A classical view on nonclassical nucleation
| Autor: | Nico A. J. M. Sommerdijk, Aaron R. Finney, Jozua Laven, James J. De Yoreo, Paul J. M. Smeets, Fabio Nudelman, Heiner Friedrich, P. Mark Rodger, Wouter J. E. M. Habraken |
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| Přispěvatelé: | Materials and Interface Chemistry, Institute for Complex Molecular Systems |
| Jazyk: | angličtina |
| Rok vydání: | 2017 |
| Předmět: |
Nucleation
Crystal growth 02 engineering and technology 010402 general chemistry 01 natural sciences Ion law.invention law Phase (matter) Vaterite Crystallization Supersaturation Multidisciplinary Precipitation (chemistry) Chemistry 021001 nanoscience & nanotechnology 0104 chemical sciences PNAS Plus Molecular simulation Chemical physics Physical chemistry Cryo-electron microscopy 0210 nano-technology Calcium carbonate |
| Zdroj: | Smeets, P J M, Finney, A R, Habraken, W J E M, Nudelman, F, Friedrich, H, Laven, J, De Yoreo, J J, Rodger, P M & Sommerdijk, N A J M 2017, ' A classical view on nonclassical nucleation ', Proceedings of the National Academy of Sciences, vol. 114, no. 38, pp. E7882-E7890 . https://doi.org/10.1073/pnas.1700342114 Proceedings of the National Academy of Sciences of the United States of America (PNAS), 114(38), E7882-E7890. National Academy of Sciences Proceedings of the National Academy of Sciences of the United States of America |
| ISSN: | 0027-8424 |
| DOI: | 10.1073/pnas.1700342114 |
| Popis: | Understanding and controlling nucleation is important for many crystallization applications. Calcium carbonate (CaCO3) is often used as a model system to investigate nucleation mechanisms. Despite its great importance in geology, biology, and many industrial applications, CaCO3 nucleation is still a topic of intense discussion, with new pathways for its growth from ions in solution proposed in recent years. These new pathways include the so-called nonclassical nucleation mechanism via the assembly of thermodynamically stable prenucleation clusters, as well as the formation of a dense liquid precursor phase via liquid–liquid phase separation. Here, we present results from a combined experimental and computational investigation on the precipitation of CaCO3 in dilute aqueous solutions. We propose that a dense liquid phase (containing 4–7 H2O per CaCO3 unit) forms in supersaturated solutions through the association of ions and ion pairs without significant participation of larger ion clusters. This liquid acts as the precursor for the formation of solid CaCO3 in the form of vaterite, which grows via a net transfer of ions from solution according to z Ca2+ + z CO3 2− → z CaCO3. The results show that all steps in this process can be explained according to classical concepts of crystal nucleation and growth, and that long-standing physical concepts of nucleation can describe multistep, multiphase growth mechanisms. |
| Databáze: | OpenAIRE |
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