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Isotopic effect and amorphization of deuterated hydrogen hydrate under high pressure

机译：高压氘化氢的同位素效应和非晶化

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摘要

High-pressure experiments of a mixture of H_2 and D_2O were performed using a diamond-anvil cell in the pressure range of 0.5-77.0 GPa under room temperature. Raman measurements revealed that an exchange of the hydrogen atoms occurred between fluid hydrogen and liquid water before the formation of deuterated hydrogen hydrate, and that a high-pressure structure of hydrogen hydrate, a filled ice Ic structure, formed at the same pressure as H_2-H_2O system hydrate. Additionally, the Raman spectra of the vibron for the D_2, HD and H_2 molecules revealed that the guest hydrogen molecules were partly extracted from the filled ice Ic structure above 20 GPa. The extraction of hydrogen molecules occurred depending on the atomic weight of the guest hydrogen molecules, and the heavier molecules were selectively released from the filled ice Ic structure. This isotopic effect in the extraction of hydrogen molecules showed differences in the stability of hydrogen hydrate depending on the species of guest molecules between D_2, HD, and H_2. Above 65 GPa, the filled ice Ic structure of hydrogen hydrate transformed to an amorphous phase. Formation of the amorphous phase showed the high-pressure limitation of hydrogen hydrate as a crystal structure and a new mechanism for the dissociation of gas hydrates under high pressure and room temperature.
机译：在室温下，在0.5-77.0 GPa的压力范围内，使用金刚石-砧形电池对H_2和D_2O的混合物进行高压实验。拉曼测量表明，在氘化水合氢形成之前，液态氢和液态水之间发生了氢原子交换，并且在与H_2-相同的压力下形成了高压氢水合物结构，即填充的冰Ic结构。 H_2O系统水合物。此外，D_2，HD和H_2分子的振动子拉曼光谱表明，客体氢分子部分从20 GPa以上的填充冰Ic结构中提取。取决于客体氢分子的原子量发生氢分子的提取，并且较重的分子从填充的冰Ic结构中选择性地释放。氢分子提取中的这种同位素效应显示出水合氢稳定性的差异，这取决于D_2，HD和H_2之间的客体分子的种类。高于65 GPa，水合氢的填充冰Ic结构转变为非晶相。非晶相的形成显示出水合氢作为晶体结构的高压极限，以及在高压和室温下气体水合物解离的新机理。

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  • 来源
    《Physical review》 |2011年第14期|p.144101.1-144101.5|共5页
  • 作者

    Shin-ichi Machida; Hisako Hirai; Taro Kawamura; Yoshitaka Yamamoto; Takehiko Yagi;

  • 作者单位

    Geodynamics Research Center, Ehime University, 2-5 Bunkyocho, Matsuyama, Ehime 790-8577, Japan;

    Geodynamics Research Center, Ehime University, 2-5 Bunkyocho, Matsuyama, Ehime 790-8577, Japan;

    National Institute of Advanced Industrial Science and Technology, Tsukuba, Ibaraki 305-8569, Japan;

    National Institute of Advanced Industrial Science and Technology, Tsukuba, Ibaraki 305-8569, Japan;

    Institute for Solid State Physics, University of Tokyo, 5-1-5 Kashiwanoha Kashiwa, Chiba 277-8581, Japan;

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  • 正文语种 eng
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  • 关键词

    pressure treatment; infrared and raman spectra;

    机译：压力处理;红外光谱和拉曼光谱;

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