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Zafer Maşlakcı1, J Paul Devlin2, Nevin Uras-Aytemiz1

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Ammonia (NH3) in clathrate hydrates (CHs) exhibits unique behaviors, influencing water bonding and potentially acting as a catalyst. This study identifies three NH3 types and their interactions within CH structures.

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Area of Science:

  • Chemistry
  • Materials Science
  • Spectroscopy

Background:

  • Clathrate hydrates (CHs) are inclusion compounds formed by water cages trapping guest molecules.
  • Ammonia (NH3) is a key molecule in various chemical processes, but its behavior in CHs is not fully understood.
  • Vibrational spectroscopy is crucial for identifying molecular structures and interactions within CHs.

Purpose of the Study:

  • To identify and characterize the vibrational spectroscopic signatures of ammonia (NH3) within binary clathrate hydrates (CHs).
  • To elucidate the role of ammonia in the formation and stabilization of clathrate hydrate structures.
  • To investigate the long-term effects of guest molecule replacement on ternary CHs.

Main Methods:

  • High-quality Fourier-transform infrared (FTIR) spectroscopy was used to analyze aerosols of NH3-THF and NH3-TMO binary clathrate hydrates.
  • An all-vapor, sub-second clathrate hydrate formation approach was employed.
  • Computational studies were integrated to aid in the identification of spectroscopic signatures.

Main Results:

  • Three distinct types of ammonia (NH3) were identified within the clathrate hydrate structure: classical small-cage, nonclassical small-cage, and network ammonia.
  • Network ammonia perturbs water bonding, creating orientational defects stabilized by guest molecules, rather than directly inducing non-classical structures.
  • The study observed the impact of CO2 and CH4 as NH3 replacement molecules on ternary CHs over time.

Conclusions:

  • Ammonia's behavior in clathrate hydrates is complex, involving perturbation of water networks and potential catalytic activity during CH formation.
  • The findings offer new insights into the structure and dynamics of ammonia-containing clathrate hydrates.
  • Understanding these interactions is vital for applications involving gas storage and separation using clathrate hydrates.