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Stable Prenucleation Calcium Carbonate Clusters Define Liquid-Liquid Phase Separation.
Angewandte Chemie International Edition ( IF 12.959 ) Pub Date : 2020-02-25 , DOI: 10.1002/anie.201915350
Jonathan T Avaro,Stefan L P Wolf,Karin Hauser,Denis Gebauer

Liquid-liquid phase separation (LLPS) is an intermediate step during the precipitation of calcium carbonate, and is assumed to play a key role in biomineralization processes. Here, we have developed a model where ion association thermodynamics in homogeneous phases determine the liquid-liquid miscibility gap of the aqueous calcium carbonate system, verified experimentally using potentiometric titrations, and kinetic studies based on stopped-flow ATR-FTIR spectroscopy. The proposed mechanism explains the variable solubilities of solid amorphous calcium carbonates, reconciling previously inconsistent literature values. Accounting for liquid-liquid amorphous polymorphism, the model also provides clues to the mechanism of polymorph selection. It is general and should be tested for systems other than calcium carbonate to provide a new perspective on the physical chemistry of LLPS mechanisms based on stable prenucleation clusters rather than un-/metastable fluctuations in biomineralization, and beyond.
更新日期:2020-02-25

 

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