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

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Autorschaft

  • Matthias Kellermeier
  • Johanna Scheck
  • Markus Drechsler
  • Rose Rosenberg
  • Tomasz M. Stawski
  • Alejandro Fernandez-Martinez
  • Denis Gebauer
  • Alexander E.S. Van Driessche

Organisationseinheiten

Externe Organisationen

  • BASF SE
  • Universität Konstanz
  • Universität Bayreuth
  • Bundesanstalt für Materialforschung und -prüfung (BAM)
  • Université Grenoble Alpes (UGA)
  • Spanish National Research Council (CSIC)
Forschungs-netzwerk anzeigen

Details

OriginalspracheEnglisch
Aufsatznummere202408429
Seitenumfang12
FachzeitschriftAngewandte Chemie - International Edition
Jahrgang63
Ausgabenummer51
Frühes Online-Datum7 Okt. 2024
PublikationsstatusVeröffentlicht - 9 Dez. 2024

Abstract

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.

ASJC Scopus Sachgebiete

Zitieren

From Ions to Crystals: A Comprehensive View of the Non-Classical Nucleation of Calcium Sulfate. / Kellermeier, Matthias; Scheck, Johanna; Drechsler, Markus et al.
in: Angewandte Chemie - International Edition, Jahrgang 63, Nr. 51, e202408429, 09.12.2024.

Publikation: Beitrag in FachzeitschriftArtikelForschungPeer-Review

Kellermeier, M, Scheck, J, Drechsler, M, Rosenberg, R, Stawski, TM, Fernandez-Martinez, A, Gebauer, D & Van Driessche, AES 2024, 'From Ions to Crystals: A Comprehensive View of the Non-Classical Nucleation of Calcium Sulfate', Angewandte Chemie - International Edition, Jg. 63, Nr. 51, e202408429. https://doi.org/10.1002/anie.202408429
Kellermeier, M., Scheck, J., Drechsler, M., Rosenberg, R., Stawski, T. M., Fernandez-Martinez, A., Gebauer, D., & Van Driessche, A. E. S. (2024). From Ions to Crystals: A Comprehensive View of the Non-Classical Nucleation of Calcium Sulfate. Angewandte Chemie - International Edition, 63(51), Artikel e202408429. https://doi.org/10.1002/anie.202408429
Kellermeier M, Scheck J, Drechsler M, Rosenberg R, Stawski TM, Fernandez-Martinez A et al. From Ions to Crystals: A Comprehensive View of the Non-Classical Nucleation of Calcium Sulfate. Angewandte Chemie - International Edition. 2024 Dez 9;63(51):e202408429. Epub 2024 Okt 7. doi: 10.1002/anie.202408429
Kellermeier, Matthias ; Scheck, Johanna ; Drechsler, Markus et al. / From Ions to Crystals : A Comprehensive View of the Non-Classical Nucleation of Calcium Sulfate. in: Angewandte Chemie - International Edition. 2024 ; Jahrgang 63, Nr. 51.
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AU - Scheck, Johanna

AU - Drechsler, Markus

AU - Rosenberg, Rose

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