高自由度的低共熔溶剂微环境反应器的构筑和水油界面烷基化反应性能研究

低共熔溶剂（DES）是近年来受到广泛关注的双组分类离子液体。催化应用方面，DES有极性高、氢键丰富、能形成协同效应等优点，也存在着热稳定性差、粘度大和不易回收等缺点。构建DES微环境的纳米反应器能解决上述问题，也存在难点：如何将DES双组分共同固载在同一反应器内且保持高自由度；如何在有载体信号干扰的情况下表征担载型DES两组分之间的氢键作用；如何挖掘和利用DES独特优点，如表面亲（疏）水性等。本研究在笼形介孔氧化硅孔道内，以多层“分子刷”结构固载DES组分A，“瓶中造船”法非共价限域固载组分B的线形聚合物，保持DES组分的高自由度。通过探针分子和探针反应表征多相DES组分的相互作用，实现可控制备。以水油界面烷基化反应考察DES反应器的微环境和表面性质，研究其相转移和微乳液（pickering乳液）催化能力，并构建构效关系。本研究将拓展微环境可调控反应器的科学理论和实际应用，具有鲜明原创性。

Deep Eutectic Solvents (DES) are new solvents with properties which are similar to ionic liquid, and DES are composited of hydrogen-bond acceptors (HBA) and hydrogen-bond donors (HBD). With the advantages of high polarity and solubility, abundant hydrogen-bonds and cooperative effects, DES have great potential in catalytic applications. However, several drawbacks also limit the application of DES, such as poor thermal stability, high viscosity and inconvenient recycle ability. Heterogeneous DES catalysts can avoid above disadvantages, but there are several obstacles in designing and synthesis of DES reactors. It is difficult to immobilize both components of DES in the same reactor with high freedom of movement. There are some problems with characterization of hydrogen bonds between HBA and HBD, especially with the disturbance of noisy signals from the matrix. How to utilize the distinguishing features of DES, such as unique surface hydrophobicity/hydrophilicity, is still to be improved. DES components (parts A) will be grafted onto the long-chain “silane brushes”, and parts B will be assembled as linear polymers via the “ship-in-a-bottle” method (non-covalent method) in the cage-type mesoporous silica. These heterogeneous DES components can move freely to interact with each other. Suitable probe molecules and reactions are utilized to characterize the interaction between components of immobilized DES, and controllable synthesis will be achieved. The catalytic performance of DES microenvironment reactors will be tested in alkylation reaction with oil-water interface. DES reactors will act as phase-transfer and micro-emulsion (pickering emulsion) catalysts with specific surface properties. The relationship between microenvironment, surface properties and catalytic performance will also be discussed. This project will contribute to the scientific research and applications of nano-reactors with controllable microenvironments, and this research is with distinct originality.