Ionic-Liquid Surface Structure: Informing Applications through Dynamical Measurements

离子液体表面结构：通过动态测量为应用提供信息

• 批准号: EP/K032062/1
• 负责人: Kenneth McKendrick
• 金额: $ 78.82万
• 依托单位: Heriot-Watt University
• 依托单位国家: 英国
• 项目类别: Research Grant
• 财政年份: 2013
• 资助国家: 英国
• 起止时间: 2013 至 无数据
• 项目状态: 已结题
• 来源: https://gtr.ukri.org/projects?ref=EP%2FK032062%2F1
• 关键词: Ionic; Liquid; Surface; Structure; Informing

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.

美国合作者：T K Minton教授，蒙大拿州立大学。我们的目标是提高离子液体（IL）表面结构的基本理解，并将这种新的见解与离子液体的一些关键的可持续应用。原子和分子从液体表面的非弹性和反应性散射将发展成为一种新的，化学特定的分析探针。两个不同的和互补的实验方法将追求，基于激光光解激光光谱探测和分子束散射。基于激光的方法与一系列样品表面成分的更高通量筛选非常匹配，而分子束散射将提供有关选定液体表面结构的额外信息。结合起来，他们将探测在定制合成的，高纯度离子液体的公认的实际利益的表面偏析的程度。研究将按照复杂程度和风险程度分阶段进行。第一阶段将解决未回答的结构问题的纯离子液体代表的重要家庭的大有机阳离子结合的阴离子的范围。第二部分将研究IL混合物中的表面富集。第三部分将通过动力学和产物状态分布的支持测量，探索IL溶液的表面结构与其在催化中的应用之间的关系。最终相将进入液晶离子液体表面性质的未知领域。整个解释将支持分子动力学（MD）模拟和选择QM/MM散射计算。 这些结果将在多个层面上产生科学影响。我们希望直接影响科学家的未来计划已经从事密切同源研究的碰撞动力学在液体或相关的表面。我们的研究结果也将直接影响到更广泛的社区，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，研究结果将为从事新离子液体合成及其未来应用开发的大型研究团体提供信息。研究人员代表了一个独特的组合建立的专业知识在化学合成和催化应用的离子液体（斯莱特里和布鲁斯;约克，英国），实验测量散射动力学使用激光为基础的（McKendrick和Costen;赫瑞瓦特，英国）或分子束（明顿;蒙大拿州，美国）的方法，和理论建模的气液相互作用（沙茨;西北，美国）。该项目旨在通过广泛的人员交流，扩大他们的经验，促进思想交流和技术专长互补，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的促进作用得到利用，用于众多“环保”应用。最直接的影响将是涉及通过气液界面的运输过程，包括各种形式的催化作用。所雇用的工作人员将接受现代研究方法的特殊和异常多样化的培训。他们将有充分的机会发展更广泛的、可转移的技能，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。将通过建立一个新网站和相关的YouTube频道积极促进外联活动。这将促进所提议的关于国际土地法的成果及其广泛的使用。下载对象将适用于教程和其他教学工具。该网站将在MSU托管。它将充满针对多个层次的材料，从特别感兴趣的科学专家，通过科学倾向的观众，到学校（K-12）教师和普通公众。

项目成果

Scattering dynamics of hyperthermal oxygen atoms on a series of ionic liquid surfaces: [C

高温氧原子在一系列离子液体表面上的散射动力学：[C

• 发表时间: 2014
• 期刊: ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY
• 作者: Minton Timothy K.

Scattering Dynamics of Oxygen Atoms on Imidazolium Tetrafluoroborate Ionic Liquid Surfaces: Dependence on Alkyl Chain Length

氧原子在四氟硼酸咪唑离子液体表面的散射动力学：对烷基链长度的依赖性

• DOI: 10.1021/acs.jpcc.6b02288
• 发表时间: 2016
• 期刊: The Journal of Physical Chemistry C
• 作者: Marshall B

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

• DOI: 10.1021/acs.jpclett.8b02920
• 发表时间: 2018-12
• 期刊: The journal of physical chemistry letters
• 作者: E. Smoll;S. Purcell;Lucía D'Andrea;John M. Slattery;D. Bruce;M. Costen;K. McKendrick;T. Minton

Surface Structure of Alkyl/Fluoroalkylimidazolium Ionic-Liquid Mixtures.

• DOI: 10.1021/acs.jpcb.1c10460
• 发表时间: 2022-03-10
• 期刊: JOURNAL OF PHYSICAL CHEMISTRY B
• 影响因子: 3.3
• 作者: Purcell, Simon M.;Lane, Paul D.;D'Andrea, Lucia;Elstone, Naomi S.;Bruce, Duncan W.;Slattery, John M.;Smoll, Eric J., Jr.;Greaves, Stuart J.;Costen, Matthew L.;Minton, Timothy K.;McKendrick, Kenneth G.
• 通讯作者: McKendrick, Kenneth G.