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    Replacement of Calcium Carbonate Polymorphs by Cerussite
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    ACS Earth and Space Chemistry

    Cite this: ACS Earth Space Chem. 2021, 5, 9, 2433–2441
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    https://doi.org/10.1021/acsearthspacechem.1c00177
    Published September 1, 2021
    Copyright © 2021 UChicago Argonne, LLC, Operator of Argonne National Laboratory. Published by American Chemical Society
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    Abstract

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    Calcium carbonate (CaCO3) polymorphs, calcite, aragonite, and vaterite, serve as a major sink to retain various metal ions in natural and engineered systems. Here, we visualize the systematic trends in reactivities of calcite, vaterite, and aragonite to Pb2+ dissolved in acidic aqueous solutions using in situ optical microscopy combined with ex situ scanning electron and transmission X-ray microscopies. All three polymorphs undergo pseudomorphic replacement by cerussite (PbCO3) but with distinct differences in the evolution of their morphologies. The replacement of calcite and aragonite occurs through the formation of a pseudomorphic cerussite shell (typically 5–10 μm thick) followed by a slower inward propagation of reaction fronts through a thin solution gap (∼0.1 μm wide) between the shell and the CaCO3 substrate. The replacement of vaterite is characterized by the formation of a thinner cerussite shell (≤1 μm thick) and a larger cavity between the shell and the host mineral. These systematic differences in cerussite morphology for different CaCO3 polymorphs are explained by the relative dissolution and precipitation rates of the reactant and product minerals, coupled with the role of ion transport through the cerussite shells. We also find that the replacement of calcite by cerussite is the slowest when all three polymorphs coexisted. Our results provide mechanistic insights into the growth mode of cerussite on dissolving calcium carbonate and demonstrate these CaCO3 polymorphs as promising substrate materials for removal and recycling of Pb from acidic polluted water and industrial effluents.

    Copyright © 2021 UChicago Argonne, LLC, Operator of Argonne National Laboratory. Published by American Chemical Society

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsearthspacechem.1c00177.

    • X-ray diffraction patterns of aragonite, calcite, and vaterite/calcite mixture before and after the reaction with the acidic Pb2+-containing solution; variation in the morphology of a calcite/vaterite; in the acidic Pb2+ solution; and SEM images and energy-dispersive X-ray spectroscopy measurement of a calcite/aragonite/vaterite mixture reacted in the acidic Pb2+-containing solution (PDF)

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    Cited By

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    This article is cited by 13 publications.

    1. Bektur Abdilla, Sang Soo Lee, Paul Fenter, Neil C. Sturchio. Dynamic Surface Incorporation of Pb2+ Ions at the Actively Dissolving Calcite (104) Surface. Environmental Science & Technology 2024, 58 (37) , 16525-16534. https://doi.org/10.1021/acs.est.4c03567
    2. Bektur Abdilla, Sang Soo Lee, Paul Fenter, Neil C. Sturchio. Dynamic Inhibition of Calcite Dissolution in Flowing Acidic Pb2+ Solutions. Environmental Science & Technology 2024, 58 (16) , 7133-7143. https://doi.org/10.1021/acs.est.3c10105
    3. Maggie A. Cooper, Bruno C. Batista, Oliver Steinbock. Non-equilibrium Composition of Mixed Metal Hydroxide Membranes Grown in Flow Systems. ACS Earth and Space Chemistry 2023, 7 (12) , 2410-2419. https://doi.org/10.1021/acsearthspacechem.3c00188
    4. Peng Yang, Sang Soo Lee, Paul Fenter, Jacquelyn N. Bracco, Andrew G. Stack. Sorption of Arsenate, Selenate, and Molybdate on the Barite (001) Surface. ACS Earth and Space Chemistry 2023, 7 (8) , 1545-1556. https://doi.org/10.1021/acsearthspacechem.3c00096
    5. Julie J. Kim, Sang Soo Lee, Paul Fenter, Satish C. B. Myneni, Viktor Nikitin, Catherine A. Peters. Carbonate Coprecipitation for Cd and Zn Treatment and Evaluation of Heavy Metal Stability Under Acidic Conditions. Environmental Science & Technology 2023, 57 (8) , 3104-3113. https://doi.org/10.1021/acs.est.2c07678
    6. Pablo Forjanes, Carlos Pérez-Garrido, Pedro Álvarez-Lloret, José Manuel Astilleros, Lurdes Fernández-Díaz. Formation of Strontianite and Witherite Cohesive Layers on Calcite Surfaces for Building Stone Conservation. Crystal Growth & Design 2022, 22 (11) , 6418-6428. https://doi.org/10.1021/acs.cgd.2c00383
    7. William D. Leal, Caroline L. Bergeron, Tyler J. Rutherford, Marek B. Majewski. Conversion of Electrochemically Deposited Aragonite Crystallites to Perovskite through Ion Exchange. Crystal Growth & Design 2022, 22 (4) , 2364-2371. https://doi.org/10.1021/acs.cgd.1c01449
    8. YoungJae Kim. Preliminary study on calcite replacement by strontianite. Journal of the Geological Society of Korea 2024, 60 (4) , 399-404. https://doi.org/10.14770/jgsk.2024.040
    9. YoungJae Kim, Sang Soo Lee, Bektur Abdilla, Viktor Nikitin, Neil C. Sturchio, Paul Fenter. Formation of zinc carbonate phases on dissolving calcite, aragonite, and vaterite in acidic aqueous solutions. Geochimica et Cosmochimica Acta 2024, 380 , 131-139. https://doi.org/10.1016/j.gca.2024.06.034
    10. YoungJae Kim, Seon Yong Lee, Young Jae Lee. Review of Water-Based Synthetic Methods of Calcium Carbonate Polymorphs and Their Morphological Features. Economic and Environmental Geology 2023, 56 (3) , 217-227. https://doi.org/10.9719/EEG.2023.56.3.217
    11. Marwa Eltarahony, Eman Ibrahim, Ghada Hegazy, Amira Sabry. Microbial Remediation of Mercury: An Overview. 2023, 201-234. https://doi.org/10.1007/978-981-99-7719-2_8
    12. YoungJae Kim, Aniket Tekawade, Sang Soo Lee, Paul Fenter. Morphological and crystallographic controls in the replacement of calcite and aragonite by cerussite and otavite. Geochimica et Cosmochimica Acta 2023, 341 , 16-27. https://doi.org/10.1016/j.gca.2022.11.010
    13. Catherine Noiriel, François Renard. Four-dimensional X-ray micro-tomography imaging of dynamic processes in geosciences. Comptes Rendus. Géoscience 2022, 354 (G2) , 255-280. https://doi.org/10.5802/crgeos.137
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    ACS Earth and Space Chemistry

    Cite this: ACS Earth Space Chem. 2021, 5, 9, 2433–2441
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsearthspacechem.1c00177
    Published September 1, 2021
    Copyright © 2021 UChicago Argonne, LLC, Operator of Argonne National Laboratory. Published by American Chemical Society
    Request reuse permissions

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