Abstract

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 (δ13C and δ2H 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.

Highlights

  • IntroductionPowder 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)

  • We reported the characteristics of hydrate-bound hydrocarbons in lake-bottom sediments at the Kedr mud volcano in Lake Baikal

  • Sassen et al.[8] studied the gas hydrates retrieved at the Gulf of Mexico and found that they are high in ­C2, ­C3 and butane ­(C4) but exclude isopentane (i-C5, 2-methylbutane), because the crystal structure II cannot encage such large guest molecules

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Summary

Introduction

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. Sassen et al.[8] studied the gas hydrates retrieved at the Gulf of Mexico and found that they are high in ­C2, ­C3 and butane ­(C4) but exclude isopentane (i-C5, 2-methylbutane), because the crystal structure II (sII) cannot encage such large guest molecules. Because ­C2 is prone to be encaged in the hydrate phase rather than ­C1, ­C2 can be concentrated into the hydrate during the re-crystallisation process with C­ 2-rich sII ­forming[18]

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