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RESEARCH ON COUPLED RELATIONSHIP BETWEEN HYDRATION NUMBER WITH RAMAN SPECTRUM

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【Author】 LEI Huaiyan~(1,2), LIU Zhihong~3, FAN Shuanshi~2, XU Maoquan~1 and GUAN Baocong~1 (~1 Institute of Oceanography and Environment, Xiamen University; ~2 Guangzhou Institute of Energy Conversion, CAS; ~3 Institute of Chemical Engineering, Xiamen University)

【摘要】 <正> As we know, there are three structures-sⅠ, sⅡ, and sH, with hydrocarbonate gas hydrate. Because of those special structures characteristics and potentail large fossil energy resource, gas hydrate play an important role in natural carbonate cycle system. In this paper, CH4, CO2, C3H8, and CH4+CO2 system have been experimental performed in order to model hydrate formation and discomposition and to obtain hydrate stability conditions of tempreature and pressure. The results from laboratory using Raman spectra show that Raman spectrascopy is a effective tool to identify hydrate structure. Raman spectra of clathrate hydrate guest molecules are presented for two structure (sⅠ and sⅡ) in the following systems: CH4, CO2, C3H8. Relatively occupancy of CH4 in the large and small cavities of sⅠ were determined by deconvoluting the v1 symmetric bands, resulting in hydration numbers of 6.04±0.03. The freqyuency of the v1 bands for CH4 in structures Ⅰ and Ⅱ differ statistically. The large cavities were measured to be almost fully occupied by CH4 and CO2, whereas only a small fraction of the small cavities are occupied by CH4. No CO2 was found in the small cavities.

【Abstract】 As we know, there are three structures-sⅠ, sⅡ, and sH, with hydrocarbonate gas hydrate. Because of those special structures characteristics and potentail large fossil energy resource, gas hydrate play an important role in natural carbonate cycle system. In this paper, CH4, CO2, C3H8, and CH4+CO2 system have been experimental performed in order to model hydrate formation and discomposition and to obtain hydrate stability conditions of tempreature and pressure. The results from laboratory using Raman spectra show that Raman spectrascopy is a effective tool to identify hydrate structure. Raman spectra of clathrate hydrate guest molecules are presented for two structure (sⅠ and sⅡ) in the following systems: CH4, CO2, C3H8. Relatively occupancy of CH4 in the large and small cavities of sⅠ were determined by deconvoluting the v1 symmetric bands, resulting in hydration numbers of 6.04±0.03. The freqyuency of the v1 bands for CH4 in structures Ⅰ and Ⅱ differ statistically. The large cavities were measured to be almost fully occupied by CH4 and CO2, whereas only a small fraction of the small cavities are occupied by CH4. No CO2 was found in the small cavities.

【基金】 Supported by the National Natural Science Foundation of China (No. 49973024, 40272066);211 Projects of Xiamen University.
  • 【文献出处】 化工学报 ,Journal fo Chemical Industry and Engineering , 编辑部邮箱 ,2003年S1期
  • 【分类号】O657.3;O621.3
  • 【下载频次】19
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