Anomalously Preserved Clathrate Hydrate of Natural Gas in Pellet Form at 253 K

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Abstract

Storage of natural gas (NG) is required for a range of applications. In this study, we succeeded to maintain NG within water cages of anomalously preserved NG hydrate crystal for more than three weeks under thermodynamically unstable conditions at 253 K and atmospheric pressure. This anomalous preservation phenomenon of NG hydrate pellet was measured quantitatively by powder X-ray diffraction and gas chromatography as well as measuring the change in weight caused by hydrate dissociation. In addition, two different types of phase contrast X-ray imaging techniques, X-ray interferometric imaging and diffraction enhanced imaging, also revealed that the NG hydrate was maintained inside the pellet. Also, scanning electron microscopy showed that the outer ice layer formed contained many pores while the internal microstructure of NG hydrate pellet was dense without pores. These experimental results suggest that formation of the outer ice layer may not be related to anomalous preservation of NG hydrate, but formation of pore space may cause hydrate dissociation.

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