Ionic-Liquid Mixtures: from Surface Structure to Catalytic Performance

近年来，离子液体以其独特的性能组合和丰富的潜在应用吸引了大量科学家的想象力。对ILs的基础研究使我们的理解取得了突破，并使ILs的发展成为有前途的候选应用领域，如催化、碳捕获和储存（CCS）、生物质处理、电池电解质、超级电容器和染料敏化太阳能电池等。该项目旨在开发和利用广泛的实验和计算方法来研究IL混合物的表面和体积结构，这些结构目前知之甚少，因此未得到充分利用。我们之前开发了一种新的技术，可以用直接的化学特异性探测液体界面，反应原子散射-激光诱导荧光（RAS-LIF），并使用它来检测IL界面上含H（或D）的官能团。我们将通过使用高能al原子作为IL表面（在正离子和阴离子上）氟化官能团的反应探针，将其适用性扩展到新的化学官能团，特别是氟化物种。这将通过在催化相关条件下通过x射线和中子反射率研究液体表面以及通过体结构/性质研究的新能力加以补充。所开发的详细理解将导致IL混合物系统中的结构-性质关系，这些关系将在项目的最后阶段用于支持IL相（SILP）催化，并将支持在SILP系统中部署新的和定制的功能性IL。这个雄心勃勃的项目旨在涵盖从制备到结构理解，然后到工业相关应用的整个IL开发管道。

Ionic liquids (ILs), with their unique combination of properties and wealth of potential applications, have captured the imagination of a large community of scientists in recent years. Fundamental studies on ILs have led to breakthroughs in our understanding and have enabled the development of ILs that are promising candidates for use in areas such as catalysis, carbon-capture and storage (CCS), biomass processing, as electrolytes in batteries, supercapacitors and dye-sensitised solar cells and more. This project aims to develop and utilise a wide range of experimental and computational methodologies to investigate the surface, and bulk, structure of IL mixtures that are currently poorly understood and consequently underutilised. We previously developed a novel technique that can probe liquid interfaces with direct chemical specificity, Reactive-Atom Scattering - Laser-Induced Fluorescence (RAS-LIF), and used it to detect H (or D)-containing functional groups at IL interfaces. We will extend its applicability to new chemical functionalities, in particular fluorinated species, by using high-energy Al-atoms as reactive probes of fluorinated functionality (on both cations and anions) at IL surfaces. This will be complemented by new capabilities for studying liquid surfaces by X-ray and neutron reflectivity under catalytically relevant conditions, and by bulk structure/property studies. The detailed understanding developed will lead to structure-property relationships in IL mixture systems that will be used in the final stages of the project in supported IL phase (SILP) catalysis and will support the deployment of new and bespoke functional ILs for catalysis in SILP systems. This ambitious project aims to cover the whole pipeline of IL development from preparation, to structural understanding, and then to industrially relevant applications.