Kitami Institute of Technology, 165 Koen-cho, Kitami, 090-8507, Japan.
Limnological Institute, SB RAS, 3 Ulan-Batorskaya St, Irkutsk, Russia, 664033.
Sci Rep. 2020 Sep 8;10(1):14747. doi: 10.1038/s41598-020-71410-2.
We reported the characteristics of hydrate-bound hydrocarbons in lake-bottom sediments at the Kedr mud volcano in Lake Baikal. Twenty hydrate-bearing sediment cores were retrieved, and methane-stable isotopes of hydrate-bound gases (δC and δH of - 47.8‰ to - 44.0‰ V-PDB and - 280.5‰ to - 272.8‰ V-SMOW, respectively) indicated their thermogenic origin accompanied with secondary microbial methane. Powder X-ray diffraction patterns of the crystals and molecular composition of the hydrate-bound gases suggested that structure II crystals showed a high concentration of ethane (around 14% of hydrate-bound hydrocarbons), whereas structure I crystals showed a relatively low concentration of ethane (2-5% of hydrate-bound hydrocarbons). These different crystallographic structures comprised complicated layers in the sub-lacustrine sediment, suggesting that the gas hydrates partly dissociate, concentrate ethane and form structure II crystals. We concluded that a high concentration of thermogenic ethane primarily controls the crystallographic structure of gas hydrates and that propane, iso-butane (2-methylpropane) and neopentane (2,2-dimethylpropane) are encaged into crystals in the re-crystallisation process.
我们报道了贝加尔湖凯德尔泥火山湖底沉积物中结合水合物的烃类特征。共采集了 20 个含天然气水合物的沉积物岩芯,水合物中气体的甲烷稳定同位素(δC 为-47.8‰至-44.0‰ V-PDB,δH 为-280.5‰至-272.8‰ V-SMOW)表明其具有热成因特征,并伴有次生微生物甲烷。晶体的粉末 X 射线衍射图谱和水合物结合气体的分子组成表明,II 型晶体表现出高浓度的乙烷(约占水合物结合烃类的 14%),而 I 型晶体表现出相对较低浓度的乙烷(占水合物结合烃类的 2-5%)。这些不同的晶体结构在亚湖底沉积物中组成了复杂的层状结构,表明气体水合物部分分解,浓缩乙烷并形成 II 型晶体。我们得出结论,高浓度的热成因乙烷主要控制着天然气水合物的晶体结构,而丙烷、异丁烷(2-甲基丙烷)和新戊烷(2,2-二甲基丙烷)在再结晶过程中被包裹在晶体中。