Phase changes of CO2 hydrate under high pressure and low temperature (original) (raw)
Research Article| September 29 2010
1Geodynamics Research Center,
Ehime University
, Matsuyama, Ehime 790-8577,
Japan
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2Geochemical Research Center,
Tokyo University
, Bunkyo-ku, Tokyo 113-0033,
Japan
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1Geodynamics Research Center,
Ehime University
, Matsuyama, Ehime 790-8577,
Japan
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3
National Institute of Advanced Industrial Science and Technology
, Tsukuba, Ibaraki 305-8569,
Japan
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3
National Institute of Advanced Industrial Science and Technology
, Tsukuba, Ibaraki 305-8569,
Japan
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4Institute for Solid State Physics,
Tokyo University
, Kashiwa, Chiba 277-8581,
Japan
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J. Chem. Phys. 133, 124511 (2010)
High pressure and low temperature experiments with CO2 hydrate were performed using diamond anvil cells and a helium-refrigeration cryostat in the pressure and temperature range of 0.2–3.0 GPa and 280–80 K, respectively. In situ x-ray diffractometry revealed that the phase boundary between CO2 hydrate and water+CO2 extended below the 280 K reported previously, toward a higher pressure and low temperature region. The results also showed the existence of a new high pressure phase above approximately 0.6 GPa and below 1.0 GPa at which the hydrate decomposed to dry ice and ice VI. In addition, in the lower temperature region of structure I, a small and abrupt lattice expansion was observed at approximately 210 K with decreasing temperature under fixed pressures. The expansion was accompanied by a release of water content from the sI structure as ice Ih, which indicates an increased cage occupancy. A similar lattice expansion was also described in another clathrate, SiO2 clathrate, under high pressure. Such expansion with increasing cage occupancy might be a common manner to stabilize the clathrate structures under high pressure and low temperature.
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