Position and orientation of water protons need to be specified when the molecular simulation studies are performed for clathrate hydrates. Positions of oxygen atoms in water are experimentally determined by X-ray diffraction analysis of clathrate hydrate structures, but positions of water hydrogen atoms in the lattice are disordered. This study reports a determination of the water proton coordinates in unit cell of structure I (sI), II (sII), and H (sH) clathrate hydrates that satisfy the ice rules, have the lowest potential energy configuration for the protons, and give a net zero dipole moment. Possible proton coordinates in the unit cell were chosen by analyzing the symmetry of protons on the hexagonal or pentagonal faces in the hydrate cages and generating all possible proton distributions which satisfy the ice rules. We found that in the sI and sII unit cells, proton distributions with small net dipole moments have fairly narrow potential energy spreads of about 1 kJ/mol. The total Coulomb potential on a test unit charge placed in the cage center for the minimum energy/minimum dipole unit cell configurations was calculated. In the sI small cages, the Coulomb potential energy spread in each class of cage is less than 0.1 kJ/mol, while the potential energy spread increases to values up to 6 kJ/mol in sH and 15 kJ/mol in the sII cages. The guest environments inside the cages can therefore be substantially different in the sII case. Cartesian coordinates for oxygen and hydrogen atoms in the sI, sII, and sH unit cells are reported for reference.
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28 March 2013
Research Article|
March 27 2013
Water proton configurations in structures I, II, and H clathrate hydrate unit cells
Fumihito Takeuchi;
Fumihito Takeuchi
1Department of Mechanical Engineering,
Keio University
, 3-14-1 Hiyoshi, Kohoku-Ku, Yokohama 223-8522, Japan
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Masaki Hiratsuka;
Masaki Hiratsuka
1Department of Mechanical Engineering,
Keio University
, 3-14-1 Hiyoshi, Kohoku-Ku, Yokohama 223-8522, Japan
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Ryo Ohmura;
Ryo Ohmura
1Department of Mechanical Engineering,
Keio University
, 3-14-1 Hiyoshi, Kohoku-Ku, Yokohama 223-8522, Japan
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Saman Alavi;
Saman Alavi
2Centre for Catalysis Research and Innovation, Department of Chemistry,
University of Ottawa
, Ottawa, Ontario K1N 6N5, Canada
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Amadeu K. Sum;
Amadeu K. Sum
3Center for Hydrate Research, Department of Chemical and Biological Engineering,
Colorado School of Mines
, Golden, Colorado 80401, USA
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Kenji Yasuoka
Kenji Yasuoka
1Department of Mechanical Engineering,
Keio University
, 3-14-1 Hiyoshi, Kohoku-Ku, Yokohama 223-8522, Japan
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Fumihito Takeuchi
1
Masaki Hiratsuka
1
Ryo Ohmura
1
Saman Alavi
2
Amadeu K. Sum
3
Kenji Yasuoka
1
1Department of Mechanical Engineering,
Keio University
, 3-14-1 Hiyoshi, Kohoku-Ku, Yokohama 223-8522, Japan
2Centre for Catalysis Research and Innovation, Department of Chemistry,
University of Ottawa
, Ottawa, Ontario K1N 6N5, Canada
3Center for Hydrate Research, Department of Chemical and Biological Engineering,
Colorado School of Mines
, Golden, Colorado 80401, USA
J. Chem. Phys. 138, 124504 (2013)
Article history
Received:
September 24 2012
Accepted:
March 04 2013
Citation
Fumihito Takeuchi, Masaki Hiratsuka, Ryo Ohmura, Saman Alavi, Amadeu K. Sum, Kenji Yasuoka; Water proton configurations in structures I, II, and H clathrate hydrate unit cells. J. Chem. Phys. 28 March 2013; 138 (12): 124504. https://doi.org/10.1063/1.4795499
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