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    Entropy Drives Calcium Carbonate Ion Association

    245751_245751.pdf (805.2Kb)
    Access Status
    Open access
    Authors
    Kellermeier, M.
    Raiteri, Paolo
    Berg, J.
    Kempter, A.
    Gale, Julian
    Gebauer, D.
    Date
    2016
    Type
    Journal Article
    
    Metadata
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    Citation
    Kellermeier, M. and Raiteri, P. and Berg, J. and Kempter, A. and Gale, J. and Gebauer, D. 2016. Entropy Drives Calcium Carbonate Ion Association. ChemPhysChem. 17 (21): pp. 3535-3541.
    Source Title
    ChemPhysChem
    DOI
    10.1002/cphc.201600653
    ISSN
    1439-4235
    School
    Department of Chemistry
    Funding and Sponsorship
    http://purl.org/au-research/grants/arc/DP160100677
    http://purl.org/au-research/grants/arc/FT130100463
    URI
    http://hdl.handle.net/20.500.11937/5346
    Collection
    • Curtin Research Publications
    Abstract

    The understanding of the molecular mechanisms underlying the early stages of crystallisation is still incomplete. In the case of calcium carbonate, experimental and computational evidence suggests that phase separation relies on so-called pre-nucleation clusters (PNCs). A thorough thermodynamic analysis of the enthalpic and entropic contributions to the overall free energy of PNC formation derived from three independent methods demonstrates that solute clustering is driven by entropy. This can be quantitatively rationalised by the release of water molecules from ion hydration layers, explaining why ion association is not limited to simple ion pairing. The key role of water release in this process suggests that PNC formation should be a common phenomenon in aqueous solutions.

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