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Water Dynamics from THz Spectroscopy Reveal the Locus of a Liquid–Liquid Binodal Limit in Aqueous CaCO<sub>3</sub> Solutions

Water Dynamics from THz Spectroscopy Reveal the Locus of a Liquid–Liquid Binodal Limit in Aqueous CaCO3 Solutions

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SEBASTIANI, Federico, Stefan L. P. WOLF, Benjamin BORN, Trung Quan LUONG, Helmut CÖLFEN, Denis GEBAUER, Martina HAVENITH, 2017. Water Dynamics from THz Spectroscopy Reveal the Locus of a Liquid–Liquid Binodal Limit in Aqueous CaCO3 Solutions. In: Angewandte Chemie International Edition. 56(2), pp. 490-495. ISSN 1433-7851. eISSN 1521-3773. Available under: doi: 10.1002/anie.201610554

@article{Sebastiani2017-01-09Water-37236, title={Water Dynamics from THz Spectroscopy Reveal the Locus of a Liquid–Liquid Binodal Limit in Aqueous CaCO3 Solutions}, year={2017}, doi={10.1002/anie.201610554}, number={2}, volume={56}, issn={1433-7851}, journal={Angewandte Chemie International Edition}, pages={490--495}, author={Sebastiani, Federico and Wolf, Stefan L. P. and Born, Benjamin and Luong, Trung Quan and Cölfen, Helmut and Gebauer, Denis and Havenith, Martina} }

Wolf, Stefan L. P. Havenith, Martina Born, Benjamin Many phenomena depend on CaCO<sub>3</sub> nucleation where the role of water remains enigmatic. Changes in THz absorption during the early stages of CaCO<sub>3</sub> nucleation evidence altered coupled motions of hydrated calcium and carbonate ions. The direct link between these changes and the continuous development of the ion activity product reveals the locus of a liquid–liquid binodal limit. The data strongly suggest that proto-structured amorphous CaCO<sub>3</sub> forms through solidification of initially liquid precursors. Furthermore, polycarboxylates, which stabilize liquid precursors of CaCO<sub>3</sub>, significantly enhance the kinetic stability of the metastable liquid–liquid state, but they do not affect the locus of the binodal limit. The importance of water network dynamics in phase separation mechanisms can be understood based on the notions of the pre-nucleation cluster pathway, and is likely to be more general for aqueous systems. Luong, Trung Quan Cölfen, Helmut Born, Benjamin Gebauer, Denis Havenith, Martina Water Dynamics from THz Spectroscopy Reveal the Locus of a Liquid–Liquid Binodal Limit in Aqueous CaCO<sub>3</sub> Solutions Luong, Trung Quan Sebastiani, Federico 2017-02-09T07:40:58Z Wolf, Stefan L. P. 2017-01-09 2017-02-09T07:40:58Z Sebastiani, Federico eng Gebauer, Denis Cölfen, Helmut

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