Short-lived calcium carbonate precursors observed in situ via Bullet-dynamic nuclear polarization

Autor: Ertan Turhan, Masoud Minaei, Pooja Narwal, Benno Meier, Karel Kouřil, Dennis Kurzbach
Jazyk: angličtina
Rok vydání: 2024
Předmět:
Zdroj: Communications Chemistry, Vol 7, Iss 1, Pp 1-6 (2024)
Druh dokumentu: article
ISSN: 2399-3669
DOI: 10.1038/s42004-024-01300-5
Popis: Abstract The discovery of (meta)stable pre-nucleation species (PNS) challenges the established nucleation-and-growth paradigm. While stable PNS with long lifetimes are readily accessible experimentally, identifying and characterizing early-stage intermediates with short lifetimes remains challenging. We demonstrate that species with lifetimes ≪ 5 s can be characterized by nuclear magnetic resonance spectroscopy when boosted by ‘Bullet’ dynamic nuclear polarization (Bullet-DNP). We investigate the previously elusive early-stage prenucleation of calcium carbonates in the highly supersaturated concentration regime, characterizing species that form within milliseconds after the encounter of calcium and carbonate ions and show that ionic pre-nucleation species not only govern the solidification of calcium carbonates at weak oversaturation but also initiate rapid precipitation events at high concentrations. Such, we report a transient co-existence of two PNS with distinct molecular sizes and different compositions. This methodological advance may open new possibilities for studying and exploiting carbonate-based material formation in unexplored parts of the phase space.
Databáze: Directory of Open Access Journals
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