Microscopic evidence for liquid-liquid separation in supersaturated CaCO3 solutions
Recent experimental observations of the onset of calcium carbonate (CaCO3) mineralization suggest the emergence of a population of clusters that are stable rather than unstable as predicted by classical nucleation theory. This study uses molecular dynamics simulations to probe the structure, dynamic...
| Main Authors: | , , , , , , , , |
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| Format: | Journal Article |
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The American Association for the Advancement of Science
2013
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| Online Access: | http://www.sciencemag.org/content/341/6148/885 http://hdl.handle.net/20.500.11937/26522 |
| _version_ | 1848752010733551616 |
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| author | Wallace, A. Hedges, L. Fernandez-Martinez, A. Raiteri, Paolo Gale, Julian Waychunas, G. Whitelam, S. Banfield, J. De Yoreo, J. |
| author_facet | Wallace, A. Hedges, L. Fernandez-Martinez, A. Raiteri, Paolo Gale, Julian Waychunas, G. Whitelam, S. Banfield, J. De Yoreo, J. |
| author_sort | Wallace, A. |
| building | Curtin Institutional Repository |
| collection | Online Access |
| description | Recent experimental observations of the onset of calcium carbonate (CaCO3) mineralization suggest the emergence of a population of clusters that are stable rather than unstable as predicted by classical nucleation theory. This study uses molecular dynamics simulations to probe the structure, dynamics, and energetics of hydrated CaCO3 clusters and lattice gas simulations to explore the behavior of cluster populations before nucleation. Our results predict formation of a dense liquid phase through liquid-liquid separation within the concentration range in which clusters are observed. Coalescence and solidification of nanoscale droplets results in formation of a solid phase, the structure of which is consistent with amorphous CaCO3. The presence of a liquid-liquid binodal enables a diverse set of experimental observations to be reconciled within the context of established phase-separation mechanisms. |
| first_indexed | 2025-11-14T08:01:49Z |
| format | Journal Article |
| id | curtin-20.500.11937-26522 |
| institution | Curtin University Malaysia |
| institution_category | Local University |
| last_indexed | 2025-11-14T08:01:49Z |
| publishDate | 2013 |
| publisher | The American Association for the Advancement of Science |
| recordtype | eprints |
| repository_type | Digital Repository |
| spelling | curtin-20.500.11937-265222017-09-13T15:51:39Z Microscopic evidence for liquid-liquid separation in supersaturated CaCO3 solutions Wallace, A. Hedges, L. Fernandez-Martinez, A. Raiteri, Paolo Gale, Julian Waychunas, G. Whitelam, S. Banfield, J. De Yoreo, J. liquid-liquid separation CaCO3 Recent experimental observations of the onset of calcium carbonate (CaCO3) mineralization suggest the emergence of a population of clusters that are stable rather than unstable as predicted by classical nucleation theory. This study uses molecular dynamics simulations to probe the structure, dynamics, and energetics of hydrated CaCO3 clusters and lattice gas simulations to explore the behavior of cluster populations before nucleation. Our results predict formation of a dense liquid phase through liquid-liquid separation within the concentration range in which clusters are observed. Coalescence and solidification of nanoscale droplets results in formation of a solid phase, the structure of which is consistent with amorphous CaCO3. The presence of a liquid-liquid binodal enables a diverse set of experimental observations to be reconciled within the context of established phase-separation mechanisms. 2013 Journal Article http://hdl.handle.net/20.500.11937/26522 10.1126/science.1230915 http://www.sciencemag.org/content/341/6148/885 The American Association for the Advancement of Science fulltext |
| spellingShingle | liquid-liquid separation CaCO3 Wallace, A. Hedges, L. Fernandez-Martinez, A. Raiteri, Paolo Gale, Julian Waychunas, G. Whitelam, S. Banfield, J. De Yoreo, J. Microscopic evidence for liquid-liquid separation in supersaturated CaCO3 solutions |
| title | Microscopic evidence for liquid-liquid separation in supersaturated CaCO3 solutions |
| title_full | Microscopic evidence for liquid-liquid separation in supersaturated CaCO3 solutions |
| title_fullStr | Microscopic evidence for liquid-liquid separation in supersaturated CaCO3 solutions |
| title_full_unstemmed | Microscopic evidence for liquid-liquid separation in supersaturated CaCO3 solutions |
| title_short | Microscopic evidence for liquid-liquid separation in supersaturated CaCO3 solutions |
| title_sort | microscopic evidence for liquid-liquid separation in supersaturated caco3 solutions |
| topic | liquid-liquid separation CaCO3 |
| url | http://www.sciencemag.org/content/341/6148/885 http://hdl.handle.net/20.500.11937/26522 |