Nucleation rate analysis of methane hydrate from molecular dynamics simulations

Daisuke Yuhara, Brian C. Barnes, Donguk Suh, Brandon C. Knott, Gregg T. Beckham, Kenji Yasuoka, David T. Wu, Amadeu K. Sum

Research output: Contribution to journalArticle

25 Citations (Scopus)

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. 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 calculated by MFPT and SP methods are within 5%, and 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.

Original languageEnglish
Pages (from-to)463-474
Number of pages12
JournalFaraday Discussions
Volume179
DOIs
Publication statusPublished - 2015 Jul 1

Fingerprint

Methane
Hydrates
hydrates
Molecular dynamics
clathrates
Nucleation
methane
nucleation
molecular dynamics
Computer simulation
simulation
nuclei
maximum likelihood estimates
Energy barriers
Maximum likelihood
Free energy
Gases
free energy
chemistry
Crystalline materials

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

Yuhara, D., Barnes, B. C., Suh, D., Knott, B. C., Beckham, G. T., Yasuoka, K., ... Sum, A. K. (2015). Nucleation rate analysis of methane hydrate from molecular dynamics simulations. Faraday Discussions, 179, 463-474. https://doi.org/10.1039/c4fd00219a

Nucleation rate analysis of methane hydrate from molecular dynamics simulations. / Yuhara, Daisuke; Barnes, Brian C.; Suh, Donguk; Knott, Brandon C.; Beckham, Gregg T.; Yasuoka, Kenji; Wu, David T.; Sum, Amadeu K.

In: Faraday Discussions, Vol. 179, 01.07.2015, p. 463-474.

Research output: Contribution to journalArticle

Yuhara, D, Barnes, BC, Suh, D, Knott, BC, Beckham, GT, Yasuoka, K, Wu, DT & Sum, AK 2015, 'Nucleation rate analysis of methane hydrate from molecular dynamics simulations', Faraday Discussions, vol. 179, pp. 463-474. https://doi.org/10.1039/c4fd00219a
Yuhara, Daisuke ; Barnes, Brian C. ; Suh, Donguk ; Knott, Brandon C. ; Beckham, Gregg T. ; Yasuoka, Kenji ; Wu, David T. ; Sum, Amadeu K. / Nucleation rate analysis of methane hydrate from molecular dynamics simulations. In: Faraday Discussions. 2015 ; Vol. 179. pp. 463-474.
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