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Title: Nucleation Rate Analysis of Methane Hydrate from Molecular Dynamics Simulations

Abstract

Clathrate hydrates are solid crystalline structures most commonly formed from solutions that have nucleated to form a mixed solid composed of water and gas. Understanding the mechanism of clathrate hydrate nucleation is essential to grasp the fundamental chemistry of these complex structures and their applications. Molecular dynamics (MD) simulation is an ideal method to study nucleation at the molecular level because the size of the critical nucleus and formation rate occur on the nano scale. Moreover, various analysis methods for nucleation have been developed through MD to analyze nucleation. In particular, the mean first-passage time (MFPT) and survival probability (SP) methods have proven to be effective in procuring the nucleation rate and critical nucleus size for monatomic systems. This study assesses the MFPT and SP methods, previously used for monatomic systems, when applied to analyzing clathrate hydrate nucleation. Because clathrate hydrate nucleation is relatively difficult to observe in MD simulations (due to its high free energy barrier), these methods have yet to be applied to clathrate hydrate systems. In this study, we have analyzed the nucleation rate and critical nucleus size of methane hydrate using MFPT and SP methods from data generated by MD simulations at 255 K and 50more » MPa. MFPT was modified for clathrate hydrate from the original version by adding the maximum likelihood estimate and growth effect term. The nucleation rates were calculated by MFPT and SP methods and are within 5%; the critical nucleus size estimated by the MFPT method was 50% higher, than values obtained through other more rigorous but computationally expensive estimates. These methods can also be extended to the analysis of other clathrate hydrates.« less

Authors:
 [1];  [2];  [1];  [3];  [3];  [1];  [2];
+ Show Author Affiliations
  1. Keio Univ., Yokohama (Japan)
  2. Colorado School of Mines, Golden, CO (United States)
  3. National Renewable Energy Lab. (NREL), Golden, CO (United States)
Publication Date:
Research Org.:
National Renewable Energy Laboratory (NREL), Golden, CO (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1242024
Report Number(s):
NREL/JA-5100-64933
Journal ID: ISSN 1359-6640
Grant/Contract Number:  
AC36-08GO28308
Resource Type:
Accepted Manuscript
Journal Name:
Faraday Discussions
Additional Journal Information:
Journal Volume: 179; Related Information: Faraday Discussions; Journal ID: ISSN 1359-6640
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
59 BASIC BIOLOGICAL SCIENCES; molecular dynamics (MD) simulation; mean first-passage time (MFPT); survival probability (SP); clathrate hydrate nucleation

Citation Formats

Yuhara, Daisuke, Barnes, Brian C., Suh, Donguk, Knott, Brandon C., Beckham, Gregg T., Yasuoka, Kenji, Wu, David T., and Amadeu K. Sum. Nucleation Rate Analysis of Methane Hydrate from Molecular Dynamics Simulations. United States: N. p., 2015. Web. doi:10.1039/C4FD00219A.
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Yuhara, Daisuke, Barnes, Brian C., Suh, Donguk, Knott, Brandon C., Beckham, Gregg T., Yasuoka, Kenji, Wu, David T., & Amadeu K. Sum. Nucleation Rate Analysis of Methane Hydrate from Molecular Dynamics Simulations. United States. https://doi.org/10.1039/C4FD00219A
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Yuhara, Daisuke, Barnes, Brian C., Suh, Donguk, Knott, Brandon C., Beckham, Gregg T., Yasuoka, Kenji, Wu, David T., and Amadeu K. Sum. Tue . "Nucleation Rate Analysis of Methane Hydrate from Molecular Dynamics Simulations". United States. https://doi.org/10.1039/C4FD00219A. https://www.osti.gov/servlets/purl/1242024.
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@article{osti_1242024,
title = {Nucleation Rate Analysis of Methane Hydrate from Molecular Dynamics Simulations},
author = {Yuhara, Daisuke and Barnes, Brian C. and Suh, Donguk and Knott, Brandon C. and Beckham, Gregg T. and Yasuoka, Kenji and Wu, David T. and Amadeu K. Sum},
abstractNote = {Clathrate hydrates are solid crystalline structures most commonly formed from solutions that have nucleated to form a mixed solid composed of water and gas. Understanding the mechanism of clathrate hydrate nucleation is essential to grasp the fundamental chemistry of these complex structures and their applications. Molecular dynamics (MD) simulation is an ideal method to study nucleation at the molecular level because the size of the critical nucleus and formation rate occur on the nano scale. Moreover, various analysis methods for nucleation have been developed through MD to analyze nucleation. In particular, the mean first-passage time (MFPT) and survival probability (SP) methods have proven to be effective in procuring the nucleation rate and critical nucleus size for monatomic systems. This study assesses the MFPT and SP methods, previously used for monatomic systems, when applied to analyzing clathrate hydrate nucleation. Because clathrate hydrate nucleation is relatively difficult to observe in MD simulations (due to its high free energy barrier), these methods have yet to be applied to clathrate hydrate systems. In this study, we have analyzed the nucleation rate and critical nucleus size of methane hydrate using MFPT and SP methods from data generated by MD simulations at 255 K and 50 MPa. MFPT was modified for clathrate hydrate from the original version by adding the maximum likelihood estimate and growth effect term. The nucleation rates were calculated by MFPT and SP methods and are within 5%; the critical nucleus size estimated by the MFPT method was 50% higher, than values obtained through other more rigorous but computationally expensive estimates. These methods can also be extended to the analysis of other clathrate hydrates.},
doi = {10.1039/C4FD00219A},
journal = {Faraday Discussions},
number = ,
volume = 179,
place = {United States},
year = {Tue Jan 06 00:00:00 EST 2015},
month = {Tue Jan 06 00:00:00 EST 2015}
}
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https://doi.org/10.1039/C4FD00219A
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