Research output: Contribution to journal › Article › peer-review
Transformation of hydrogen bond network during CO2 clathrate hydrate dissociation. / Gets, Kirill; Belosludov, Vladimir; Zhdanov, Ravil et al.
In: Applied Surface Science, Vol. 499, 143644, 01.01.2020.Research output: Contribution to journal › Article › peer-review
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TY - JOUR
T1 - Transformation of hydrogen bond network during CO2 clathrate hydrate dissociation
AU - Gets, Kirill
AU - Belosludov, Vladimir
AU - Zhdanov, Ravil
AU - Bozhko, Yulia
AU - Belosludov, Rodion
AU - Subbotin, Oleg
AU - Marasanov, Nikita
AU - Kawazoe, Yoshiyuki
N1 - Publisher Copyright: © 2019 Elsevier B.V.
PY - 2020/1/1
Y1 - 2020/1/1
N2 - The kinetic process of the solid-liquid first-order phase transition of carbon dioxide CS-I hydrates with various cavity occupation ratios has been investigated in order to understand the framework of the H-bond network and the local structure of each water molecule. This includes the time dependent change in short-range order at temperatures close to the melting point and comparison with the hexagonal ice structure. Using the molecular dynamics method, dependencies of the internal energy of the studied systems on the time of heating were found. Jumps in the internal energy of solids in the range at 275–300 K indicate a phase transition. The study of the oxygen‑oxygen radial distribution and hydrogen‑oxygen‑oxygen mutual orientation angles between molecules detached at no >3.2 Å led to the determination of the H-bond coordination number for all molecules and the total number of H-bonds and showed instantaneous (<1 ns) reorganization of the short-range order of all molecules. Structural analysis of neighbor water molecule pairs showed ~10–15% decrease in the H-bond number after melting whereas all molecules form a single long-range H-bond network. Analysis of the H-bond network showed minor changes in the H-bond interaction energy at the solid-liquid phase transition.
AB - The kinetic process of the solid-liquid first-order phase transition of carbon dioxide CS-I hydrates with various cavity occupation ratios has been investigated in order to understand the framework of the H-bond network and the local structure of each water molecule. This includes the time dependent change in short-range order at temperatures close to the melting point and comparison with the hexagonal ice structure. Using the molecular dynamics method, dependencies of the internal energy of the studied systems on the time of heating were found. Jumps in the internal energy of solids in the range at 275–300 K indicate a phase transition. The study of the oxygen‑oxygen radial distribution and hydrogen‑oxygen‑oxygen mutual orientation angles between molecules detached at no >3.2 Å led to the determination of the H-bond coordination number for all molecules and the total number of H-bonds and showed instantaneous (<1 ns) reorganization of the short-range order of all molecules. Structural analysis of neighbor water molecule pairs showed ~10–15% decrease in the H-bond number after melting whereas all molecules form a single long-range H-bond network. Analysis of the H-bond network showed minor changes in the H-bond interaction energy at the solid-liquid phase transition.
KW - CO gas hydrate
KW - Hydrogen bond network
KW - Molecular dynamics simulation
KW - Phase transitions
KW - Short-range order
KW - MOLECULAR-DYNAMICS
KW - CO2 gas hydrate
KW - DIRECT COEXISTENCE
KW - SIMULATION
KW - SEQUESTRATION
KW - WATER MODELS
KW - METHANE HYDRATE
KW - GAS
KW - MELTING-POINT
KW - FREE-ENERGY
KW - PHASE-DIAGRAM
UR - http://www.scopus.com/inward/record.url?scp=85074720687&partnerID=8YFLogxK
U2 - 10.1016/j.apsusc.2019.143644
DO - 10.1016/j.apsusc.2019.143644
M3 - Article
AN - SCOPUS:85074720687
VL - 499
JO - Applied Surface Science
JF - Applied Surface Science
SN - 0169-4332
M1 - 143644
ER -
ID: 22334508