All-Atom Molecular Dynamics of Pure Water–Methane Gas Hydrate Systems under Pre-Nucleation Conditions: A Direct Comparison between Experiments and Simulations of Transport Properties for the Tip4p/Ice Water Model
(1) Background: New technologies involving gas hydrates under pre-nucleation conditions such as gas separations and storage have become more prominent. This has necessitated the characterization and modeling of the transport properties of such systems. (2) Methodology: This work explored methane hyd...
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| Format: | Article |
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MDPI AG
2022-08-01
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| Series: | Molecules |
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| Online Access: | https://www.mdpi.com/1420-3049/27/15/5019 |
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| author | André Guerra Samuel Mathews Milan Marić Phillip Servio Alejandro D. Rey |
| author_facet | André Guerra Samuel Mathews Milan Marić Phillip Servio Alejandro D. Rey |
| author_sort | André Guerra |
| collection | DOAJ |
| description | (1) Background: New technologies involving gas hydrates under pre-nucleation conditions such as gas separations and storage have become more prominent. This has necessitated the characterization and modeling of the transport properties of such systems. (2) Methodology: This work explored methane hydrate systems under pre-nucleation conditions. All-atom molecular dynamics simulations were used to quantify the performance of the TIP4P/2005 and TIP4P/Ice water models to predict the viscosity, diffusivity, and thermal conductivity using various formulations. (3) Results: Molecular simulation equilibrium was robustly demonstrated using various measures. The Green–Kubo estimation of viscosity outperformed other formulations when combined with TIP4P/Ice, and the same combination outperformed all TIP4P/2005 formulations. The Green–Kubo TIP4P/Ice estimation of viscosity overestimates (by 84% on average) the viscosity of methane hydrate systems under pre-nucleation conditions across all pressures considered (0–5 MPag). The presence of methane was found to increase the average number of hydrogen bonds over time (6.7–7.8%). TIP4P/Ice methane systems were also found to have 16–19% longer hydrogen bond lifetimes over pure water systems. (4) Conclusion: An inherent limitation in the current water force field for its application in the context of transport properties estimations for methane gas hydrate systems. A re-parametrization of the current force field is suggested as a starting point. Until then, this work may serve as a characterization of the deviance in viscosity prediction. |
| first_indexed | 2024-03-09T05:08:59Z |
| format | Article |
| id | doaj.art-57803440f74c4eb8ac3c7819692ceb01 |
| institution | Directory Open Access Journal |
| issn | 1420-3049 |
| language | English |
| last_indexed | 2024-03-09T05:08:59Z |
| publishDate | 2022-08-01 |
| publisher | MDPI AG |
| record_format | Article |
| series | Molecules |
| spelling | doaj.art-57803440f74c4eb8ac3c7819692ceb012023-12-03T12:51:06ZengMDPI AGMolecules1420-30492022-08-012715501910.3390/molecules27155019All-Atom Molecular Dynamics of Pure Water–Methane Gas Hydrate Systems under Pre-Nucleation Conditions: A Direct Comparison between Experiments and Simulations of Transport Properties for the Tip4p/Ice Water ModelAndré Guerra0Samuel Mathews1Milan Marić2Phillip Servio3Alejandro D. Rey4Department of Chemical Engineering, McGill University, Montréal, QC H3A 0G, CanadaDepartment of Chemical Engineering, McGill University, Montréal, QC H3A 0G, CanadaDepartment of Chemical Engineering, McGill University, Montréal, QC H3A 0G, CanadaDepartment of Chemical Engineering, McGill University, Montréal, QC H3A 0G, CanadaDepartment of Chemical Engineering, McGill University, Montréal, QC H3A 0G, Canada(1) Background: New technologies involving gas hydrates under pre-nucleation conditions such as gas separations and storage have become more prominent. This has necessitated the characterization and modeling of the transport properties of such systems. (2) Methodology: This work explored methane hydrate systems under pre-nucleation conditions. All-atom molecular dynamics simulations were used to quantify the performance of the TIP4P/2005 and TIP4P/Ice water models to predict the viscosity, diffusivity, and thermal conductivity using various formulations. (3) Results: Molecular simulation equilibrium was robustly demonstrated using various measures. The Green–Kubo estimation of viscosity outperformed other formulations when combined with TIP4P/Ice, and the same combination outperformed all TIP4P/2005 formulations. The Green–Kubo TIP4P/Ice estimation of viscosity overestimates (by 84% on average) the viscosity of methane hydrate systems under pre-nucleation conditions across all pressures considered (0–5 MPag). The presence of methane was found to increase the average number of hydrogen bonds over time (6.7–7.8%). TIP4P/Ice methane systems were also found to have 16–19% longer hydrogen bond lifetimes over pure water systems. (4) Conclusion: An inherent limitation in the current water force field for its application in the context of transport properties estimations for methane gas hydrate systems. A re-parametrization of the current force field is suggested as a starting point. Until then, this work may serve as a characterization of the deviance in viscosity prediction.https://www.mdpi.com/1420-3049/27/15/5019watermethanehydratesviscositydiffusivitymolecular dynamics |
| spellingShingle | André Guerra Samuel Mathews Milan Marić Phillip Servio Alejandro D. Rey All-Atom Molecular Dynamics of Pure Water–Methane Gas Hydrate Systems under Pre-Nucleation Conditions: A Direct Comparison between Experiments and Simulations of Transport Properties for the Tip4p/Ice Water Model Molecules water methane hydrates viscosity diffusivity molecular dynamics |
| title | All-Atom Molecular Dynamics of Pure Water–Methane Gas Hydrate Systems under Pre-Nucleation Conditions: A Direct Comparison between Experiments and Simulations of Transport Properties for the Tip4p/Ice Water Model |
| title_full | All-Atom Molecular Dynamics of Pure Water–Methane Gas Hydrate Systems under Pre-Nucleation Conditions: A Direct Comparison between Experiments and Simulations of Transport Properties for the Tip4p/Ice Water Model |
| title_fullStr | All-Atom Molecular Dynamics of Pure Water–Methane Gas Hydrate Systems under Pre-Nucleation Conditions: A Direct Comparison between Experiments and Simulations of Transport Properties for the Tip4p/Ice Water Model |
| title_full_unstemmed | All-Atom Molecular Dynamics of Pure Water–Methane Gas Hydrate Systems under Pre-Nucleation Conditions: A Direct Comparison between Experiments and Simulations of Transport Properties for the Tip4p/Ice Water Model |
| title_short | All-Atom Molecular Dynamics of Pure Water–Methane Gas Hydrate Systems under Pre-Nucleation Conditions: A Direct Comparison between Experiments and Simulations of Transport Properties for the Tip4p/Ice Water Model |
| title_sort | all atom molecular dynamics of pure water methane gas hydrate systems under pre nucleation conditions a direct comparison between experiments and simulations of transport properties for the tip4p ice water model |
| topic | water methane hydrates viscosity diffusivity molecular dynamics |
| url | https://www.mdpi.com/1420-3049/27/15/5019 |
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