Ionic-Liquid Mixtures: from Surface Structure to Catalytic Performance

近年来，离子液体(ILS)以其独特的性质和丰富的潜在应用，吸引了一大批科学家的想象力。对离子液体的基础研究突破了我们的理解，并使离子液体的开发成为可能，这些离子液体有望用于催化、碳捕获和储存(CCS)、生物质加工、电池电解液、超级电容器和染料敏化太阳能电池等领域。该项目旨在开发和利用广泛的实验和计算方法来研究目前知之甚少并因此未得到充分利用的IL混合物的表面和体相结构。我们以前开发了一种新的技术，可以探测具有直接化学特异性的液体界面，反应原子散射-激光诱导荧光(RAS-LIF)，并用它来检测IL界面上含有H(或D)的官能团。我们将把它的适用性扩展到新的化学功能，特别是氟化物种，通过在IL表面使用高能Al原子作为氟化官能团的反应探针(在阳离子和阴离子上)。此外，还将通过X射线和中子在催化相关条件下的反射率研究液体表面，以及整体结构/性质研究来补充这一新能力。开发的详细了解将导致IL混合体系的结构-性质关系，这些关系将用于项目的最后阶段的负载型IL阶段(SILP)催化，并将支持在SILP系统中部署用于催化的新的和定制的功能性ILS。这个雄心勃勃的项目旨在涵盖从准备到结构理解，再到工业相关应用的整个IL开发流程。

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.