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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craippubl:10.1063/1.4922696 2024-06-23T07:54:37+00:00 Clathrate structure-type recognition: Application to hydrate nucleation and crystallisation Lauricella, Marco Meloni, Simone Liang, Shuai English, Niall J. Kusalik, Peter G. Ciccotti, Giovanni Ireland-Canada University Foundation MIUR-FIRB Natural Sciences and Engineering Research Council of Canada Science Foundation Ireland National Natural Science Foundation of China 2015 http://dx.doi.org/10.1063/1.4922696 https://pubs.aip.org/aip/jcp/article-pdf/doi/10.1063/1.4922696/15497631/244503_1_online.pdf en eng AIP Publishing The Journal of Chemical Physics volume 142, issue 24 ISSN 0021-9606 1089-7690 journal-article 2015 craippubl https://doi.org/10.1063/1.4922696 2024-06-13T04:04:23Z 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. Article in Journal/Newspaper Methane hydrate AIP Publishing The Journal of Chemical Physics 142 24 |
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AIP Publishing |
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English |
description |
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. |
author2 |
Ireland-Canada University Foundation MIUR-FIRB Natural Sciences and Engineering Research Council of Canada Science Foundation Ireland National Natural Science Foundation of China |
format |
Article in Journal/Newspaper |
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 |
AIP Publishing |
publishDate |
2015 |
url |
http://dx.doi.org/10.1063/1.4922696 https://pubs.aip.org/aip/jcp/article-pdf/doi/10.1063/1.4922696/15497631/244503_1_online.pdf |
genre |
Methane hydrate |
genre_facet |
Methane hydrate |
op_source |
The Journal of Chemical Physics volume 142, issue 24 ISSN 0021-9606 1089-7690 |
op_doi |
https://doi.org/10.1063/1.4922696 |
container_title |
The Journal of Chemical Physics |
container_volume |
142 |
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24 |
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1802646827598610432 |