Two-Step Formation of Methane-Propane Mixed Gas Hydrates in A Batch-Type Reactor

Tsutomu Uchida, Minoru Moriwaki, Satoshi Takeya, Ikuko Y. Ikeda, Ryo Ohmura, Jiro Nagao, Hideki Minagawa, Takao Ebinuma, Hideo Narita, Kazutoshi Gohara, Shinji Mae

Research output: Contribution to journalArticlepeer-review

87 Citations (Scopus)


Vapor compositions of methane and propane mixed gas in a batch-type reactor were measured by gas chromatography during hydrate crystallization at 274 K with molar ratios of propane below 10 vol %. The volume ratio of propane in the vapor decreased as the hydrate crystallization progressed. When the initial propane concentration was between 4 and 8 vol %, rapid gas consumption occurred for about 1 h, causing an initial pressure drop, and after a temporary stabilization of the pressure, a second pressure drop occurred; that is, hydrate crystallization occurred in two steps. X-Ray diffraction and Raman spectroscopic analyses on samples taken from the reactor during each step revealed that the structure II methane-propane mixed gas hydrates crystallized in the first step, and structure I methane hydrates in the second step. This process was observed only when the partial pressure of methane was above the equilibrium pressure of methane hydrate at the end of the first step.

Original languageEnglish
Pages (from-to)518-523
Number of pages6
JournalAIChE Journal
Issue number2
Publication statusPublished - 2004 Feb
Externally publishedYes


  • Batch-type reactor
  • Crystallographic structure
  • Methane-propane hydrate
  • Second induction time

ASJC Scopus subject areas

  • Biotechnology
  • Environmental Engineering
  • Chemical Engineering(all)


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