Probing Conformational Heterogeneity at the Ionic Liquid-Vacuum Interface by Reactive-Atom Scattering.
Probing Conformational Heterogeneity at the Ionic Liquid-Vacuum Interface by Reactive-Atom Scattering.
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DOI：
10.1021/acs.jpclett.8b02920
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发表时间：
2018-12
期刊：
影响因子：
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通讯作者：
E. Smoll;S. Purcell;Lucía D'Andrea;John M. Slattery;D. Bruce;M. Costen;K. McKendrick;T. Minton
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文献类型：
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作者：
E. Smoll;S. Purcell;Lucía D'Andrea;John M. Slattery;D. Bruce;M. Costen;K. McKendrick;T. Minton
液体界面的原子水平描述落后于固体晶体表面，因为现有的实验技术在报告波动液体界面层中的分子结构方面受到限制。通过研究常见离子液体1-丁基-3-甲基咪唑双（三氟甲基磺酰基）亚胺上的f原子散射动力学，我们对气液界面进行了更详细的实验描述。在氘标记的对比下，反应分散的HF同位素物的产率和动力学行为可以从阳离子丁基、甲基和环基中分辨出不同的特征，这有助于量化液-真空界面上阳离子构象的相对居群。这些结果证明了分子组织在驱动气液界面极端外部区域的位点特异性反应中的重要性。
The atomic-level description of liquid interfaces has lagged behind that of solid crystalline surfaces because existing experimental techniques have been limited in their capability to report molecular structure in a fluctuating liquid interfacial layer. We have moved toward a more detailed experimental description of the gas-liquid interface by studying the F-atom scattering dynamics on a common ionic liquid, 1-butyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide. When given contrast by deuterium labeling, the yield and dynamical behavior of reactively scattered HF isotopologues can resolve distinct signatures from the cation butyl, methyl, and ring groups, which help to quantify the relative populations of cation conformations at the liquid-vacuum interface. These results demonstrate the importance of molecular organization in driving site-specific reactions at the extreme outer regions of the gas-liquid interface.