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Area of Science:

  • Physical Chemistry
  • Materials Science
  • Thermodynamics

Background:

  • Gas hydrates form complex structures trapping gas molecules under specific temperature and pressure conditions.
  • Existing theories on hydrate lattice distortion primarily explain cavity expansion, not contraction, based on guest size.
  • This limitation leads to a simplified, monotonous relationship between guest size and lattice distortion.

Purpose of the Study:

  • To develop a novel model for gas hydrate lattice distortion that accounts for both contraction and expansion.
  • To investigate the non-monotonous relationship between guest size and lattice distortion.
  • To establish a baseline for undistorted sII-type hydrate lattice distortion.

Main Methods:

  • Statistical thermodynamics-based model combined with the modified Patel-Teja equation of state.
  • Ab initio quantum mechanical calculations using spin-component-scaled second-order Møller-Plesset (SCS-MP2) perturbation theory.
  • Calculation of reference chemical potential difference (RCPD) from experimental hydrate phase equilibrium data.

Main Results:

  • A non-monotonous lattice distortion model was identified, where RCPD initially decreases then increases with guest size.
  • Small guests were shown to contract the hydrate cavity, while larger guests cause expansion.
  • The minimum lattice distortion (794.0913 J mol⁻¹) for an undistorted sII-type hydrate lattice was reported.

Conclusions:

  • The proposed model accurately captures the complex, non-monotonous lattice distortion in gas hydrates.
  • This research provides a more comprehensive understanding of guest-host interactions within hydrate structures.
  • The findings are validated across a range of guest molecules, including methane, nitrogen, and propane hydrates.