Tesa-Serrate Maria A, Smoll Eric J, Minton Timothy K, McKendrick Kenneth G
Institute of Chemical Sciences, School of Engineering and Physical Sciences, Heriot-Watt University, Edinburgh EH14 4AS, United Kingdom; email:
Department of Chemistry and Biochemistry, Montana State University, Bozeman, Montana 59717; email:
Annu Rev Phys Chem. 2016 May 27;67:515-40. doi: 10.1146/annurev-physchem-040215-112355. Epub 2016 Apr 18.
The gas-liquid interface remains one of the least explored, but nevertheless most practically important, environments in which molecular collisions take place. These molecular-level processes underlie many bulk phenomena of fundamental and applied interest, spanning evaporation, respiration, multiphase catalysis, and atmospheric chemistry. We review here the research that has, during the past decade or so, been unraveling the molecular-level mechanisms of inelastic and reactive collisions at the gas-liquid interface. Armed with the knowledge that such collisions with the outer layers of the interfacial region can be unambiguously distinguished, we show that the scattering of gas-phase projectiles is a promising new tool for the interrogation of liquid surfaces with extreme surface sensitivity. Especially for reactive scattering, this method also offers absolute chemical selectivity for the groups that react to produce a specific observed product.
气液界面仍然是研究最少但实际上最重要的分子碰撞发生环境之一。这些分子层面的过程是许多具有基础和应用价值的宏观现象的基础，涵盖蒸发、呼吸作用、多相催化和大气化学等领域。在这里，我们回顾过去十年左右揭示气液界面非弹性和反应性碰撞分子层面机制的研究。基于与界面区域外层的此类碰撞能够被明确区分这一认知，我们表明气相抛射体的散射是一种具有极高表面灵敏度的探测液体表面的新方法。特别是对于反应性散射，该方法还能对产生特定观测产物的反应基团提供绝对的化学选择性。
