Clathrate structure-type recognition: Application to hydrate nucleation and crystallisation
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 stu...
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2015
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Online Access: | https://doi.org/10.1063/1.4922696 http://infoscience.epfl.ch/record/212463 |
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ftinfoscience:oai:infoscience.tind.io:212463 2023-05-15T17:11:57+02:00 Clathrate structure-type recognition: Application to hydrate nucleation and crystallisation Lauricella, Marco Meloni, Simone Liang, Shuai English, Niall J. Kusalik, Peter G. Ciccotti, Giovanni 2015-09-28T07:53:53Z https://doi.org/10.1063/1.4922696 http://infoscience.epfl.ch/record/212463 unknown Melville, Amer Inst Physics doi:10.1063/1.4922696 ISI:000357615100038 http://infoscience.epfl.ch/record/212463 http://infoscience.epfl.ch/record/212463 Text 2015 ftinfoscience https://doi.org/10.1063/1.4922696 2023-02-13T22:29:42Z 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, similar to 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. (C) 2015 AIP Publishing LLC. Text Methane hydrate EPFL Infoscience (Ecole Polytechnique Fédérale Lausanne) The Journal of Chemical Physics 142 24 244503 |
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EPFL Infoscience (Ecole Polytechnique Fédérale Lausanne) |
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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, similar to 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. (C) 2015 AIP Publishing LLC. |
format |
Text |
author |
Lauricella, Marco Meloni, Simone Liang, Shuai English, Niall J. Kusalik, Peter G. Ciccotti, Giovanni |
spellingShingle |
Lauricella, Marco Meloni, Simone Liang, Shuai English, Niall J. Kusalik, Peter G. Ciccotti, Giovanni Clathrate structure-type recognition: Application to hydrate nucleation and crystallisation |
author_facet |
Lauricella, Marco Meloni, Simone Liang, Shuai English, Niall J. Kusalik, Peter G. Ciccotti, Giovanni |
author_sort |
Lauricella, Marco |
title |
Clathrate structure-type recognition: Application to hydrate nucleation and crystallisation |
title_short |
Clathrate structure-type recognition: Application to hydrate nucleation and crystallisation |
title_full |
Clathrate structure-type recognition: Application to hydrate nucleation and crystallisation |
title_fullStr |
Clathrate structure-type recognition: Application to hydrate nucleation and crystallisation |
title_full_unstemmed |
Clathrate structure-type recognition: Application to hydrate nucleation and crystallisation |
title_sort |
clathrate structure-type recognition: application to hydrate nucleation and crystallisation |
publisher |
Melville, Amer Inst Physics |
publishDate |
2015 |
url |
https://doi.org/10.1063/1.4922696 http://infoscience.epfl.ch/record/212463 |
genre |
Methane hydrate |
genre_facet |
Methane hydrate |
op_source |
http://infoscience.epfl.ch/record/212463 |
op_relation |
doi:10.1063/1.4922696 ISI:000357615100038 http://infoscience.epfl.ch/record/212463 |
op_doi |
https://doi.org/10.1063/1.4922696 |
container_title |
The Journal of Chemical Physics |
container_volume |
142 |
container_issue |
24 |
container_start_page |
244503 |
_version_ |
1766068717243858944 |