Rate Prediction for Homogeneous Nucleation of Methane Hydrate at Moderate Supersaturation Using Transition Interface Sampling
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...
Published in: | The Journal of Physical Chemistry B |
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Online Access: | https://dare.uva.nl/personal/pure/en/publications/rate-prediction-for-homogeneous-nucleation-of-methane-hydrate-at-moderate-supersaturation-using-transition-interface-sampling(ec6df73c-1b2c-4d5e-94b9-4ebdbc3c6fc0).html https://doi.org/10.1021/acs.jpcb.0c04582 https://hdl.handle.net/11245.1/ec6df73c-1b2c-4d5e-94b9-4ebdbc3c6fc0 https://pure.uva.nl/ws/files/58929529/acs.jpcb.0c04582.pdf |
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ftunivamstpubl:oai:dare.uva.nl:openaire_cris_publications/ec6df73c-1b2c-4d5e-94b9-4ebdbc3c6fc0 2024-09-30T14:38:30+00:00 Rate Prediction for Homogeneous Nucleation of Methane Hydrate at Moderate Supersaturation Using Transition Interface Sampling Arjun, A. Bolhuis, P.G. 2020-09-17 application/pdf https://dare.uva.nl/personal/pure/en/publications/rate-prediction-for-homogeneous-nucleation-of-methane-hydrate-at-moderate-supersaturation-using-transition-interface-sampling(ec6df73c-1b2c-4d5e-94b9-4ebdbc3c6fc0).html https://doi.org/10.1021/acs.jpcb.0c04582 https://hdl.handle.net/11245.1/ec6df73c-1b2c-4d5e-94b9-4ebdbc3c6fc0 https://pure.uva.nl/ws/files/58929529/acs.jpcb.0c04582.pdf eng eng https://dare.uva.nl/personal/pure/en/publications/rate-prediction-for-homogeneous-nucleation-of-methane-hydrate-at-moderate-supersaturation-using-transition-interface-sampling(ec6df73c-1b2c-4d5e-94b9-4ebdbc3c6fc0).html info:eu-repo/semantics/openAccess Arjun , A & Bolhuis , P G 2020 , ' Rate Prediction for Homogeneous Nucleation of Methane Hydrate at Moderate Supersaturation Using Transition Interface Sampling ' , Journal of Physical Chemistry B , vol. 124 , no. 37 , pp. 8099-8109 . https://doi.org/10.1021/acs.jpcb.0c04582 article 2020 ftunivamstpubl https://doi.org/10.1021/acs.jpcb.0c04582 2024-09-12T16:38:39Z 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 similar to 10 -17 nuclei per nanosecond per simulation volume or similar to 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. Article in Journal/Newspaper Methane hydrate Universiteit van Amsterdam: Digital Academic Repository (UvA DARE) The Journal of Physical Chemistry B 124 37 8099 8109 |
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Universiteit van Amsterdam: Digital Academic Repository (UvA DARE) |
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English |
description |
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 similar to 10 -17 nuclei per nanosecond per simulation volume or similar to 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 |
Article in Journal/Newspaper |
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 |
publishDate |
2020 |
url |
https://dare.uva.nl/personal/pure/en/publications/rate-prediction-for-homogeneous-nucleation-of-methane-hydrate-at-moderate-supersaturation-using-transition-interface-sampling(ec6df73c-1b2c-4d5e-94b9-4ebdbc3c6fc0).html https://doi.org/10.1021/acs.jpcb.0c04582 https://hdl.handle.net/11245.1/ec6df73c-1b2c-4d5e-94b9-4ebdbc3c6fc0 https://pure.uva.nl/ws/files/58929529/acs.jpcb.0c04582.pdf |
genre |
Methane hydrate |
genre_facet |
Methane hydrate |
op_source |
Arjun , A & Bolhuis , P G 2020 , ' Rate Prediction for Homogeneous Nucleation of Methane Hydrate at Moderate Supersaturation Using Transition Interface Sampling ' , Journal of Physical Chemistry B , vol. 124 , no. 37 , pp. 8099-8109 . https://doi.org/10.1021/acs.jpcb.0c04582 |
op_relation |
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op_rights |
info:eu-repo/semantics/openAccess |
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 |
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8099 |
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8109 |
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