Cage Occupancy of Hydrogen in Carbon Dioxide, Ethane, Cyclopropane, and Propane Hydrates

The Open Thermodynamics Journal Pub Date : 2008-02-11 DOI:10.2174/1874396X00802010001

T. Sugahara, Hiroki Mori, J. Sakamoto, S. Hashimoto, K. Ogata, K. Ohgaki

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引用次数: 27

Abstract

We have already reported the cage unoccupancy of hydrogen in the CO2 hydrate from the Raman spectroscopic analysis and the thermodynamic analysis using Soave Redlich Kwong equation of state. On the other hand, at the low temperatures, Kim and Lee (Journal of American Chemical Society, vol. 127, pp. 9996-9997, Jul. 2005) claimed that hydrogen is enclathrated in the CO2 hydrate. In the present study, the cage unoccupancy of hydrogen in the CO2 hydrate was reconfirmed clearly by in situ Raman spectroscopy for single crystal of gas hydrates. Isothermal phase equilibria (pressure composition) and Raman spectra for three ternary systems of hydrogen + hydrocarbon (ethane, cyclopropane, propane) + water with same experimental procedures as hydrogen + CO2 + water system were measured at 276.1 K in the pressure range up to 5 MPa. In addition, the released gas from hydrates was analyzed to confirm the occupancy or unoccupancy of hydrogen at the temperature. All analyses arrive at the single conclusion that hydrogen is enclathrated in only propane hydrate under the present experimental conditions.

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氢气在二氧化碳、乙烷、环丙烷和丙烷水合物中的笼型占有

我们已经从拉曼光谱分析和Soave Redlich Kwong状态方程的热力学分析中报道了CO2水合物中氢的笼状空位。另一方面，在低温下，Kim和Lee (Journal of American Chemical Society, vol. 127, pp. 9996-9997, july . 2005)声称氢被包裹在CO2水合物中。在本研究中，利用气体水合物单晶的原位拉曼光谱再次清楚地证实了CO2水合物中氢的笼状空占现象。采用与氢+ CO2 +水体系相同的实验方法，在276.1 K温度下，在5 MPa压力范围内测量了氢+烃(乙烷、环丙烷、丙烷)+水三元体系的等温相平衡(压力组成)和拉曼光谱。此外，对水合物释放的气体进行了分析，以确定在该温度下氢气的占用或不占用。所有的分析都得出一个单一的结论，即在目前的实验条件下，氢只在丙烷水合物中被包合。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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The Open Thermodynamics Journal

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