Multiple adsorption resistance model for constituent molecular effects in hydrogen clathration kinetics in clathrate hydrate particles

Hiroyuki Komatsu; Masaki Ota; Yoshiyuki Sato; Masaru Watanabe; Richard L. Smith

doi:10.1016/j.ces.2014.01.001

Multiple adsorption resistance model for constituent molecular effects in hydrogen clathration kinetics in clathrate hydrate particles

Hiroyuki Komatsu, Masaki Ota, Yoshiyuki Sato, Masaru Watanabe, Richard L. Smith

Research output: Contribution to journal › Article › peer-review

3 Citations (Scopus)

Abstract

Adsorption rates are reported for H₂-tetrahydrofuran (THF), H₂-THF (D₂O), H₂-THF-d8, H₂-furan, H₂-cyclopentane (CP) and H₂-tetrahydrothiophene (THT) binary clathrate hydrates at temperatures of 265-273K and pressures of 4-10MPa. Adsorption rates of H₂-furan and H₂-6.8mol% THF binary clathrate hydrates were the fastest among these binary clathrate hydrates. The lattice constant of hydrates were determined to analyze the adsorption data with a newly proposed multiple adsorption resistance (MAR) model. The effect of the non-included additive guest molecule on hydrogen adsorption rate was important because they promoted formation of pores and grain boundaries when hydrate particles formed. Activation energies, δEDa, for H₂ diffusion into clathrate hydrates calculated from the Arrhenius plots depended on the hydrate guest additive and were determined to be: 18.0kJ/mol (6.2mol% THF), 30.7kJ/mol (5.6mol% THF), and 100kJ/mol (cyclopentane). Based on the δEDa values, H₂ diffusion pathway in hydrate particles depends on the clathrate hydrate formation process and the interactions between guest additive molecule and the host molecule.

Original language	English
Pages (from-to)	270-282
Number of pages	13
Journal	Chemical Engineering Science
Volume	108
DOIs	https://doi.org/10.1016/j.ces.2014.01.001
Publication status	Published - 2014 Apr 28

Keywords

Adsorption
Clathrate hydrates
Diffusion
Hydrogen
Kinetic model
Lattice constant

ASJC Scopus subject areas

Chemistry(all)
Chemical Engineering(all)
Industrial and Manufacturing Engineering

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10.1016/j.ces.2014.01.001

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title = "Multiple adsorption resistance model for constituent molecular effects in hydrogen clathration kinetics in clathrate hydrate particles",

abstract = "Adsorption rates are reported for H2-tetrahydrofuran (THF), H2-THF (D2O), H2-THF-d8, H2-furan, H2-cyclopentane (CP) and H2-tetrahydrothiophene (THT) binary clathrate hydrates at temperatures of 265-273K and pressures of 4-10MPa. Adsorption rates of H2-furan and H2-6.8mol% THF binary clathrate hydrates were the fastest among these binary clathrate hydrates. The lattice constant of hydrates were determined to analyze the adsorption data with a newly proposed multiple adsorption resistance (MAR) model. The effect of the non-included additive guest molecule on hydrogen adsorption rate was important because they promoted formation of pores and grain boundaries when hydrate particles formed. Activation energies, δEDa, for H2 diffusion into clathrate hydrates calculated from the Arrhenius plots depended on the hydrate guest additive and were determined to be: 18.0kJ/mol (6.2mol% THF), 30.7kJ/mol (5.6mol% THF), and 100kJ/mol (cyclopentane). Based on the δEDa values, H2 diffusion pathway in hydrate particles depends on the clathrate hydrate formation process and the interactions between guest additive molecule and the host molecule.",

keywords = "Adsorption, Clathrate hydrates, Diffusion, Hydrogen, Kinetic model, Lattice constant",

author = "Hiroyuki Komatsu and Masaki Ota and Yoshiyuki Sato and Masaru Watanabe and Smith, {Richard L.}",

note = "Funding Information: The authors wish to acknowledge the financial support of Japan Society for Promotion of Science (JSPS) and the experimental support of Dr. Satoshi Takeya (National Institute of Advanced Industrial Science and Technology). ",

year = "2014",

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day = "28",

doi = "10.1016/j.ces.2014.01.001",

language = "English",

volume = "108",

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journal = "Chemical Engineering Science",

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TY - JOUR

T1 - Multiple adsorption resistance model for constituent molecular effects in hydrogen clathration kinetics in clathrate hydrate particles

AU - Komatsu, Hiroyuki

AU - Ota, Masaki

AU - Sato, Yoshiyuki

AU - Watanabe, Masaru

AU - Smith, Richard L.

N1 - Funding Information: The authors wish to acknowledge the financial support of Japan Society for Promotion of Science (JSPS) and the experimental support of Dr. Satoshi Takeya (National Institute of Advanced Industrial Science and Technology).

PY - 2014/4/28

Y1 - 2014/4/28

N2 - Adsorption rates are reported for H2-tetrahydrofuran (THF), H2-THF (D2O), H2-THF-d8, H2-furan, H2-cyclopentane (CP) and H2-tetrahydrothiophene (THT) binary clathrate hydrates at temperatures of 265-273K and pressures of 4-10MPa. Adsorption rates of H2-furan and H2-6.8mol% THF binary clathrate hydrates were the fastest among these binary clathrate hydrates. The lattice constant of hydrates were determined to analyze the adsorption data with a newly proposed multiple adsorption resistance (MAR) model. The effect of the non-included additive guest molecule on hydrogen adsorption rate was important because they promoted formation of pores and grain boundaries when hydrate particles formed. Activation energies, δEDa, for H2 diffusion into clathrate hydrates calculated from the Arrhenius plots depended on the hydrate guest additive and were determined to be: 18.0kJ/mol (6.2mol% THF), 30.7kJ/mol (5.6mol% THF), and 100kJ/mol (cyclopentane). Based on the δEDa values, H2 diffusion pathway in hydrate particles depends on the clathrate hydrate formation process and the interactions between guest additive molecule and the host molecule.

AB - Adsorption rates are reported for H2-tetrahydrofuran (THF), H2-THF (D2O), H2-THF-d8, H2-furan, H2-cyclopentane (CP) and H2-tetrahydrothiophene (THT) binary clathrate hydrates at temperatures of 265-273K and pressures of 4-10MPa. Adsorption rates of H2-furan and H2-6.8mol% THF binary clathrate hydrates were the fastest among these binary clathrate hydrates. The lattice constant of hydrates were determined to analyze the adsorption data with a newly proposed multiple adsorption resistance (MAR) model. The effect of the non-included additive guest molecule on hydrogen adsorption rate was important because they promoted formation of pores and grain boundaries when hydrate particles formed. Activation energies, δEDa, for H2 diffusion into clathrate hydrates calculated from the Arrhenius plots depended on the hydrate guest additive and were determined to be: 18.0kJ/mol (6.2mol% THF), 30.7kJ/mol (5.6mol% THF), and 100kJ/mol (cyclopentane). Based on the δEDa values, H2 diffusion pathway in hydrate particles depends on the clathrate hydrate formation process and the interactions between guest additive molecule and the host molecule.

KW - Adsorption

KW - Clathrate hydrates

KW - Diffusion

KW - Hydrogen

KW - Kinetic model

KW - Lattice constant

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DO - 10.1016/j.ces.2014.01.001

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EP - 282

JO - Chemical Engineering Science

JF - Chemical Engineering Science

ER -

Multiple adsorption resistance model for constituent molecular effects in hydrogen clathration kinetics in clathrate hydrate particles

Abstract

Keywords

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