SFB 1452: Catalysis at Liquid Interfaces (CLINT)

该CRC，液体界面催化（克林特），将遵循一个新的范式：我们的目标是探索液体界面的高度动态，各向异性环境，以创建，定制和稳定具有独特反应性和性能的催化活性位点。基于这一理念，我们的目标是开发新型催化材料，将选择性、生产率、耐用性和易加工性结合在一起。克林特由四个密切相关的研究领域（A，B，C和M）组成。所有方法都集中在超低蒸汽压的固体支撑液体上，以在连续气相反应中实现稳定的催化性能。区域A 'SCALMS'涉及在反应性气体存在下支撑的液体合金界面的动态形成，代表了一种新的、技术上相关的多相单原子催化剂路线。最近由四个PI联合建立的“负载催化活性液态金属溶液（SCALMS）”概念将系统地探索优化材料性能和提高性能。我们的目标是将SCALMS开发成一种基本理解和可扩展的方法，用于具有最高反应性，金属效率和最终鲁棒性的新催化材料。区域B“界面增强SILP”集中于溶解的分子催化剂络合物，其显示出非常高的优先性以位于“负载离子液相（SILP）”系统的界面处。界面亲和力应是所应用的配体、支持化学、离子液体和气相的函数。我们的研究目标是阐明和利用位于气/液和液/固界面的特定反应性。C区“高级SCILL”涉及离子液体和催化活性金属之间反应界面的动态相互作用。我们的目标是从根本上扩大强大的方法“固体催化剂与离子液体层（SCILL）”的操作传统的负载型催化剂，通过使用新的功能化离子液体，并通过应用新的概念（电）催化转化。区域A、B和C通过润湿、选择性分子相互作用或吸附、扩散和流动性、分离和富集、配体和集合效应以及界面处反应环境的各向异性的总体研究方面紧密相连。为了在对这些方面的详细理解和新催化剂材料的开发之间架起桥梁，每个领域将把对模型系统的基础研究与使用真实的催化剂的动力学研究联系起来。区域M“建模和模拟”通过理论研究阐明这些联合方面，例如复杂液体界面的电子结构，活性位点的分布，或界面处自组织和结构形成的动力学。通过这种方式，我们将寻求开发一个全面的方法，在液体界面催化的新概念。

This CRC, Catalysis at Liquid Interfaces (CLINT), will follow a new paradigm: We aim to explore the highly dynamic, anisotropic environment of liquid interfaces to create, tailor and stabilise catalytically active sites with unique reactivity and performance. With this concept, we aim to develop novel catalytic materials that combine selectivity, productivity, robustness, and ease of processing at the highest level. CLINT consists of four strongly interlinked research areas (A, B, C, and M). All approaches centre on solid-supported liquids of ultralow vapour pressure to enable stable catalytic performance in continuous gas-phase reactions. Area A ‘SCALMS’ deals with the dynamic formation of supported liquid alloy interfaces in the presence of reactive gases, representing a new, technically relevant route toward heterogeneous single-atom catalysts. The concept of ‘Supported Catalytically Active Liquid Metal Solutions (SCALMS)’, established recently by four PIs jointly, will be explored systematically towards optimised materials properties and enhanced performance. We aim to develop SCALMS into a fundamentally understood and scalable approach for new catalytic materials with highest reactivity, metal efficiency and ultimate robustness. Area B ‘Interface-enhanced SILP’ focusses on dissolved molecular catalyst complexes that show a very high preference to be located at the interfaces of ‘Supported Ionic Liquid Phase (SILP)’ systems. The interface affinity should be a function of the applied ligands, support chemistry, ionic liquid, and gas phase. Our research target is to elucidate and exploit the specific reactivity located at both, the gas/liquid and the liquid/solid interface. Area C ‘Advanced SCILL’ deals with dynamic interactions at the reactive interfaces between ionic liquids and catalytically active metals. We aim to radically expand the powerful approach of ‘Solid Catalysts with Ionic Liquid Layer (SCILL)’ for the manipulation of traditional supported catalysts by using novel functionalised ILs and by applying the concept to novel (electro)catalytic transformations. The areas A, B, and C are tightly interlinked by the overarching research aspects of wetting, selective molecular interaction or adsorption, diffusion and mobility, segregation and enrichment, ligand and ensemble effects, and the anisotropy of reactive environments at the interface. To bridge between a detailed understanding of these aspects and the development of new catalyst materials, each area will link fundamental studies on model systems with kinetic investigations using real catalysts. Area M ‘Modelling and simulation’ addresses these joint aspects by theoretical studies elucidating, e.g. the electronic structure of complex liquid interfaces, the distributions of active sites, or the dynamics of self-organisation and structure formation at the interface. In this way, we will seek to develop a comprehensive approach to the new concept of catalysis at liquid interfaces.