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Particle-Mediated Nucleation Pathways Are Imprinted in the Internal Structure of Calcium Sulfate Single Crystals

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    Particle-Mediated Nucleation Pathways Are Imprinted in the Internal Structure of Calcium Sulfate Single Crystals
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    • Tomasz M. Stawski*
      Tomasz M. Stawski
      German Research Centre for Geosciences, GFZ, Interface Geochemistry, Telegrafenberg, 14473, Potsdam, Germany
      *E-mail: [email protected]. Webpage: www.researchgate.net/profile/Tomasz_Stawski.
      More by Tomasz M. Stawski
      Orcidhttp://orcid.org/0000-0002-0881-5808
    • Helen M. Freeman
      Helen M. Freeman
      German Research Centre for Geosciences, GFZ, Interface Geochemistry, Telegrafenberg, 14473, Potsdam, Germany
      School of Chemical and Process Engineering, University of Leeds, Woodhouse Lane, LS2 9JT, Leeds, U.K.
      More by Helen M. Freeman
    • Alexander E. S. Van Driessche*
      Alexander E. S. Van Driessche
      Université Grenoble Alpes, Université Savoie Mont Blanc, CNRS, IRD, IFSTTAR, ISTerre, 38000 Grenoble, France
      *E-mail: [email protected]
      More by Alexander E. S. Van Driessche
      Orcidhttp://orcid.org/0000-0003-2528-3425
    • Jörn Hövelmann
      Jörn Hövelmann
      German Research Centre for Geosciences, GFZ, Interface Geochemistry, Telegrafenberg, 14473, Potsdam, Germany
      More by Jörn Hövelmann
      Orcidhttp://orcid.org/0000-0002-1961-653X
    • Rogier Besselink
      Rogier Besselink
      German Research Centre for Geosciences, GFZ, Interface Geochemistry, Telegrafenberg, 14473, Potsdam, Germany
      Université Grenoble Alpes, Université Savoie Mont Blanc, CNRS, IRD, IFSTTAR, ISTerre, 38000 Grenoble, France
      More by Rogier Besselink
      Orcidhttp://orcid.org/0000-0002-2027-9403
    • Richard Wirth
      Richard Wirth
      German Research Centre for Geosciences, GFZ, Interface Geochemistry, Telegrafenberg, 14473, Potsdam, Germany
      More by Richard Wirth
    • Liane G. Benning
      Liane G. Benning
      German Research Centre for Geosciences, GFZ, Interface Geochemistry, Telegrafenberg, 14473, Potsdam, Germany
      Department of Earth Sciences, Free University of Berlin, Malteserstr. 74-100/Building A, 12249, Berlin, Germany
      School of Earth and Environment, University of Leeds, Woodhouse Lane, LS2 9JT, Leeds, U.K.
      More by Liane G. Benning
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    Crystal Growth & Design

    Cite this: Cryst. Growth Des. 2019, 19, 7, 3714–3721
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    https://doi.org/10.1021/acs.cgd.9b00066
    Published June 11, 2019
    Copyright © 2019 American Chemical Society
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    Abstract

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    Calcium sulfate minerals are found in nature as three hydrates: gypsum (CaSO4·2H2O), bassanite (CaSO4·0.5H2O), and anhydrite (CaSO4). Due to their relevance in natural and industrial processes, the formation pathways of calcium sulfates from aqueous solution have been the subject of intensive research, and there is a growing body of literature, suggesting that calcium sulfates form through nonclassical nanoparticle-mediated crystallization processes. We showed earlier (Stawski et al. Nat. Commun.2016, 7, 11177) that at the early stages in the precipitation reaction, calcium sulfate nanocrystals nucleate through the reorganization and coalescence of aggregates rather than through classical unit addition. Here, we used low-dose dark field (DF) transmission electron microscopy (TEM) and electron diffraction and document that these restructuring processes do not continue until a final near-perfectly homogeneous single crystal is obtained. Instead, we show that the growth process yields a final imperfect mesocrystal with an overall morphology resembling that of a single crystal, yet composed of smaller nanodomains. Our data reveal that organic-free calcium sulfate mesocrystals grown by a particle mediated-pathway may preserve in the final crystal structure a “memory” or “imprint” of their nonclassical nucleation process, something that has been overlooked until now. Furthermore, the nanoscale misalignment of the structural subunits within these crystals might propagate through the length-scales, which is potentially expressed macroscopically as misaligned zones/domains in large single crystals. This is akin to observations in some of the giant crystals from the Naica Mine, Chihuahua, Mexico.

    Copyright © 2019 American Chemical Society

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    The Supporting Information is available free of charge on the ACS Publications website at DOI: 10.1021/acs.cgd.9b00066.

    • Figure S1. TEM analysis of a FIB thin-foil cut from a natural forsterite (nominally Mg2SiO4) and generic olivine ((Mg,Fe2+)2SiO4) single crystals (PDF)

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    Cited By

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    This article is cited by 38 publications.

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    2. Laura Nielsen Lammers Ayumi Koishi . Isotopic Tracers of Nonclassical Crystallization. , 167-198. https://doi.org/10.1021/bk-2021-1383.ch007
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    Crystal Growth & Design

    Cite this: Cryst. Growth Des. 2019, 19, 7, 3714–3721
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.cgd.9b00066
    Published June 11, 2019
    Copyright © 2019 American Chemical Society
    Request reuse permissions

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