Rate Prediction for Homogeneous Nucleation of Methane Hydrate at Moderate Supersaturation Using Transition Interface Sampling
[Image: see text] The crystallization of methane hydrates via homogeneous nucleation under natural, moderate conditions is of both industrial and scientific relevance, yet still poorly understood. Predicting the nucleation rates at such conditions is notoriously difficult due to high nucleation barr...
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ftpubmed:oai:pubmedcentral.nih.gov:7503527 2023-05-15T17:12:02+02:00 Rate Prediction for Homogeneous Nucleation of Methane Hydrate at Moderate Supersaturation Using Transition Interface Sampling Arjun, A. Bolhuis, P. G. 2020-08-17 http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7503527/ https://doi.org/10.1021/acs.jpcb.0c04582 en eng American Chemical Society http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7503527/ http://dx.doi.org/10.1021/acs.jpcb.0c04582 Copyright © 2020 American Chemical Society This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes. CC-BY-NC-ND J Phys Chem B Text 2020 ftpubmed https://doi.org/10.1021/acs.jpcb.0c04582 2020-09-27T00:37:38Z [Image: see text] The crystallization of methane hydrates via homogeneous nucleation under natural, moderate conditions is of both industrial and scientific relevance, yet still poorly understood. Predicting the nucleation rates at such conditions is notoriously difficult due to high nucleation barriers, and requires, besides an accurate molecular model, enhanced sampling. Here, we apply the transition interface sampling technique, which efficiently computes the exact rate of nucleation by generating ensembles of unbiased dynamical trajectories crossing predefined interfaces located between the stable states. Using an accurate atomistic force field and focusing on specific conditions of 280 K and 500 bar, we compute for nucleation directly into the sI crystal phase at a rate of ∼10(–17) nuclei per nanosecond per simulation volume or ∼10(2) nuclei per second per cm(3), in agreement with consensus estimates for nearby conditions. As this is most likely fortuitous, we discuss the causes of the large differences between our results and previous simulation studies. Our work shows that it is now possible to compute rates for methane hydrates at moderate supersaturation, without relying on any assumptions other than the force field. Text Methane hydrate PubMed Central (PMC) The Journal of Physical Chemistry B 124 37 8099 8109 |
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[Image: see text] The crystallization of methane hydrates via homogeneous nucleation under natural, moderate conditions is of both industrial and scientific relevance, yet still poorly understood. Predicting the nucleation rates at such conditions is notoriously difficult due to high nucleation barriers, and requires, besides an accurate molecular model, enhanced sampling. Here, we apply the transition interface sampling technique, which efficiently computes the exact rate of nucleation by generating ensembles of unbiased dynamical trajectories crossing predefined interfaces located between the stable states. Using an accurate atomistic force field and focusing on specific conditions of 280 K and 500 bar, we compute for nucleation directly into the sI crystal phase at a rate of ∼10(–17) nuclei per nanosecond per simulation volume or ∼10(2) nuclei per second per cm(3), in agreement with consensus estimates for nearby conditions. As this is most likely fortuitous, we discuss the causes of the large differences between our results and previous simulation studies. Our work shows that it is now possible to compute rates for methane hydrates at moderate supersaturation, without relying on any assumptions other than the force field. |
format |
Text |
author |
Arjun, A. Bolhuis, P. G. |
spellingShingle |
Arjun, A. Bolhuis, P. G. Rate Prediction for Homogeneous Nucleation of Methane Hydrate at Moderate Supersaturation Using Transition Interface Sampling |
author_facet |
Arjun, A. Bolhuis, P. G. |
author_sort |
Arjun, A. |
title |
Rate Prediction for Homogeneous Nucleation of Methane Hydrate at Moderate Supersaturation Using Transition Interface Sampling |
title_short |
Rate Prediction for Homogeneous Nucleation of Methane Hydrate at Moderate Supersaturation Using Transition Interface Sampling |
title_full |
Rate Prediction for Homogeneous Nucleation of Methane Hydrate at Moderate Supersaturation Using Transition Interface Sampling |
title_fullStr |
Rate Prediction for Homogeneous Nucleation of Methane Hydrate at Moderate Supersaturation Using Transition Interface Sampling |
title_full_unstemmed |
Rate Prediction for Homogeneous Nucleation of Methane Hydrate at Moderate Supersaturation Using Transition Interface Sampling |
title_sort |
rate prediction for homogeneous nucleation of methane hydrate at moderate supersaturation using transition interface sampling |
publisher |
American Chemical Society |
publishDate |
2020 |
url |
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7503527/ https://doi.org/10.1021/acs.jpcb.0c04582 |
genre |
Methane hydrate |
genre_facet |
Methane hydrate |
op_source |
J Phys Chem B |
op_relation |
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC7503527/ http://dx.doi.org/10.1021/acs.jpcb.0c04582 |
op_rights |
Copyright © 2020 American Chemical Society This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes. |
op_rightsnorm |
CC-BY-NC-ND |
op_doi |
https://doi.org/10.1021/acs.jpcb.0c04582 |
container_title |
The Journal of Physical Chemistry B |
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124 |
container_issue |
37 |
container_start_page |
8099 |
op_container_end_page |
8109 |
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1766068786657492992 |