.1016/j.gca.2023.06.014.
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@article{osti_1987401,
title = {Activity model for 36 elements in Fe-Ni-Si-S-C liquids with application to terrestrial planet accretion and mantle geochemistry: New data for Ru, Re, Pt, Os, Ti, Nb, and Ta},
author = {Righter, Kevin and Boujibar, Asmaa and Humayun, Munir and Yang, Shuying and Rowland, II, Richard Lee and Pando, Kellye},
abstractNote = {Understanding siderophile element partitioning between metal and silicate melts under diverse conditions can be used to place important constraints on the materials and conditions of planetary accretion and core formation, as well as post core formation processes. However, the effects of Si on the partitioning and activity coefficients for these elements are not well known, despite Si likely being one of the dominant light elements in Earth’s core. To address this gap in understanding, we have undertaken a systematic study of the highly siderophile elements Re, Pt, Os, and Ru, and the refractory lithophile elements Nb, Ta and Ti at 1600 °C and 1 GPa, to derive epsilon interaction parameters for these elements in FeSi metallic liquids. Positive epsilon interaction parameters were measured for Nb, Ta, Ti, Ru, Re, Pt, and Os, indicating that dissolved Si in Fe liquids causes a decrease in their metal/silicate partition coefficients (or ‘silicophobic’ behavior). Furthermore, ε$_{Re, Os, or Ru}^{Si}$ > ε$_{Re, Os, or Ru}^{S}$ which means Si causes a larger decrease in D(metal/silicate) than S, and the chalcophile behavior expected from some elements will be completely masked by the presence of Si in a metallic liquid. The new parameters are used to update an activity model that now includes 36 siderophile elements in Fe-Ni-Si-S-C liquids (27 trace elements considered here). Systematic assessment of these 27 elements shows which have the strongest affinity for Si, C, and S, and also how activity coefficients for these elements would vary during accretion and core formation in Earth, Mars, and Mercury of widely differing fO2 and core compositional conditions. The activity model is combined with new partitioning expressions for Mo, W, Cr, Re Ru, Pt, and Os and applied to aspects of post core formation mantle geochemistry of Earth, Mars, and Mercury. Our updated expressions show that the BSE Mo/W ratio can easily be achieved with metal/silicate partitioning during growth of the Earth, whereas Re, Os and Ru become lower than and highly fractionated compared with BSE values during core formation and accretion, and thus nearly 99% of their BSE abundances are likely contributed by late accretion. Ru isotopes should be a very good indicator of the source material for the late accretion. The high Pt/Os and Re/Os developed in a deepening magma ocean during the growth of the Earth, indicates 186Os and 187Os isotopes could be coupled if this ancient material remained isolated and subsequently became entrained in mantle plumes and measured in surficial lavas. The extent to which this occurred will be limited by the low Os content of this ancient material, thus requiring mixing as a major component in plume sources. Martian mantle Hf/W ratio stays low during accretion and core formation modelling, suggesting that W isotope anomalies are more likely due to solid/liquid silicate fractionation than to core formation. Finally, Ti contents measured by MESSENGER at Mercury’s surface can be explained by segregation of either a metallic core (IW-6 to -8) or metallic core + sulfide (IW-4 to -7.5) followed by mantle melting.},
doi = {10.1016/j.gca.2023.06.014},
journal = {Geochimica et Cosmochimica Acta},
number = ,
volume = 354,
place = {United States},
year = {Fri Jun 16 00:00:00 EDT 2023},
month = {Fri Jun 16 00:00:00 EDT 2023}
}
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  • Lee, Der-Chuen; Halliday, Alex N.
  • Nature, Vol. 388, Issue 6645
  • DOI: 10.1038/42206

Constraints on core formation from Pt partitioning in mafic silicate liquids at high temperatures
journal, March 2006

Light elements in the Earth’s core
journal, August 2021

  • Hirose, Kei; Wood, Bernard; Vočadlo, Lidunka
  • Nature Reviews Earth & Environment, Vol. 2, Issue 9
  • DOI: 10.1038/s43017-021-00203-6

Thermometry of the magma ocean: Controls on the metal–silicate partitioning of gold
journal, July 2016

Ruthenium isotope fractionation in protoplanetary cores
journal, February 2018

  • Hopp, Timo; Fischer-Gödde, Mario; Kleine, Thorsten
  • Geochimica et Cosmochimica Acta, Vol. 223
  • DOI: 10.1016/j.gca.2017.11.033

The influence of FeO on the solubilities of cobalt and nickel in silicate melts
journal, April 1996

The effect of fO on the diffusion of redox-sensitive elements in haplobasaltic melt at 1 GPa and 1300 °C
journal, May 2019

The initial abundance and distribution of 92 Nb in the Solar System
journal, April 2016

Modeling fractional crystallization of group IVB iron meteorites
journal, April 2008

  • Walker, Richard J.; McDonough, William F.; Honesto, Jenise
  • Geochimica et Cosmochimica Acta, Vol. 72, Issue 8
  • DOI: 10.1016/j.gca.2008.01.021
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