Derivation of an Accurate Force-Field for Simulating the Growth of Calcium Carbonate from Aqueous Solution: A New Model for the Calcite−Water Interface
| Autor: | P. Mark Rodger, David Quigley, Julian D. Gale, Paolo Raiteri |
|---|---|
| Rok vydání: | 2010 |
| Předmět: |
Calcite
Aqueous solution Chemistry Enthalpy Inorganic chemistry Solvation Thermodynamics chemistry.chemical_element Calcium Surfaces Coatings and Films Electronic Optical and Magnetic Materials chemistry.chemical_compound General Energy Calcium carbonate Carbonate Physical and Theoretical Chemistry Dissolution |
| Zdroj: | The Journal of Physical Chemistry C. 114:5997-6010 |
| ISSN: | 1932-7455 1932-7447 |
| DOI: | 10.1021/jp910977a |
| Popis: | The performance of existing force-field models for the calcium carbonate - water system has been critically assessed with particular reference to the thermodynamic consequences. It is demonstrated that all currently available parametrizations fail to describe the calcite-aragonite phase transition, and the free energies of solvation for the calcium cation are also considerably in error leading to a poor description of the dissolution enthalpy for calcite. A new force-field, based on rigid carbonate ions, has been developed that corrects these deficiencies and accurately describes the thermodynamics of the aqueous calcium carbonate system within molecular dynamics simulations. Not only does this new model lead to quantitative changes in the properties of the calcite (1014) surface in contact with water, but also significant qualitative differences. With this more accurate model it is found that calcium ions do not adsorb at the pristine basal plane of calcite, while carbonate ions only weakly bind. Carbon... |
| Databáze: | OpenAIRE |
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