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Title: Stability of iron-bearing carbonates in the deep Earth’s interior

Abstract

The presence of carbonates in inclusions in diamonds coming from depths exceeding 670 km are obvious evidence that carbonates exist in the Earth’s lower mantle. However, their range of stability, crystal structures and the thermodynamic conditions of the decarbonation processes remain poorly constrained. We investigate the behaviour of pure iron carbonate at pressures over 100 GPa and temperatures over 2,500 K using single-crystal X-ray diffraction and Mossbauer spectroscopy in laser-heated diamond anvil cells. On heating to temperatures of the Earth’s geotherm at pressures to B 50 GPa FeCO 3 partially dissociates to form various iron oxides. Furthermore, at higher pressures FeCO 3 forms two new structures— tetrairon(III) orthocarbonate Fe$$3+\atop{4}$$C 3O 12 and diiron(II) diiron(III) tetracarbonate Fe$$2+\atop{2}$$ Fe$$3+\atop{2}$$C 4 O 13, both phases containing CO 4 tetrahedra. Fe 4 C 4 O 13 is stable at conditions along the entire geotherm to depths of at least 2,500 km, thus demonstrating that self-oxidation-reduction reactions can preserve carbonates in the Earth’s lower mantle.

Authors:
 [1];  [2];  [3];  [4];  [5]; ORCiD logo [6];  [7];  [3];  [6];  [3];  [3];  [3];  [3];  [3];  [8];  [3];  [9];  [6]
  1. European Synchrotron Radiation Facility (ESRF), Grenoble (France); Univ. of Bayreuth (Germany). Bavarian Geoinstitute
  2. Univ. of Bayreuth (Germany). Bavarian Geoinstitute; Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)
  3. European Synchrotron Radiation Facility (ESRF), Grenoble (France)
  4. Univ. of Milan (Italy). Dept. of Earth Sciences
  5. Center for Hydrocarbon Recovery, Moscow (Russia). Skolkovo Inst. of Science and Technology
  6. Univ. of Bayreuth (Germany). Bavarian Geoinstitute
  7. Univ. of Bayreuth (Germany). Bavarian Geoinstitute; National Univ., of Science and Technology, Moscow (Russia). Material Modeling and Development Lab.
  8. Univ. of Cologne (Germany). Inst. of Geology and Mineralogy
  9. Univ. of Chicago, IL (United States). Center for Advanced Radiation Sources
Publication Date:
Research Org.:
Univ. of Chicago, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1393163
Grant/Contract Number:  
FG02-94ER14466; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 8; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES

Citation Formats

Cerantola, Valerio, Bykova, Elena, Kupenko, Ilya, Merlini, Marco, Ismailova, Leyla, McCammon, Catherine, Bykov, Maxim, Chumakov, Alexandr I., Petitgirard, Sylvain, Kantor, Innokenty, Svitlyk, Volodymyr, Jacobs, Jeroen, Hanfland, Michael, Mezouar, Mohamed, Prescher, Clemens, Rüffer, Rudolf, Prakapenka, Vitali B., and Dubrovinsky, Leonid. Stability of iron-bearing carbonates in the deep Earth’s interior. United States: N. p., 2017. Web. doi:10.1038/ncomms15960.
Cerantola, Valerio, Bykova, Elena, Kupenko, Ilya, Merlini, Marco, Ismailova, Leyla, McCammon, Catherine, Bykov, Maxim, Chumakov, Alexandr I., Petitgirard, Sylvain, Kantor, Innokenty, Svitlyk, Volodymyr, Jacobs, Jeroen, Hanfland, Michael, Mezouar, Mohamed, Prescher, Clemens, Rüffer, Rudolf, Prakapenka, Vitali B., & Dubrovinsky, Leonid. Stability of iron-bearing carbonates in the deep Earth’s interior. United States. doi:10.1038/ncomms15960.
Cerantola, Valerio, Bykova, Elena, Kupenko, Ilya, Merlini, Marco, Ismailova, Leyla, McCammon, Catherine, Bykov, Maxim, Chumakov, Alexandr I., Petitgirard, Sylvain, Kantor, Innokenty, Svitlyk, Volodymyr, Jacobs, Jeroen, Hanfland, Michael, Mezouar, Mohamed, Prescher, Clemens, Rüffer, Rudolf, Prakapenka, Vitali B., and Dubrovinsky, Leonid. Wed . "Stability of iron-bearing carbonates in the deep Earth’s interior". United States. doi:10.1038/ncomms15960. https://www.osti.gov/servlets/purl/1393163.
@article{osti_1393163,
title = {Stability of iron-bearing carbonates in the deep Earth’s interior},
author = {Cerantola, Valerio and Bykova, Elena and Kupenko, Ilya and Merlini, Marco and Ismailova, Leyla and McCammon, Catherine and Bykov, Maxim and Chumakov, Alexandr I. and Petitgirard, Sylvain and Kantor, Innokenty and Svitlyk, Volodymyr and Jacobs, Jeroen and Hanfland, Michael and Mezouar, Mohamed and Prescher, Clemens and Rüffer, Rudolf and Prakapenka, Vitali B. and Dubrovinsky, Leonid},
abstractNote = {The presence of carbonates in inclusions in diamonds coming from depths exceeding 670 km are obvious evidence that carbonates exist in the Earth’s lower mantle. However, their range of stability, crystal structures and the thermodynamic conditions of the decarbonation processes remain poorly constrained. We investigate the behaviour of pure iron carbonate at pressures over 100 GPa and temperatures over 2,500 K using single-crystal X-ray diffraction and Mossbauer spectroscopy in laser-heated diamond anvil cells. On heating to temperatures of the Earth’s geotherm at pressures to B 50 GPa FeCO 3 partially dissociates to form various iron oxides. Furthermore, at higher pressures FeCO 3 forms two new structures— tetrairon(III) orthocarbonate Fe$3+\atop{4}$C3O12 and diiron(II) diiron(III) tetracarbonate Fe$2+\atop{2}$ Fe$3+\atop{2}$C4 O13, both phases containing CO4 tetrahedra. Fe4 C4 O13 is stable at conditions along the entire geotherm to depths of at least 2,500 km, thus demonstrating that self-oxidation-reduction reactions can preserve carbonates in the Earth’s lower mantle.},
doi = {10.1038/ncomms15960},
journal = {Nature Communications},
number = ,
volume = 8,
place = {United States},
year = {2017},
month = {7}
}

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    • Thomson, Andrew R.; Walter, Michael J.; Kohn, Simon C.
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    • DOI: 10.1038/nature16174

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    • Hu, Qingyang; Kim, Duck Young; Yang, Wenge
    • Nature, Vol. 534, Issue 7606
    • DOI: 10.1038/nature18018

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    • Ovsyannikov, Sergey V.; Bykov, Maxim; Bykova, Elena
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    • DOI: 10.1038/ncomms10661

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    • DOI: 10.1038/ncomms7311

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    • DOI: 10.1038/srep07640

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    Portable double-sided laser-heating system for Mössbauer spectroscopy and X-ray diffraction experiments at synchrotron facilities with diamond anvil cells
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    • Kupenko, I.; Dubrovinsky, L.; Dubrovinskaia, N.
    • Review of Scientific Instruments, Vol. 83, Issue 12
    • DOI: 10.1063/1.4772458

    Toward an internally consistent pressure scale
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    • Fei, Y.; Ricolleau, A.; Frank, M.
    • Proceedings of the National Academy of Sciences, Vol. 104, Issue 22
    • DOI: 10.1073/pnas.0609013104

    New host for carbon in the deep Earth
    journal, March 2011

    • Boulard, E.; Gloter, A.; Corgne, A.
    • Proceedings of the National Academy of Sciences, Vol. 108, Issue 13
    • DOI: 10.1073/pnas.1016934108

    Structures of dolomite at ultrahigh pressure and their influence on the deep carbon cycle
    journal, August 2012

    • Merlini, M.; Crichton, W. A.; Hanfland, M.
    • Proceedings of the National Academy of Sciences, Vol. 109, Issue 34
    • DOI: 10.1073/pnas.1201336109

    Reevaluating carbon fluxes in subduction zones, what goes down, mostly comes up
    journal, June 2015

    • Kelemen, Peter B.; Manning, Craig E.
    • Proceedings of the National Academy of Sciences, Vol. 112, Issue 30
    • DOI: 10.1073/pnas.1507889112

    The structure of the metallic high-pressure Fe 3 O 4 polymorph: experimental and theoretical study
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    • Dubrovinsky, L. S.; Dubrovinskaia, N. A.; McCammon, C.
    • Journal of Physics: Condensed Matter, Vol. 15, Issue 45
    • DOI: 10.1088/0953-8984/15/45/009

    GEOCHEMISTRY: The Paradox of Mantle Redox
    journal, May 2005


    Deep Mantle Cycling of Oceanic Crust: Evidence from Diamonds and Their Mineral Inclusions
    journal, September 2011


    Optical properties of siderite (FeCO 3 ) across the spin transition: Crossover to iron-rich carbonates in the lower mantle
    journal, May 2015

    • Lobanov, Sergey S.; Goncharov, Alexander F.; Litasov, Konstantin D.
    • American Mineralogist, Vol. 100, Issue 5-6
    • DOI: 10.2138/am-2015-5053

    High-pressure spectroscopic study of siderite (FeCO 3 ) with a focus on spin crossover
    journal, November 2015

    • Cerantola, Valerio; McCammon, Catherine; Kupenko, Ilya
    • American Mineralogist, Vol. 100, Issue 11-12
    • DOI: 10.2138/am-2015-5319

    The MnCO 3 -II high-pressure polymorph of rhodocrosite
    journal, November 2015

    • Merlini, Marco; Hanfland, Michael; Gemmi, Mauro
    • American Mineralogist, Vol. 100, Issue 11-12
    • DOI: 10.2138/am-2015-5320

    The crystal structures of Mg 2 Fe 2 C 4 O 13 , with tetrahedrally coordinated carbon, and Fe 13 O 19 , synthesized at deep mantle conditions
    journal, August 2015

    • Merlini, Marco; Hanfland, Michael; Salamat, Ashkan
    • American Mineralogist, Vol. 100, Issue 8-9
    • DOI: 10.2138/am-2015-5369

    Stability of the MgCO3 structures under lower mantle conditions
    journal, May 2005


    High-pressure transition of CaCO3
    journal, July 2007

    • Ono, S.; Kikegawa, T.; Ohishi, Y.
    • American Mineralogist, Vol. 92, Issue 7
    • DOI: 10.2138/am.2007.2649

    Static disorders of atoms and experimental determination of Debye temperature in pyrope: Low- and high-temperature single-crystal X-ray diffraction study
    journal, September 2011

    • Nakatsuka, A.; Shimokawa, M.; Nakayama, N.
    • American Mineralogist, Vol. 96, Issue 10
    • DOI: 10.2138/am.2011.3714

    Vibrational and elastic properties of ferromagnesite across the electronic spin-pairing transition of iron
    journal, March 2012

    • Lin, J. -F.; Liu, J.; Jacobs, C.
    • American Mineralogist, Vol. 97, Issue 4
    • DOI: 10.2138/am.2012.3961

    Experimental determination of siderite stability at high pressure
    journal, August 2013


    Thermal equation of state and spin transition of magnesiosiderite at high pressure and temperature
    journal, January 2014


    Structure, Bonding, and Mineralogy of Carbon at Extreme Conditions
    journal, January 2013

    • Oganov, A. R.; Hemley, R. J.; Hazen, R. M.
    • Reviews in Mineralogy and Geochemistry, Vol. 75, Issue 1
    • DOI: 10.2138/rmg.2013.75.3

    Polymerized 4-Fold Coordinated Carbonate Melts in the Deep Mantle
    journal, April 2019

    • Sanloup, Chrystèle; Hudspeth, Jessica M.; Afonina, Veronika
    • Frontiers in Earth Science, Vol. 7
    • DOI: 10.3389/feart.2019.00072

    High-Pressure Synthesis of a Nitrogen-Rich Inclusion Compound ReN 8 ⋅ x  N 2 with Conjugated Polymeric Nitrogen Chains
    journal, June 2018

    • Bykov, Maxim; Bykova, Elena; Koemets, Egor
    • Angewandte Chemie, Vol. 130, Issue 29
    • DOI: 10.1002/ange.201805152

    High-Pressure Synthesis of a Nitrogen-Rich Inclusion Compound ReN 8 ⋅ x  N 2 with Conjugated Polymeric Nitrogen Chains
    journal, June 2018

    • Bykov, Maxim; Bykova, Elena; Koemets, Egor
    • Angewandte Chemie, Vol. 130, Issue 29
    • DOI: 10.1002/ange.201805152

    High-Pressure Synthesis of a Nitrogen-Rich Inclusion Compound ReN 8x  N 2 with Conjugated Polymeric Nitrogen Chains
    journal, June 2018

    • Bykov, Maxim; Bykova, Elena; Koemets, Egor
    • Angewandte Chemie International Edition, Vol. 57, Issue 29
    • DOI: 10.1002/anie.201805152

    Pressure driven spin transition in siderite and magnesiosiderite single crystals
    text, January 2017

    • Weis, Christopher; Sternemann, Christian; Cerantola, Valerio
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2017-12450

    Polymerized 4-Fold Coordinated Carbonate Melts in the Deep Mantle
    text, January 2019

    • Sanloup, Chrystèle; Hudspeth, Jessica M.; Afonina, Veronika
    • Deutsches Elektronen-Synchrotron, DESY, Hamburg
    • DOI: 10.3204/pubdb-2019-02016