Homogeneous Catalysts for the Production of Monomers for Sustainable Polymers from CO2 and Diols

1)初步致力于开发用于二氧化碳和二元醇偶联形成6元环状碳酸酯的催化剂2)开发用于其他小分子偶联的催化方案，例如CS23)开发用于开环聚合反应的催化剂在布哈德实验室先前发表的结果的基础上，初步研究的目标是开发一种用于二氧化碳和1，3二醇偶联生成环状碳酸酯的催化方案。希望通过使用受挫的Bronsted碱：Lewis酸对策略来实现这一目标。将采用双边实验和计算方法，用密度泛函计算补充实际数据。这样的计算将用于实验室内的进一步研究。一旦完成，将进行研究，以阐明反应环化步骤的机理路径。智能催化剂设计可能允许调节环化步骤的方向，潜在地导致以前无法获得的环状碳酸酯单体的形成。此外，应用于二氧化碳和二醇偶联的催化策略也有望应用于其他环化试剂(如碳硫化物、硅烷、羰基硫化物等)。与此同时，将开展聚合反应新催化体系的研究(有机催化剂和金属络合物)，包括可切换催化剂的研究和流动应用的表面固定化。

1) Initial focus on the development of catalysts for CO2 and diol coupling to form 6 membered cyclic carbonates.2) Develop catalytic protocols for other small molecule coupling e.g. CS23) Develop catalysts for ring opening polymerisation reactionsBuilding on previously published results from the Buchard laboratory, the initial research will aim to develop a catalytic protocol for the coupling of carbon dioxide with 1,3 diols to form cyclic carbonates. It is hoped this will be achieved through utilisation of a frustrated Bronsted base: Lewis acid pair strategy. A bilateral experimental and computational approach will be adopted, by supplementing practical data with DFT calculations. Such calculations will be used to inform further study within the laboratory.Once achieved, research will be undertaken to elucidate the mechanistic pathway of the cyclisation step of the reaction. Intelligent catalyst design may allow for tuned direction of the cyclisation step, potentially leading to formation of previously inaccessible cyclic carbonate monomers. In addition, it is hoped the catalytic strategy as applied to CO2 and diol coupling may also find application with other, cyclisation reagents (e.g. carbon sulphide, silanes, carbonyl sulphide etc).Alongside this, studies into novel catalytic systems for polymerisation reactions will be undertaken (organocatalysts and metal complexes), including investigation into switchable catalysts and immobilisation on surfaces for flow applications.