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Computation of Atmospheric Concentrations of Molecular Clusters from ab initio Thermochemistry
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Excess Gibbs potential model for multicomponent hydrogen clathrates.

Sangyong Lee1, Prasad Yedlapalli, Jae W Lee

  • 1Department of Chemical and Natural Gas Engineering, Texas A&M University, Kingsville, Texas 78363, USA.

The Journal of Physical Chemistry. B
|December 22, 2006
PubMed
Summary

A new thermodynamic model predicts multicomponent gas hydrate equilibrium conditions, incorporating excess Gibbs potential for accurate cavity distortion calculations. This method enhances predictions for hydrogen-containing hydrates, crucial for energy storage and transport.

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Area of Science:

  • Thermodynamics
  • Physical Chemistry
  • Materials Science

Background:

  • Accurate prediction of multicomponent gas hydrate equilibrium is essential for various industrial applications.
  • Existing models often struggle to account for complex interactions and distortions in hydrate structures with multiple guest molecules.
  • Hydrogen-containing gas hydrates present unique challenges due to their specific molecular interactions and potential for significant water-cavity distortions.

Purpose of the Study:

  • To introduce a novel thermodynamic calculation procedure for predicting equilibrium conditions of multicomponent gas hydrates, specifically including hydrogen.
  • To develop a model that accounts for water-cavity distortions caused by multiple guest species using an excess Gibbs potential term.
  • To integrate this new approach with established models like Lee-Holder and Zele-Lee-Holder for enhanced predictive accuracy.

Main Methods:

  • Development of a new thermodynamic calculation procedure.
  • Incorporation of an excess Gibbs potential term to model water-cavity distortions.
  • Integration of the excess Gibbs potential with the Lee-Holder and Zele-Lee-Holder models for multicomponent gas hydrate equilibrium calculations.

Main Results:

  • The model accurately predicts equilibrium conditions for binary gas hydrates containing hydrogen, with deviations within 10-20% of experimental values.
  • Predictions for ternary and quaternary mixture hydrates show reasonable accuracy.
  • Model error increases with rising pressure and temperature, particularly in the presence of tetrahydrofuran (THF).

Conclusions:

  • The proposed thermodynamic calculation procedure, incorporating an excess Gibbs potential, effectively predicts multicomponent gas hydrate equilibrium, especially for hydrogen-containing systems.
  • The model provides a valuable tool for understanding and predicting the behavior of complex gas hydrates.
  • Further refinement may be needed to improve accuracy at higher pressures and temperatures, especially for systems with specific additives like THF.