Crystal Growth of Clathrate Hydrate in Liquid Water Saturated with a Simulated Natural Gas
Crystal Growth of Clathrate Hydrate in Liquid Water Saturated with a Simulated Natural Gas
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DOI：
10.1021/cg2005024
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发表时间：
2011-06
影响因子：
3.8
通讯作者：
Sho Watanabe;Kota Saito;R. Ohmura
中科院分区：
文献类型：
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作者：
Sho Watanabe;Kota Saito;R. Ohmura
本文报道了用模拟天然气（甲烷+乙烷+丙烷混合气）预饱和的液态水中笼形水合物晶体的形成和生长过程。甲烷+乙烷+丙烷气体混合物的组成为（i）90：7：3，（ii）94.1：5.8：0.1，和（iii）99.47：0.51：0.02摩尔比。混合气体和液态水之间首先形成水合物膜，然后在液态水相中生长水合物晶体。在液态水中生长的水合物晶体的形貌随系统过冷度ΔTsub的变化而明显变化。当ΔTsub小于0.7K时，在液态水中没有观察到水合物晶体的生长。在107 K ~ 12 K时，多角形晶体被树枝状晶体所取代.用所有三种气体混合物观察到形态的这些变化。结果表明，在摩尔比为99.47：0.51：0.02的混合气体体系中，产物的形貌发生了变化。
This paper reports the visual observation of the formation and growth of clathrate hydrate crystals in liquid water presaturated with a simulated natural gas (methane + ethane + propane mixture). The compositions of the methane + ethane + propane gas mixtures are (i) 90:7:3, (ii) 94.1:5.8:0.1, and (iii) 99.47:0.51:0.02 in molar ratio. A hydrate film first formed to intervene between the mixed gas and liquid water, and then hydrate crystals grew in the liquid water phase. The morphology of hydrate crystals grown in liquid water distinctly varied depending on the system subcooling ΔTsub. When ΔTsub is smaller than ∼7 K, hydrate crystal growth in liquid water was not observed. At ∼7 K ∼12 K, polygonal crystals were replaced by dendritic crystals. These changes in morphology were observed with all three gas mixtures. It was found that the morphology in the system with mixed gas of the molar ratio 99.47:0.51:0.02 was differen...