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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Raman Spectroscopic Studies of Clathrate Hydrate Formation in the Presence of Hydrophobized Particles
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Raman Spectroscopic Studies of Clathrate Hydrate Formation in the Presence of Hydrophobized Particles

机译：疏水颗粒存在下包合物水合物形成的拉曼光谱研究

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摘要

In the present work, Raman spectroscopy was used to study the structure of water molecules in the vicinity of glass particles with different hydrophobicity, immersed in water and in tetrahydrofuran and cyclopentane hydrates. The glass particle surfaces were clean (hydrophilic)) coated with N,N-dimethyl-N octadecyl-3-aminopropyl trimethoxysilyl chloride (partially hydrophobic), or coated with octadecyltrichlorosilane (hydrophobic). The Raman spectra indicate that, prior to nucleation, water molecules in the vicinity of hydrophobic surfaces are more ice-like ordered than those in the bulk liquid or near either hydrophilic or partially hydrophobic surfaces. Furthermore, the degree of hydrogen-bond ordering of water observed prior to hydrate nucleation, as measured by the ratio of the inter- and intra-molecular Raman OH bands, was found to have an inverse relationship with the mean induction time for hydrate formation. Following hydration formation, no significant difference in the water molecule structure was observed in the hydrate phase based on their Raman OH bands, irrespective of surface hydrophobicity. These observations made with Raman spectroscopy provide the foundations for a quantitative link between hydrate nucleation promotion and water-ordering near solid surfaces, which could enable direct comparisons with results from corresponding molecular dynamics simulations.
机译：在目前的工作中，拉曼光谱法用于研究具有不同疏水性的玻璃颗粒附近的水分子结构，该玻璃颗粒浸入水中以及四氢呋喃和环戊烷水合物中。玻璃颗粒表面是干净的（亲水的）），涂有N，N-二甲基-N十八烷基-3-氨基丙基三甲氧基甲硅烷基氯（部分疏水），或涂有十八烷基三氯硅烷（疏水）。拉曼光谱表明，在成核之前，疏水表面附近的水分子比散装液体中或亲水或部分疏水表面附近的水分子更像冰。此外，发现在水合物成核之前观察到的水的氢键有序度，通过分子间和分子内拉曼OH带的比率测量，与水合物形成的平均诱导时间成反比关系。水合形成后，根据水合物相的拉曼OH谱带，无论表面疏水性如何，在水合物相中均未观察到水分子结构的显着差异。拉曼光谱学的这些发现为水合物成核促进与固体表面附近的水有序之间的定量联系奠定了基础，这可以与相应的分子动力学模拟结果进行直接比较。

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