Crystal growth of clathrate hydrate in liquid water saturated with a simulated natural gas

Sho Watanabe, Kota Saito, Ryo Ohmura

Research output: Contribution to journalArticle

28 Citations (Scopus)

Abstract

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 < δTsub < ∼12 K, hydrate crystals with polygonal morphology were observed. At δTsub > ∼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 different from those of the other two systems. We also observed the hydrate crystals floating to the hydrate film from liquid water phase. Floating crystals formed in the bulk of liquid water, attached the hydrate film, and then continued to grow in liquid water. The morphology of floating crystals varied with δTsub and the gas composition.

Original languageEnglish
Pages (from-to)3235-3242
Number of pages8
JournalCrystal Growth and Design
Volume11
Issue number7
DOIs
Publication statusPublished - 2011 Jul 6

Fingerprint

clathrates
natural gas
Crystallization
Hydrates
Crystal growth
hydrates
crystal growth
Natural gas
Crystals
Water
Liquids
liquids
water
crystals
floating
Propane
Ethane
Gases
Methane
Gas mixtures

ASJC Scopus subject areas

  • Chemistry(all)
  • Materials Science(all)
  • Condensed Matter Physics

Cite this

Crystal growth of clathrate hydrate in liquid water saturated with a simulated natural gas. / Watanabe, Sho; Saito, Kota; Ohmura, Ryo.

In: Crystal Growth and Design, Vol. 11, No. 7, 06.07.2011, p. 3235-3242.

Research output: Contribution to journalArticle

@article{79c0c10af92a4e6c95fa7c3ad93c44ac,
title = "Crystal growth of clathrate hydrate in liquid water saturated with a simulated natural gas",
abstract = "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 < δTsub < ∼12 K, hydrate crystals with polygonal morphology were observed. At δTsub > ∼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 different from those of the other two systems. We also observed the hydrate crystals floating to the hydrate film from liquid water phase. Floating crystals formed in the bulk of liquid water, attached the hydrate film, and then continued to grow in liquid water. The morphology of floating crystals varied with δTsub and the gas composition.",
author = "Sho Watanabe and Kota Saito and Ryo Ohmura",
year = "2011",
month = "7",
day = "6",
doi = "10.1021/cg2005024",
language = "English",
volume = "11",
pages = "3235--3242",
journal = "Crystal Growth and Design",
issn = "1528-7483",
publisher = "American Chemical Society",
number = "7",

}

TY - JOUR

T1 - Crystal growth of clathrate hydrate in liquid water saturated with a simulated natural gas

AU - Watanabe, Sho

AU - Saito, Kota

AU - Ohmura, Ryo

PY - 2011/7/6

Y1 - 2011/7/6

N2 - 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 < δTsub < ∼12 K, hydrate crystals with polygonal morphology were observed. At δTsub > ∼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 different from those of the other two systems. We also observed the hydrate crystals floating to the hydrate film from liquid water phase. Floating crystals formed in the bulk of liquid water, attached the hydrate film, and then continued to grow in liquid water. The morphology of floating crystals varied with δTsub and the gas composition.

AB - 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 < δTsub < ∼12 K, hydrate crystals with polygonal morphology were observed. At δTsub > ∼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 different from those of the other two systems. We also observed the hydrate crystals floating to the hydrate film from liquid water phase. Floating crystals formed in the bulk of liquid water, attached the hydrate film, and then continued to grow in liquid water. The morphology of floating crystals varied with δTsub and the gas composition.

UR - http://www.scopus.com/inward/record.url?scp=79960055336&partnerID=8YFLogxK

UR - http://www.scopus.com/inward/citedby.url?scp=79960055336&partnerID=8YFLogxK

U2 - 10.1021/cg2005024

DO - 10.1021/cg2005024

M3 - Article

AN - SCOPUS:79960055336

VL - 11

SP - 3235

EP - 3242

JO - Crystal Growth and Design

JF - Crystal Growth and Design

SN - 1528-7483

IS - 7

ER -