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From Ions to Crystals : A Comprehensive View of the Non-Classical Nucleation of Calcium Sulfate

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2024

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Drechsler, Markus
Stawski, Tomasz M.
Fernandez‐Martinez, Alejandro
Van Driessche, Alexander E. S.

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Angewandte Chemie International Edition. Wiley. 2024, 63(51), e202408429. ISSN 1433-7851. eISSN 1521-3773. Verfügbar unter: doi: 10.1002/anie.202408429

Zusammenfassung

The early stages of mineralization continue to be in the focus of intensive research due to their inherent importance for natural and engineered environments. While numerous observations have been reported for single steps in the pathways of various crystallizing phases in previous studies, the complexity of the underlying processes and their elusive character have left central questions unanswered in most cases. In the present work, we provide a detailed view on the nucleation of calcium sulfate mineralization—an abundant mineral with broad use in construction industry—in aqueous systems at ambient conditions. As experimental basis, a co-titration procedure with potentiometric, turbidimetric and conductometric detection was developed, allowing solution speciation and the formation of crystallization precursors to be monitored quantitatively as the level of nominal (super)saturation gradually increases. The nature and spatiotemporal evolution of these precursors was further elucidated by time-resolved small-angle X-ray scattering (SAXS) and analytical ultracentrifugation (AUC) experiments, complemented by cryogenic transmission electron microscopy (cryo-TEM) as a direct imaging technique. The results reveal how ions associate into nanometric primary species, which subsequently aggregate and develop anisotropic order by intrinsic structural reorganization. Our observations challenge the common understanding of fundamental notions such as the nucleation barrier or the meaning of supersaturation, with broad implications for mineralization phenomena in general and the formation of calcium sulfate in geochemical settings and industrial applications in particular.

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540 Chemie

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ISO 690KELLERMEIER, Matthias, Johanna SCHECK, Markus DRECHSLER, Rose ROSENBERG, Tomasz M. STAWSKI, Alejandro FERNANDEZ‐MARTINEZ, Denis GEBAUER, Alexander E. S. VAN DRIESSCHE, 2024. From Ions to Crystals : A Comprehensive View of the Non-Classical Nucleation of Calcium Sulfate. In: Angewandte Chemie International Edition. Wiley. 2024, 63(51), e202408429. ISSN 1433-7851. eISSN 1521-3773. Verfügbar unter: doi: 10.1002/anie.202408429
BibTex
@article{Kellermeier2024-12-16Cryst-71582,
  year={2024},
  doi={10.1002/anie.202408429},
  title={From Ions to Crystals : A Comprehensive View of the Non-Classical Nucleation of Calcium Sulfate},
  number={51},
  volume={63},
  issn={1433-7851},
  journal={Angewandte Chemie International Edition},
  author={Kellermeier, Matthias and Scheck, Johanna and Drechsler, Markus and Rosenberg, Rose and Stawski, Tomasz M. and Fernandez‐Martinez, Alejandro and Gebauer, Denis and Van Driessche, Alexander E. S.},
  note={Article Number: e202408429}
}
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