Ionic-Liquid Surface Structure: Informing Applications through Dynamical Measurements

美国合作者：蒙大拿州立大学T·K·明顿教授。我们的目标是加强对离子液体(IL)表面结构的基本了解，并将这种新的见解与离子液体的一些关键的可持续应用联系起来。原子和分子在液体表面的非弹性和反应性散射将被开发为一种新的、具有化学特异性的分析探针。基于激光-光解-激光光谱探测和分子束散射，将寻求两种截然不同和互补的实验方法。基于激光的方法与一系列样品的表面成分的高通量筛选很好地匹配，而分子束散射将提供关于选定液体的表面结构的额外信息。结合起来，他们将探索定制合成的高纯度ILS的表面分离程度，这是公认的实用价值。研究将按复杂程度和风险程度分阶段进行。第一阶段将解决尚未回答的纯ILS的结构问题，这些ILS代表了与一系列阴离子结合的重要的有机阳离子家族。第二部分将研究IL混合物中的表面浓缩。第三部分将通过动力学和产物状态分布的测量，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离子液体表面性质的未知领域。分子动力学(MD)模拟和选定的QM/MM散射计算将始终支持这些解释。这一结果将在几个层面上产生科学影响。我们希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。我们的结果也将直接对更广泛的社区感兴趣，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，也是最广泛的，这些结果将为致力于合成新的ILS及其未来应用开发的非常大的研究社区提供信息。研究人员代表着在ILS的化学合成和催化应用方面的独特专业知识(Slattery和Bruce，英国约克)，使用激光散射动力学的实验测量(McKendrick和Costen，英国Heriot-Watt)或分子束方法(Minton，蒙大拿州，美国)，以及气液相互作用的理论建模(Schatz，美国西北)。拟议的计划建立在广泛的员工交流基础上，扩大他们的经验，促进思想交流和互补的技术专业知识。我们将产生的基本新见解最有可能通过其在设计和优化IL材料方面的促进作用而被利用，这些材料适用于许多“环境友好型”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。受雇的工作人员将接受关于现代研究方法的特殊和非同寻常的多样化培训。他们将有充分的机会发展更广泛的、可转让的技能，并享受国际交流的文化好处，使他们能够为未来的增长或高科技公司的创建做出贡献。将通过创建一个新网站和相关的YouTube频道，积极促进外联工作。这些措施将促进拟议的关于国际劳工标准的成果及其在一般情况下的更广泛应用。可下载的对象将适用于教程和其他教学工具。该网站将在密歇根州立大学托管。它将充斥着针对多个层次的材料，从特别感兴趣的科学专家，到倾向于科学的受众，到学校(K-12)教师和非专业公众。

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.