Clathrate hydrate crystal growth in liquid water saturated with a hydrate-forming substance: variations in crystal morphology

Ohmura, Ryo; Shimada, Wataru; Uchida, Tsutomu; Mori, Yasuhiko H.; Takeya, Satoshi; Nagao, Jiro; Minagawa, Hideki; Ebinuma, Takao; Narita, Hideo

doi:10.1080/14786430310001623542

Cited by 87 publications

(151 citation statements)

References 24 publications

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“…Investigations of the dominant factors in the formation and growth of clathrate hydrates have long been of scientific and industrial interest. Despite the fact that our understanding of hydrate formation from guest-water solutions has improved [9][10][11], much discussion still exists in the literature [12][13][14][15][16][17] about the dominant process controlling the hydrate-layer growth along the guest/liquid-water interface. Some previous studies [12][13][14] have suggested that the hydrate-layer growth is significantly affected by heat transfer.…”

Section: Introductionmentioning

confidence: 99%

“…In the present study, we first present the theoretical formulations representing the conjugate process of guest-in-water mass transfer and the hydrate-layer growth following to the previous study on the hydrate crystal growth into the liquid water saturated with a guest substance prior to the hydrate formation [15]. We have derived a dimensionless parameter representing the hydrate-layer growth rate.…”

Section: Introductionmentioning

confidence: 99%

“…The solubility x eq,int corresponds to the experimental system temperature T ex . As for the mathematical formulation of the conjugate process, we may follow on the previous study by Ohmura et al [15] on the hydrate crystal growth into the liquid-water. A similar analysis to the hydrate crystal growth at guest/liquid-water interface was performed.…”

Section: Introductionmentioning

confidence: 99%

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Correlation of the Growth Rate of the Hydrate Layer at a Guest/Liquid-Water Interface to Mass Transfer Resistance

Kishimoto¹,

Ohmura²

2012

Energies

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Growth rate of a hydrate layer at the guest/liquid-water interface is analyzed considering the conjugate process of the mass-transfer and hydrate crystal growth. Hydrate-layer growth rate data in the literature are often compiled according to the system subcooling (∆T ≡ T eq − T ex , where T eq is the equilibrium dissociation temperature of the hydrate and T ex is the system temperature), suggesting predominant heat transfer limitations. In this paper, we investigate how the existing data on hydrate-layer growth is better correlated to mass transfer of the guest species in liquid water in three-phase equilibrium with bulk guest fluid and hydrate. We have analyzed the conjugate processes of mass-transfer/hydrate-layer-growth following our previous study on the hydrate crystal growth into liquid water saturated with a guest substance. A dimensionless parameter representing the hydrate-layer growth rate is derived from the analysis. This analysis is based on the idea that the growth rate is controlled by the mass transfer of the hydrate-guest substance, dissolved in the bulk of liquid water, to the front of the growing hydrate-layer along the guest/water interface. The variations in the hydrate-layer growth rate observed in the previous studies are related to the dimensionless parameter.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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Correlation of the Growth Rate of the Hydrate Layer at a Guest/Liquid-Water Interface to Mass Transfer Resistance

Kishimoto¹,

Ohmura²

2012

Energies

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“…In the Kukuy K2 and Malenky-Malyutka areas, qu of the mud volcano samples is less than half for those of the reference sample at same depth. Here, the gas concentration in pore water of the mud volcano ground is possibly higher than the reference samples retrieved from the same areas, because a gas hydrate formation requires that water around gas hydrates is saturated by gas (e.g., Ohmura et al, 2004). Additionally, it is known that the strengths of soil containing gas bubble tend to be low (e.g., Wheeler, 1988).…”

Section: Onboard Test Resultsmentioning

confidence: 99%

“…In Photo 2(b), many voids (from 0.1 mm to 0.5 mm in diameter) were observed in the cut surface of the mud volcano core. Here, it is known that gas hydrate formation requires that water around the gas hydrate is saturated by gas (e.g., Ohmura et al, 2004). In addition, the high pressure and low temperature are required for higher saturation ratio of gas.…”

Section: Core Observation and Onboard Testsmentioning

confidence: 99%

The Soil Properties of Lake-Bottom Sediments in the Lake Baikal Gas Hydrate Province

Kataoka

Kawaguchi

Suzuki

2009

Soils and Foundations

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Salinity‐buffered methane hydrate formation and dissociation in gas‐rich systems

et al. 2015

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Methane hydrate formation and dissociation are buffered by salinity in a closed system. During hydrate formation, salt excluded from hydrate increases salinity, drives the system to three-phase (gas, water, and hydrate phases) equilibrium, and limits further hydrate formation and dissociation. We developed a zero-dimensional local thermodynamic equilibrium-based model to explain this concept. We demonstrated this concept by forming and melting methane hydrate from a partially brine-saturated sand sample in a controlled laboratory experiment by holding pressure constant (6.94 MPa) and changing temperature stepwise. The modeled methane gas consumptions and hydrate saturations agreed well with the experimental measurements after hydrate nucleation. Hydrate dissociation occurred synchronously with temperature increase. The exception to this behavior is that substantial subcooling (6.4°C in this study) was observed for hydrate nucleation. X-ray computed tomography scanning images showed that core-scale hydrate distribution was heterogeneous. This implied core-scale water and salt transport induced by hydrate formation. Bulk resistivity increased sharply with initial hydrate formation and then decreased as the hydrate ripened. This study reproduced the salinity-buffered hydrate behavior interpreted for natural gas-rich hydrate systems by allowing methane gas to freely enter/leave the sample in response to volume changes associated with hydrate formation and dissociation. It provides insights into observations made at the core scale and log scale of salinity elevation to three-phase equilibrium in natural hydrate systems.

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Clathrate hydrate crystal growth in liquid water saturated with a hydrate-forming substance: variations in crystal morphology

Cited by 87 publications

References 24 publications

Correlation of the Growth Rate of the Hydrate Layer at a Guest/Liquid-Water Interface to Mass Transfer Resistance

Correlation of the Growth Rate of the Hydrate Layer at a Guest/Liquid-Water Interface to Mass Transfer Resistance

The Soil Properties of Lake-Bottom Sediments in the Lake Baikal Gas Hydrate Province

Salinity‐buffered methane hydrate formation and dissociation in gas‐rich systems

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