Symmetrization and Chemical Precompression Effect of Hydrogen-Bonds in H2-H2O System

JIANG Shuqing YANG Xue WANG Yu ZHANG Xiao CHENG Peng

姜树清, 杨雪, 王宇, 张晓, 程鹏. 氢水化合物中氢键对称化和预压作用下氢行为[J]. 高压物理学报, 2019, 33(2): 020102. doi: 10.11858/gywlxb.20190730
引用本文: 姜树清, 杨雪, 王宇, 张晓, 程鹏. 氢水化合物中氢键对称化和预压作用下氢行为[J]. 高压物理学报, 2019, 33(2): 020102. doi: 10.11858/gywlxb.20190730
JIANG Shuqing, YANG Xue, WANG Yu, ZHANG Xiao, CHENG Peng. Symmetrization and Chemical Precompression Effect of Hydrogen-Bonds in H2-H2O System[J]. Chinese Journal of High Pressure Physics, 2019, 33(2): 020102. doi: 10.11858/gywlxb.20190730
Citation: JIANG Shuqing, YANG Xue, WANG Yu, ZHANG Xiao, CHENG Peng. Symmetrization and Chemical Precompression Effect of Hydrogen-Bonds in H2-H2O System[J]. Chinese Journal of High Pressure Physics, 2019, 33(2): 020102. doi: 10.11858/gywlxb.20190730

Symmetrization and Chemical Precompression Effect of Hydrogen-Bonds in H2-H2O System

doi: 10.11858/gywlxb.20190730
Funds: National Natural Science Foundation of China (21473211, 11674330, 11604342, 11504382, 51727806); Science Challenge Project (TZ2016001)
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    Author Bio:

    JIANG Shuqing (1987-), Ph.D, major in high-energy material synthesis under extreme high-temperature and high-pressure conditions. E-mail: jiangshuqing@issp.ac.cn

  • 摘要: 氢水化合物作为潜在的环境友好型储氢含能材料引起了众多关注。结合金刚石对顶砧装置和原位拉曼光谱测量、同步辐射X射线衍射光谱测量两种表征手段,试图深入理解高压驱动下氢的特征行为,寻找可能的高压富氢相。结果显示,目前已知最高含氢比例1∶1的相C2在压力24.5 GPa时发生相变,更多的氢分子特征峰随相变出现。通过对理论预测结构的拟合,该相最终被确定为P41,氢水比例达到2∶1,且在卸压时能够稳定保存至8.6 GPa。考虑到冰中氢键对称化对压致相变和结构稳定性的重要作用,着重观测了氢键的行为,首次探测到水分子之间氢键对称化过程中完整的费米共振现象。通过对O-H对称伸缩振动模式软化行为的拟合,最终确定氢键对称化发生在55 GPa,同时拉曼光谱测量显示有更进一步相变伴随发生。氢水化合物中不同氢团簇对化学预压作用表现出截然不同的应激反应,这在此体系中也是首次被注意到,对含氢体系和纯氢中氢的金属化研究具有一定参考作用。

     

  • Figure  1.  The evolution of Raman spectra of hydrogen hydrate with increasing pressure from 0.4 to 71.4 GPa. (a) The lattice peaks in the region of 0–1200 cm–1, where the spectra in each phase were marked by different colors and divided by dashed lines; the arrows marked three new broad peaks in high pressure phase IV; (b) The stretching peaks of H2 at various pressures, symbol * referred a new peak at 25.6 GPa in phase III, and the two shoulders at 55.5 GPa were marked by black arrow.

    Figure  2.  The frequency shifts of H-H stretching mode in hydrogen hydrate at various pressures in this work and referred researches. Symbols: the solid black and blue circles indicated frequency shifts collected in this work; the red triangle was frequency shift of pure H2 while the rest black triangle, green square and blue circle were hydrogen in hydrogen hydrate which were cited from previous experimental and theorical studies[15, 25, 30]. The pressure boundaries of each phase were marked by vertical dashed lines.

    Figure  3.  The synchrotron XRD measurement of hydrogen hydrate up to 63.0 GPa. The phase C2 was confirmed by characteristic diffraction lines (111), (220), (311), (400), (331) and (422) at 7.6 GPa. The splitting of line (220) was marked by red arrows at 24.5 GPa, while the splitting of line (111) at 48.9 GPa was marked by black arrows. A rough Pawley refinement of the theorical predicted P41 structure was performed with our experimental spectrum of 24.5 GPa, the short blue lines showed the calculated diffraction lines of refined structure with Materials Studio program.

    Figure  4.  (a) The soften evolution of O-H stretching peaks with increasing pressure from 2.2 to 29.0 GPa; the intensity of deformational peak increased above 29.0 GPa owing to the Fermi resonance with the soften O-H stretching mode, which further shifted to low frequency region above 49.0 GPa. (b) The pressure dependence of the O-H stretching mode; the blue line guided the extrapolation of the soften O-H stretching mode, the red dashed line showed the O-H stretching mode in solid water for comparison[31].

    Figure  5.  (a) The Raman spectra of hydrogen hydrate under decompression. (b) The comparison of pressure dependences of the H-H stretching mode during the compression and decompression process. The red and black arrows marked the disappeared peaks at 39.7 and 8.6 GPa, respectively.

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出版历程
  • 收稿日期:  2019-02-26
  • 修回日期:  2019-03-21
  • 发布日期:  2019-03-25

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