Catalytic Microgel Reactions at Interface of Immiscible Droplets

多相体系中的反应可以在较低的催化剂用量下获得较高的收率，并且由于与散装体系相比存在较大的界面面积而降低了能耗。乳剂界面的催化反应在基础科学和工业应用中具有重要意义。本研究的主要重点是利用数字微流控（DMF）平台研究表面活性微凝胶催化剂在两种不混溶液体界面上的催化性能。DMF是生成定义良好的界面和在液滴水平上研究界面反应的强大工具。合成了一系列粒径可控、交联密度可控、用量可调、有机催化剂可定位的微凝胶基催化剂，并对其进行了表征。利用DMF，我们将通过两个不混相液滴的接触产生模型界面，以定位液-液界面处的微凝胶。利用该技术，我们希望(a)在稳态下研究两个不混相液滴界面上的反应，(b)通过液-液界面的时变生成来定义反应/孵育时间，(c)分离含有产物的不混相液滴，在界面上没有任何残留物，(d)实现级联反应，(e)实现每个液滴和界面的分析。DMF装置将用于系统研究微凝胶催化剂在液-液界面的催化活性，特别关注醛醇和氧化裂解反应的反应产率、选择性和反应动力学。该项目将对微凝胶催化催化剂在不混溶液滴界面上的反应机理、物理和化学现象以及动力学等方面获得新的重要见解。该项目将允许开发灵活的微流体平台，以改进工业应用中的高通量乳化工艺。该项目将允许开发灵活的可配置微流控平台，用于工业应用中乳化工艺的高通量筛选。

Reactions in multiphase systems can lead to higher yields at lower catalyst quantities and reduced energy consumption due to the existence of a large interfacial area compared to bulk systems. Catalytic reactions at interfaces of emulsions are of great interest for fundamental science and industrial applications. The main focus of this proposal is the investigation of the catalytic performance of surface-active microgel-based catalysts at the interface between two immiscible liquids using a digital microfluidic (DMF) platform. DMF is a powerful tool to generate well-defined interfaces and study interfacial reactions on droplet level. Series of microgel-based catalysts with controlled size, crosslinking density, tunable amount and localization of organocatalysts will be synthesized and characterized. Using DMF, we will generate model interfaces by contact of two immiscible droplets to localize the microgels at the liquid-liquid interfaces. Using this technology, we would like (a) to study reactions at the interface of two immiscible droplets in steady-state, (b) to define reaction/incubation times by time-variable generation of the liquid-liquid interface, (c) to separate the immiscible droplets which contain the products without any residuals at the interface, (d) to enable cascade reactions, (e) to enable analytics of each droplet and interface. The DMF setup will be used for systematic studies of the catalytic activity of microgel catalysts at the liquid-liquid interfaces with the specific focus on the reaction yields, selectivity and reaction kinetics for aldol and oxidative cleavage reactions. This project will gain new and important insights into the mechanism, physical and chemical phenomena as well as kinetics of reactions of microgel-based cata-lysts at the interface of immiscible droplets. This project will allow development of flexible mi-crofluidic platforms for improvement of high-throughput emulsion-based processes in industri-al applications. This project will allow the development of a flexible configurable microfluidic platform for high-throughput screening of emulsion-based processes in industrial applications.