Probing Conformational Heterogeneity at the Ionic Liquid-Vacuum Interface by Reactive-Atom Scattering

被引:13
|
作者
Smoll, Eric J., Jr. [1 ]
Purcell, Simon M. [2 ]
D'Andrea, Lucia [3 ]
Slattery, John M. [3 ]
Bruce, Duncan W. [3 ]
Costen, Matthew L. [2 ]
McKendrick, Kenneth G. [2 ]
Minton, Timothy K. [1 ]
机构
[1] Montana State Univ, Dept Chem & Biochem, Bozeman, MT 59717 USA
[2] Heriot Watt Univ, Sch Engn & Phys Sci, Inst Chem Sci, Edinburgh EH14 4AS, Midlothian, Scotland
[3] Univ York, Dept Chem, York YO10 5DD, N Yorkshire, England
来源
JOURNAL OF PHYSICAL CHEMISTRY LETTERS | 2019年 / 10卷 / 02期
基金
英国工程与自然科学研究理事会; 美国国家科学基金会;
关键词
HYPERTHERMAL OXYGEN-ATOMS; MOLECULAR MOBILITY; HIGH-ENERGY; SURFACE; DYNAMICS; SIMULATIONS; COLLISIONS; DEFECTS; PENETRATION; MONOLAYER;
D O I
10.1021/acs.jpclett.8b02920
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
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.
引用
收藏
页码:156 / 163
页数:15
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