Clathrate structure-type recognition: Application to hydrate nucleation and crystallisation
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- Marco Lauricella
- University College Dublin 1 School of Physics, , Belfield, Dublin 4, Ireland
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- Simone Meloni
- University College Dublin 1 School of Physics, , Belfield, Dublin 4, Ireland
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- Shuai Liang
- University of Calgary 4 Deptartment of Chemistry, , Calgary, Alberta T2N 1N4, Canada
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- Niall J. English
- University College Dublin 6 School of Chemical and Bioprocess Engineering, , Belfield, Dublin 4, Ireland
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- Peter G. Kusalik
- University of Calgary 4 Deptartment of Chemistry, , Calgary, Alberta T2N 1N4, Canada
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- Giovanni Ciccotti
- University College Dublin 1 School of Physics, , Belfield, Dublin 4, Ireland
書誌事項
- 公開日
- 2015-06-24
- DOI
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- 10.1063/1.4922696
- 公開者
- AIP Publishing
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説明
<jats:p>For clathrate-hydrate polymorphic structure-type (sI versus sII), geometric recognition criteria have been developed and validated. These are applied to the study of the rich interplay and development of both sI and sII motifs in a variety of hydrate-nucleation events for methane and H2S hydrate studied by direct and enhanced-sampling molecular dynamics (MD) simulations. In the case of nucleation of methane hydrate from enhanced-sampling simulation, we notice that already at the transition state, ∼80% of the enclathrated CH4 molecules are contained in a well-structured (sII) clathrate-like crystallite. For direct MD simulation of nucleation of H2S hydrate, some sI/sII polymorphic diversity was encountered, and it was found that a realistic dissipation of the nucleation energy (in view of non-equilibrium relaxation to either microcanonical (NVE) or isothermal-isobaric (NPT) distributions) is important to determine the relative propensity to form sI versus sII motifs.</jats:p>
収録刊行物
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- The Journal of Chemical Physics
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The Journal of Chemical Physics 142 (24), 2015-06-24
AIP Publishing