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Journal of Chemical Physics / Volume 124 / Issue 23 / ARTICLES / Surfaces, Interfaces, and Materials

J. Chem. Phys. 124, 234710 (2006); doi:10.1063/1.2207138 (12 pages)

Multiscale approach to CO2 hydrate formation in aqueous solution: Phase field theory and molecular dynamics. Nucleation and growth

György Tegze1, Tamás Pusztai1, Gyula Tóth1, László Gránásy1, Atle Svandal2, Trygve Buanes2, Tatyana Kuznetsova2, and Bjørn Kvamme2

1Research Institute for Solid State Physics and Optics, P.O. Box 49, H-1525 Budapest, Hungary
2Institute of Physics and Technology, University of Bergen, Allégaten 55, N-5007 Bergen, Norway

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(Received 14 December 2005; accepted 27 April 2006; published online 20 June 2006)

A phase field theory with model parameters evaluated from atomistic simulations/experiments is applied to predict the nucleation and growth rates of solid CO2 hydrate in aqueous solutions under conditions typical to underwater natural gas hydrate reservoirs. It is shown that under practical conditions a homogeneous nucleation of the hydrate phase can be ruled out. The growth rate of CO2 hydrate dendrites has been determined from phase field simulations as a function of composition while using a physical interface thickness (0.85±0.07 nm) evaluated from molecular dynamics simulations. The growth rate extrapolated to realistic supersaturations is about three orders of magnitude larger than the respective experimental observation. A possible origin of the discrepancy is discussed. It is suggested that a kinetic barrier reflecting the difficulties in building the complex crystal structure is the most probable source of the deviations.

© 2006 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. MULTISCALE APPROACH TO GAS HYDRATE FORMATION
    1. Phase field theory
      1. Equilibrium interface
      2. Calculation of the nucleation barrier
      3. Phase field simulation of single crystal growth
      4. Numerical implementation
    2. Molecular dynamics
  3. PHYSICAL PROPERTIES
  4. RESULTS AND DISCUSSION
    1. The planar hydrate-solution interface
      1. Molecular dynamics
      2. Phase field theory
    2. Nucleation of CO2 hydrate
    3. Growth of CO2 hydrate dendrites in aqueous solution
  5. SUMMARY

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KEYWORDS and PACS

Keywords

nucleation, molecular dynamics method, dendrites, carbon compounds

PACS

  • 64.60.Q-

    Nucleation

  • 61.50.Ah

    Theory of crystal structure, crystal symmetry; calculations and modeling

  • 68.70.+w

    Whiskers and dendrites (growth, structure, and nonelectronic properties)

ARTICLE DATA

Permalink
http://link.aip.org/link/doi/10.1063/1.2207138

PUBLICATION DATA

ISSN:

0021-9606 (print)  
1089-7690 (online)

Publisher:

$abstract.society.value is a Member of CrossRef American Institute of Physics

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