Ionic-Liquid Surface Structure: Informing Applications through Dynamical Measurements

美国合作者：T K Minton教授，蒙大拿州立大学。我们的目标是加强对离子液体（IL）表面结构的基本理解，并将这一新见解与离子液体的一些关键可持续应用联系起来。液体表面原子和分子的非弹性和反应性散射将作为一种新的、化学特异性的分析探针而发展。两个不同的和互补的实验方法将被追求，基于激光光解-激光光谱探测和分子束散射。基于激光的方法可以很好地匹配高通量筛选一系列样品的表面组成，而分子束散射将提供有关选定液体表面结构的额外信息。结合，他们将探索定制合成的表面偏析程度，具有公认的实际意义的高纯度il。研究将根据复杂程度和风险程度分阶段进行。第一阶段将解决大型有机阳离子与一系列阴离子结合的重要家族的纯il未解决的结构问题。第二个将研究IL混合物的表面富集。第三部分将通过动力学和产物状态分布的辅助测量，探索IL溶液的表面结构与其在催化中的应用之间的关系。最后一个阶段将进入液晶ILs表面特性的未知区域。这些解释将通过分子动力学（MD）模拟和选定的QM/MM散射计算来支持。研究结果将在几个层面上产生科学影响。我们期望直接影响已经从事液体或相关表面碰撞动力学密切相关研究的科学家的未来计划。我们的结果也将对更广泛的社区直接感兴趣，他们一直在使用其他方法来分析液体表面，或通过MD模拟来表征它们。最后，最广泛的是，这些结果将为致力于合成新il及其未来应用发展的大型研究团体提供信息。研究人员在化学合成和ILs催化应用方面具有独特的专业知识（Slattery和Bruce，约克，英国），使用基于激光的散射动力学实验测量（McKendrick和Costen， herot - watt，英国）或分子束（Minton，蒙大拿州，美国）方法，以及气液相互作用的理论建模（Schatz，西北，美国）。拟议的计划建立在广泛的工作人员交流的基础上，扩大他们的经验，促进思想交流和互补的技术专长。我们将产生的基本新见解最有可能通过其在IL材料的设计和优化中发挥的作用，用于许多“环保”应用。最直接的影响将是涉及通过气液界面传输的过程，包括各种形式的催化。被雇用的工作人员将在现代研究方法方面接受特殊和不同寻常的多样化培训。他们将有充足的机会发展更广泛、可转移的技能，并享受国际交流带来的文化利益，为未来的发展或创建高科技公司做出贡献。将通过创建新网站和相关的YouTube频道积极促进外展活动。这将促进拟议的ILs的成果和其更广泛的应用。可下载对象将适用于教程和其他教学工具。该网站将由密歇根州立大学托管。它将包含针对不同层次的材料，从特别感兴趣的科学专家到有科学倾向的读者，再到学校（K-12）教师和普通公众。

US Collaborator: Prof T K Minton, Montana State University. We aim to enhance the fundamental understanding of ionic-liquid (IL) surface structure and to relate this new insight to some key sustainable applications of ILs. Inelastic and reactive scattering of atoms and molecules from liquid surfaces will be developed as a new, chemically specific analytical probe. Two distinct and complementary experimental approaches will be pursued, based on laser-photolysis-laser-spectroscopic probing and molecular-beam scattering. The laser-based method is well matched to higher-throughput screening of surface composition of a range of samples, while molecular-beam scattering will provide additional information on surface structure for selected liquids. In combination, they will probe the degree of surface segregation in custom-synthesized, high-purity ILs of recognized practical interest. The research will proceed in stages of complexity and degree of risk. The first phase will address unanswered structural questions for pure ILs representative of important families of large organic cations combined with a range of anions. The second will investigate surface enrichment in IL mixtures. The third will explore the relationship between the surface structures of IL solutions and their applications in catalysis, through supporting measurements of kinetics and product state distributions. The final phase will enter the uncharted area of the surface properties of liquid-crystalline ILs. The interpretations will be supported throughout by molecular dynamics (MD) simulations and selected QM/MM scattering calculations. The results will have scientific impact on several levels. We expect to directly influence the future programs of scientists already engaged in closely cognate studies of collision dynamics at liquid or related surfaces. Our results will also be of direct interest to a broader community who have been using other methods to analyze liquid surfaces, or characterizing them through MD simulations. Finally, and most broadly, the results will inform the very large research community working on the synthesis of new ILs and the development of their future applications. The investigators represent a unique combination of established expertise in the chemical synthesis and catalytic applications of ILs (Slattery and Bruce; York, UK), experimental measurements of scattering dynamics using laser-based (McKendrick and Costen; Heriot-Watt, UK) or molecular-beam (Minton; Montana State, USA) methods, and theoretical modeling of gas-liquid interactions (Schatz; Northwestern, USA). The proposed program is founded on extensive exchanges of staff, broadening their experience and promoting exchanges of ideas and complementary technical expertise.The fundamental new insight that we will generate is most likely to be exploited through its enabling role in the design and optimization of IL materials for numerous "environmentally friendly" applications. The most direct impact will be on processes involving transport through the gas-liquid interface, including various forms of catalysis. The staff employed will receive an exceptional and unusually diverse training in modern research methods. They will have ample opportunities to develop broader, transferable skills and enjoy the cultural benefits of international exchange, equipping them to contribute to the future growth or creation of high-technology companies. Outreach will be actively promoted through the creation of a new website, and associated YouTube Channels. These will promote both the results of the proposed on ILs and their broader uses in general. Downloadable objects will be suitable for tutorials and other teaching tools. The web site will be hosted at MSU.. It will be populated with material aimed at a number of levels, ranging from the specifically interested scientific experts, through a scientifically-inclined audience, to school (K-12) teachers and the lay public.