Microscopic insights on clathrate hydrate growth from non-equilibrium molecular dynamics simulations
Clathrate hydrates form and grow at interfaces. Understanding the relevant molecular processes is crucial for developing hydrate-based technologies. Many computational studies focus on hydrate growth within the aqueous phase using the 'direct coexistence method', which is limited in its ab...
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ftucl:oai:eprints.ucl.ac.uk.OAI2:10172799 2023-12-24T10:18:34+01:00 Microscopic insights on clathrate hydrate growth from non-equilibrium molecular dynamics simulations Phan, Anh Stamatakis, Michail Koh, Carolyn A Striolo, Alberto 2023-11 text https://discovery.ucl.ac.uk/id/eprint/10172799/1/1-s2.0-S002197972301055X-main.pdf https://discovery.ucl.ac.uk/id/eprint/10172799/ eng eng Elsevier BV https://discovery.ucl.ac.uk/id/eprint/10172799/1/1-s2.0-S002197972301055X-main.pdf https://discovery.ucl.ac.uk/id/eprint/10172799/ open Journal of Colloid and Interface Science , 649 pp. 185-193. (2023) Adsorption barriers Binding free energy Instantaneous interfaces Interfacial surface area Methane solubility Article 2023 ftucl 2023-11-27T13:07:31Z Clathrate hydrates form and grow at interfaces. Understanding the relevant molecular processes is crucial for developing hydrate-based technologies. Many computational studies focus on hydrate growth within the aqueous phase using the 'direct coexistence method', which is limited in its ability to investigate hydrate film growth at hydrocarbon-water interfaces. To overcome this shortcoming, a new simulation setup is presented here, which allows us to study the growth of a methane hydrate nucleus in a system where oil-water, hydrate-water, and hydrate-oil interfaces are all simultaneously present, thereby mimicking experimental setups. Using this setup, hydrate growth is studied here under the influence of two additives, a polyvinylcaprolactam oligomer and sodium dodecyl sulfate, at varying concentrations. Our results confirm that hydrate films grow along the oil-water interface, in general agreement with visual experimental observations; growth, albeit slower, also occurs at the hydrate-water interface, the interface most often interrogated via simulations. The results obtained demonstrate that the additives present within curved interfaces control the solubility of methane in the aqueous phase, which correlates with hydrate growth rate. Building on our simulation insights, we suggest that by combining data for the potential of mean force profile for methane transport across the oil-water interface and for the average free energy required to perturb a flat interface, it is possible to predict the performance of additives used to control hydrate growth. These insights could be helpful to achieve optimal methane storage in hydrates, one of many applications which are attracting significant fundamental and applied interests. Article in Journal/Newspaper Methane hydrate University College London: UCL Discovery |
institution |
Open Polar |
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University College London: UCL Discovery |
op_collection_id |
ftucl |
language |
English |
topic |
Adsorption barriers Binding free energy Instantaneous interfaces Interfacial surface area Methane solubility |
spellingShingle |
Adsorption barriers Binding free energy Instantaneous interfaces Interfacial surface area Methane solubility Phan, Anh Stamatakis, Michail Koh, Carolyn A Striolo, Alberto Microscopic insights on clathrate hydrate growth from non-equilibrium molecular dynamics simulations |
topic_facet |
Adsorption barriers Binding free energy Instantaneous interfaces Interfacial surface area Methane solubility |
description |
Clathrate hydrates form and grow at interfaces. Understanding the relevant molecular processes is crucial for developing hydrate-based technologies. Many computational studies focus on hydrate growth within the aqueous phase using the 'direct coexistence method', which is limited in its ability to investigate hydrate film growth at hydrocarbon-water interfaces. To overcome this shortcoming, a new simulation setup is presented here, which allows us to study the growth of a methane hydrate nucleus in a system where oil-water, hydrate-water, and hydrate-oil interfaces are all simultaneously present, thereby mimicking experimental setups. Using this setup, hydrate growth is studied here under the influence of two additives, a polyvinylcaprolactam oligomer and sodium dodecyl sulfate, at varying concentrations. Our results confirm that hydrate films grow along the oil-water interface, in general agreement with visual experimental observations; growth, albeit slower, also occurs at the hydrate-water interface, the interface most often interrogated via simulations. The results obtained demonstrate that the additives present within curved interfaces control the solubility of methane in the aqueous phase, which correlates with hydrate growth rate. Building on our simulation insights, we suggest that by combining data for the potential of mean force profile for methane transport across the oil-water interface and for the average free energy required to perturb a flat interface, it is possible to predict the performance of additives used to control hydrate growth. These insights could be helpful to achieve optimal methane storage in hydrates, one of many applications which are attracting significant fundamental and applied interests. |
format |
Article in Journal/Newspaper |
author |
Phan, Anh Stamatakis, Michail Koh, Carolyn A Striolo, Alberto |
author_facet |
Phan, Anh Stamatakis, Michail Koh, Carolyn A Striolo, Alberto |
author_sort |
Phan, Anh |
title |
Microscopic insights on clathrate hydrate growth from non-equilibrium molecular dynamics simulations |
title_short |
Microscopic insights on clathrate hydrate growth from non-equilibrium molecular dynamics simulations |
title_full |
Microscopic insights on clathrate hydrate growth from non-equilibrium molecular dynamics simulations |
title_fullStr |
Microscopic insights on clathrate hydrate growth from non-equilibrium molecular dynamics simulations |
title_full_unstemmed |
Microscopic insights on clathrate hydrate growth from non-equilibrium molecular dynamics simulations |
title_sort |
microscopic insights on clathrate hydrate growth from non-equilibrium molecular dynamics simulations |
publisher |
Elsevier BV |
publishDate |
2023 |
url |
https://discovery.ucl.ac.uk/id/eprint/10172799/1/1-s2.0-S002197972301055X-main.pdf https://discovery.ucl.ac.uk/id/eprint/10172799/ |
genre |
Methane hydrate |
genre_facet |
Methane hydrate |
op_source |
Journal of Colloid and Interface Science , 649 pp. 185-193. (2023) |
op_relation |
https://discovery.ucl.ac.uk/id/eprint/10172799/1/1-s2.0-S002197972301055X-main.pdf https://discovery.ucl.ac.uk/id/eprint/10172799/ |
op_rights |
open |
_version_ |
1786207605027241984 |