Abnormal Thermal Expansion of Clathrate Hydrates Induced by Asymmetric Guest Molecules

Authors

  • Minjun Cha,

    1. Department of Chemical and Biomolecular Engineering (BK21 program) and Graduate School of EEWS, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701 (Rep. of Korea), Fax: (+82) 42-350-3910
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  • Yeobum Youn,

    1. Department of Chemical and Biomolecular Engineering (BK21 program) and Graduate School of EEWS, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701 (Rep. of Korea), Fax: (+82) 42-350-3910
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  • Minchul Kwon,

    1. Department of Chemical and Biomolecular Engineering (BK21 program) and Graduate School of EEWS, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701 (Rep. of Korea), Fax: (+82) 42-350-3910
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  • Dr. Kyuchul Shin,

    1. National Research Council of Canada, 100 Sussex Drive, Ottawa K1A 0R6 (Canada)
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  • Dr. Seongsu Lee,

    1. Korea Atomic Energy Research Institue (KAERI), P.O. Box 105, Yuseong-gu, Daejeon 305-600 (Rep. of Korea)
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  • Prof. Dr. Huen Lee

    Corresponding author
    1. Department of Chemical and Biomolecular Engineering (BK21 program) and Graduate School of EEWS, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701 (Rep. of Korea), Fax: (+82) 42-350-3910
    • Department of Chemical and Biomolecular Engineering (BK21 program) and Graduate School of EEWS, Korea Advanced Institute of Science and Technology (KAIST), Daejeon 305-701 (Rep. of Korea), Fax: (+82) 42-350-3910

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Abstract

We investigated for the first time the abnormal thermal expansion induced by an asymmetric guest structure using high-resolution neutron powder diffraction. Three dihydrogen molecules (H2, D2, and HD) were tested to explore the guest dynamics and thermal behavior of hydrogen-doped clathrate hydrates. We confirmed the restricted spatial distribution and doughnut-like motion of the HD guest in the center of anisotropic sII-S (sII-S=small cages of structure II hydrates). However, we failed to observe a mass-dependent relationship when comparing D2 with HD. The use of asymmetric guest molecules can significantly contribute to tuning the cage dimension and thus can improve the stable inclusion of small gaseous molecules in confined cages.

Abstract

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