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：蒙大拿州立大学T K Minton教授。我们旨在增强对离子液体（IL）表面结构的基本理解，并将这种新见解与IL的某些关键可持续应用联系起来。来自液体表面的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开发。基于激光 - 光解激体光谱探测和分子梁散射，将采用两种不同的互补实验方法。基于激光的方法与一系列样品的表面组成的高通量筛选非常匹配，而分子梁散射将提供有关选定液体表面结构的其他信息。结合起来，他们将探测自定义合成的高纯度IL的表面隔离程度。该研究将在复杂性和风险程度的阶段进行。第一阶段将针对代表大型有机阳离子和一系列阴离子的重要家族的纯IL解决未解决的结构问题。第二个将研究IL混合物中的表面富集。第三将通过支持测量动力学和产品状态分布来探讨IL溶液的表面结构及其在催化中的应用之间的关系。最后一阶段将进入液晶ILS表面特性的未知区域。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。 结果将对多个层面产生科学影响。我们希望直接影响已经参与液体或相关表面上碰撞动态的科学家的未来计划。对于一个更广泛的社区，我们的结果也将引起人们的直接兴趣，他们一直使用其他方法来分析液体表面或通过MD模拟对其进行表征。最后，最广泛的是，结果将为研究新ILS的综合及其未来应用的开发而为非常庞大的研究社区提供信息。 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,美国）。拟议的计划建立在广泛的员工交流，扩大他们的经验并促进思想和互补技术专长的交流中。我们将最有可能通过在IL材料的设计和优化IL材料中对众多“环保”应用程序的设计和优化的作用来利用我们将产生的基本新见解。最直接的影响将是涉及通过气体界面传输的过程，包括各种形式的催化。雇用的工作人员将接受现代研究方法的非凡培训。他们将有足够的机会发展更广泛的，可转移的技能，并享受国际交流的文化利益，使他们有助于为未来的高科技公司的增长或创建做出贡献。外展将通过创建新网站和关联的YouTube频道积极促进外展活动。这些将促进ILS提议的结果及其一般的更广泛用途。可下载的对象适用于教程和其他教学工具。该网站将在MSU托管。它的材料将以许多层次的材料构建，从特定感兴趣的科学专家到科学上的受众群体到学校（K-12）教师和外行公众。

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.