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Updated: Apr 18, 2026

Methane Hydrate Crystallization on Sessile Water Droplets
Published on: May 26, 2021
Time-resolved X-ray diffraction and Raman studies of the phase transition mechanisms of methane hydrate
Hisako Hirai1, Hirokazu Kadobayashi1, Naohisa Hirao2
1Geodynamics Research Center, Ehime University, Matsuyama, Ehime 790-8577, Japan.
Abstract:
The mechanisms by which methane hydrate transforms from an sI to sH structure and from an sH to filled-ice Ih structure were examined using time-resolved X-ray diffractometry (XRD) and Raman spectroscopy in conjunction with charge-coupled device camera observation under fixed pressure conditions. The XRD data obtained for the sI-sH transition at 0.8 GPa revealed an inverse correlation between sI and sH, suggesting that the sI structure is replaced by sH. Meanwhile, the Raman analysis demonstrated that although the 12-hedra of sI are retained, the 14-hedra are replaced sequentially by additional 12-hedra, modified 12-hedra, and 20-hedra cages of sH. With the sH to filled-ice Ih transition at 1.8 GPa, both the XRD and Raman data showed that this occurs through a sudden collapse of the sH structure and subsequent release of solid and fluid methane that is gradually incorporated into the filled-ice Ih to complete its structure. This therefore represents a typical reconstructive transition mechanism.
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