Clathrate Hydrate Formation from a Hydrocarbon Gas Mixture: Evolution of Gas-Phase Composition in a Hydrate-Forming Reactor
Clathrate Hydrate Formation from a Hydrocarbon Gas Mixture: Evolution of Gas-Phase Composition in a Hydrate-Forming Reactor
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DOI：
10.1021/ef100950p
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发表时间：
2010-12-01
期刊：
影响因子：
5.3
通讯作者：
Mori, Yasuhiko H.
中科院分区：
文献类型：
--
作者：
Kondo, Wataru;Ogawa, Hiroyuki;Mori, Yasuhiko H.
从模型天然气，即，在恒定压力下，实验研究了摩尔比为90：7：3的甲烷、乙烷和丙烷的混合物，重点是在每个半间歇水合物形成操作期间水合物形成反应器内气相组成的演变。在以前的研究中（小林，T.; Imura，N.;奥穆拉河; Mori，Y. H. Energy Fuels 2007，21，545-553），我们测量了在水合物形成开始后的初始时期（最多近似3小时）期间气相组成的演变，其中所形成的水合物中的气体吸收总量被限制为反应器中初始包含的气体量的0.8倍。这项研究扩展了以前的研究，这样我们就可以观察到气相组成的演变更长的时间（高达50小时），直到一个准稳态内建立一个新建造的气体鼓泡型反应器配备了一个气相混合搅拌器，使气体采样从混合良好的气体在特定的时间。连续采样的气体的气相色谱分析显示甲烷馏分的单调增加和乙烷和丙烷馏分的减少，直到建立一个准稳态时，在形成的水合物中的气体吸收的总量接近最初包含在反应器中的气体的量。这些实验结果与我们最近报道的基于热力学模拟方案的预测相当吻合（Ogawa，H.; Imura，N.; Miyoshi，T.; Ohmura，R.; Mori，Y. H. Energy Fuels 2009，23，849-856）。
The clathrate hydrate formation from a model natural gas, i.e., a mixture of methane, ethane, and propane in a 90:7:3 molar ratio, under constant pressure was experimentally investigated, focusing on the evolution of the gas-phase composition inside the hydrate-forming reactor during each semi-batch hydrate-forming operation. In a previous study (Kobayashi, T.; Imura, N.; Ohmura, R.; Mori, Y. H. Energy Fuels 2007, 21, 545-553), we measured the evolution of the gas-phase composition during the initial period (up to similar to 3 h) following the inception of hydrate formation, in which the total amount of gas uptake in the formed hydrates was limited to 0.8 times the amount of gas initially contained in the reactor. This study extended the previous study, such that we could observe the evolution of the gas-phase composition for a much longer time (up to similar to 50 h) until a quasi-steady state was established inside a newly constructed gas-bubbling-type reactor equipped with a gas-phase-mixing stirrer that enabled the gas sampling from the well-mixed gas at specific times. The gas-chromatographic analyses of the continually sampled gas revealed a monotonic increase in the methane fraction and decreases in the ethane and propane fractions until a quasi-steady state was established when the total amount of gas uptake in the formed hydrates approached the amount of gas initially contained in the reactor. These experimental results are in reasonably good agreement with predictions based on the thermodynamic simulation scheme that we recently reported (Ogawa, H.; Imura, N.; Miyoshi, T.; Ohmura, R.; Mori, Y. H. Energy Fuels 2009, 23, 849-856).