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Replacement of CH_4 in the hydrate by use of liquid CO_2

机译：通过使用液态CO_2替代水合物中的CH_4

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摘要

The dynamics of CH_4 replacement in the CH_4 hydrate with saturated liquid CO_2 at 273.2K was measured with a high pressure optical cell. The results showed that CH_4 in the hydrate gradually moved to the liquid CO_2 phase while CO_2 in the liquid phase penetrated into the hydrate from the quantitative analysis. The decomposing process of the CH_4 hydrate during the replacement was analyzed with in situ Raman spectroscopy, which allowed us to distinguish the cage structure of the CH_4 hydrate and discuss the microscopic view of the replacement in the hydrate. It was found that the decomposition of the medium cage (M-cage) in the CH_4 hydrate proceeded faster than that of the small cage (S-cage). The observed rate difference could be related to the stability of the S-cage in the CH_4 hydrate or the re-formation tendency of CH_4 and water molecules in the S-cage after decomposing the hydrate structure, whereas the guest molecule exchange of CH_4 with CO_2 could occur in the M-cage. Based on the experimental data, we developed a kinetic model for calculation of the CH_4 remaining in the hydrate considering the decomposition rate difference between the M-cage and S-cage in the CH_4 hydrate. The results indicate that the driving force could be the fugacity difference between the fluid phase and the hydrate phase for the replacement process.
机译：用高压光学电池测量了在273.2K下用饱和液态CO_2在CH_4水合物中CH_4置换的动力学。结果表明，定量分析表明，水合物中的CH_4逐渐移至液相CO_2中，而液相中的CO_2则渗入水合物中。用原位拉曼光谱分析了置换过程中CH_4水合物的分解过程，这使我们能够区分CH_4水合物的笼结构，并讨论了水合物中置换的微观视图。发现CH_4水合物中的中型笼（M型笼）的分解过程比小型笼（S型笼）的分解过程快。观察到的速率差异可能与CH_4水合物中S-笼的稳定性或分解水合物结构后CH_4和S-笼中水分子的重新形成趋势有关，而CH_4与CO_2的客体分子交换可能发生在M型笼中。基于实验数据，考虑到CH_4水合物中M笼和S笼之间的分解速率差异，我们开发了动力学模型来计算水合物中残留的CH_4。结果表明，驱动力可能是置换过程中液相和水合物相的逸度差。

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