Lu Hailong, Seo Yu-taek, Lee Jong-won, Moudrakovski Igor, Ripmeester John A, Chapman N Ross, Coffin Richard B, Gardner Graeme, Pohlman John
Steacie Institute for Molecular Sciences, National Research Council of Canada Ottawa, Ontario, Canada K1A 0R6.
Nature. 2007 Jan 18;445(7125):303-6. doi: 10.1038/nature05463.
Natural gas hydrates are a potential source of energy and may play a role in climate change and geological hazards. Most natural gas hydrate appears to be in the form of 'structure I', with methane as the trapped guest molecule, although 'structure II' hydrate has also been identified, with guest molecules such as isobutane and propane, as well as lighter hydrocarbons. A third hydrate structure, 'structure H', which is capable of trapping larger guest molecules, has been produced in the laboratory, but it has not been confirmed that it occurs in the natural environment. Here we characterize the structure, gas content and composition, and distribution of guest molecules in a complex natural hydrate sample recovered from Barkley canyon, on the northern Cascadia margin. We show that the sample contains structure H hydrate, and thus provides direct evidence for the natural occurrence of this hydrate structure. The structure H hydrate is intimately associated with structure II hydrate, and the two structures contain more than 13 different hydrocarbon guest molecules. We also demonstrate that the stability field of the complex gas hydrate lies between those of structure II and structure H hydrates, indicating that this form of hydrate is more stable than structure I and may thus potentially be found in a wider pressure-temperature regime than can methane hydrate deposits.
天然气水合物是一种潜在的能源,可能在气候变化和地质灾害中发挥作用。大多数天然气水合物似乎呈“结构 I”形式,其中甲烷作为被捕获的客体分子,不过也已鉴定出“结构 II”水合物,其客体分子包括异丁烷和丙烷等以及较轻的碳氢化合物。第三种水合物结构“结构 H”能够捕获更大的客体分子,已在实验室中制备出来,但尚未证实其在自然环境中存在。在此,我们对从卡斯卡迪亚北部边缘的巴克利峡谷采集的复杂天然水合物样品的结构、气体含量与组成以及客体分子的分布进行了表征。我们表明该样品含有结构 H 水合物,从而为这种水合物结构的天然存在提供了直接证据。结构 H 水合物与结构 II 水合物紧密相关,且这两种结构包含 13 种以上不同的碳氢化合物客体分子。我们还证明了这种复杂气体水合物的稳定域介于结构 II 和结构 H 水合物的稳定域之间,这表明这种形式的水合物比结构 I 更稳定,因此可能在比甲烷水合物矿床更宽的压力 - 温度范围内被发现。