TY - JOUR

T1 - Influence of N₂ on Formation Conditions and Guest Distribution of Mixed CO₂ + CH₄ Gas Hydrates

AU - Belosludov, Vladimir R.

AU - Bozhko, Yulia Yu

AU - Subbotin, Oleg S.

AU - Belosludov, Rodion V.

AU - Zhdanov, Ravil K.

AU - Gets, Kirill V.

AU - Kawazoe, Yoshiyuki

N1 - Publisher Copyright: © 2018 by the authors.

PY - 2018/12/15

Y1 - 2018/12/15

N2 - In this contribution, a method based on a solid solution theory of clathrate hydrate for multiple cage occupancy, host lattice relaxation, and guest-guest interactions is presented to estimate hydrate formation conditions of binary and ternary gas mixtures. We performed molecular modeling of the structure, guest distribution, and hydrate formation conditions for the CO₂ + CH₄ and CO₂ + CH₄ + N₂ gas hydrates. In all considered systems with and without N₂, at high and medium content of CO₂ in the gas phase, we found that CO₂ was more favorable in occupying clathrate hydrate cavities than CH₄ or N₂. The addition of N₂ to the gas phase increased the ratio concentration of CO₂ in comparison with the concentration of CH₄ in clathrate hydrates and made gas replacement more effective. The mole fraction of CO₂ in the CO₂ + CH₄ + N₂ gas hydrate rapidly increased with the growth of its content in the gas phase, and the formation pressure of the CO₂ + CH₄ + N₂ gas hydrate rose in comparison to the formation pressure of the CO₂ + CH₄ gas hydrate. The obtained results agreed with the known experimental data for simple CH₄ and CO₂ gas hydrates and the mixed CO₂ + CH₄ gas hydrate.

AB - In this contribution, a method based on a solid solution theory of clathrate hydrate for multiple cage occupancy, host lattice relaxation, and guest-guest interactions is presented to estimate hydrate formation conditions of binary and ternary gas mixtures. We performed molecular modeling of the structure, guest distribution, and hydrate formation conditions for the CO₂ + CH₄ and CO₂ + CH₄ + N₂ gas hydrates. In all considered systems with and without N₂, at high and medium content of CO₂ in the gas phase, we found that CO₂ was more favorable in occupying clathrate hydrate cavities than CH₄ or N₂. The addition of N₂ to the gas phase increased the ratio concentration of CO₂ in comparison with the concentration of CH₄ in clathrate hydrates and made gas replacement more effective. The mole fraction of CO₂ in the CO₂ + CH₄ + N₂ gas hydrate rapidly increased with the growth of its content in the gas phase, and the formation pressure of the CO₂ + CH₄ + N₂ gas hydrate rose in comparison to the formation pressure of the CO₂ + CH₄ gas hydrate. The obtained results agreed with the known experimental data for simple CH₄ and CO₂ gas hydrates and the mixed CO₂ + CH₄ gas hydrate.

KW - Computer modeling

KW - Gas separation

KW - Greenhouse gases

KW - Lattice dynamic

KW - Mixed gas hydrates

KW - Nitrogen/chemistry

KW - Computer Simulation

KW - Carbon Dioxide/chemistry

KW - Ice

KW - Water/chemistry

KW - Pressure

KW - Methane/chemistry

KW - greenhouse gases

KW - STABILITY

KW - PHASE-EQUILIBRIA

KW - RECOVERY

KW - METHANE

KW - N-2-CLATHRATE

KW - WATER

KW - STORAGE

KW - computer modeling

KW - lattice dynamic

KW - mixed gas hydrates

KW - gas separation

KW - CLATHRATE HYDRATE FORMATION

KW - GAS

KW - CARBON-DIOXIDE

UR - http://www.scopus.com/inward/record.url?scp=85058733302&partnerID=8YFLogxK

U2 - 10.3390/molecules23123336

DO - 10.3390/molecules23123336

M3 - Article

C2 - 30558336

AN - SCOPUS:85058733302

VL - 23

JO - Molecules

JF - Molecules

SN - 1420-3049

IS - 12

M1 - 3336

ER -