CO2 Hydration Shell Structure and Transformation,The Journal of Physical Chemistry Letters

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CO2 Hydration Shell Structure and Transformation
The Journal of Physical Chemistry Letters ( IF 4.8 ) Pub Date : 2017-06-15 00:00:00 , DOI: 10.1021/acs.jpclett.7b00971
Samual R. Zukowski ₁ , Pavlin D. Mitev ₂ , Kersti Hermansson ₂ , Dor Ben-Amotz ₁

Affiliation

The hydration-shell of CO₂ is characterized using Raman multivariate curve resolution (Raman-MCR) spectroscopy combined with ab initio molecular dynamics (AIMD) vibrational density of states simulations, to validate our assignment of the experimentally observed high-frequency OH band to a weak hydrogen bond between water and CO₂. Our results reveal that while the hydration-shell of CO₂ is highly tetrahedral, it is also occasionally disrupted by the presence of entropically stabilized defects associated with the CO₂-water hydrogen bond. Moreover, we find that the hydration-shell of CO₂ undergoes a temperature-dependent structural transformation to a highly disordered (less tetrahedral) structure, reminiscent of the transformation that takes place at higher temperatures around much larger oily molecules. The biological significance of the CO₂ hydration shell structural transformation is suggested by the fact that it takes place near physiological temperatures.

中文翻译：

CO ₂水化壳结构与转化

利用拉曼多元曲线分辨率（Raman-MCR）光谱技术和从头算分子动力学（AIMD）振动态模拟得出的特征，对CO ₂的水化壳进行了表征，以验证我们将实验观察到的高频OH频段分配给了一个水和CO ₂之间的氢键弱。我们的结果表明，尽管CO ₂的水合壳高度为四面体，但偶尔也会因与CO _2-水氢键相关的熵稳定缺陷的存在而被破坏。此外，我们发现CO ₂的水合壳经历温度依赖性的结构转变为高度无序的（四面体较少）结构，让人联想到在高温下围绕大得多的油性分子发生的转变。CO ₂水合壳结构转化发生在生理温度附近这一事实表明了其生物学意义。

更新日期：2017-06-28

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