功能化多金属氧簇常压下催化转化CO2构建噁唑啉酮和异色满杂环

As the principal greenhouse gas, carbon dioxide (CO2) is also a ubiquitous C1 resource. The research of catalytic activation, transformation and utilization of CO2 have drawn much attention in the past years. The traditional CO2 transformation is usually associated with several persistent disadvantages including the need for high temperature, high pressure, air and water sensitive. This project aims at developing methodologies for heterocycle syntheses using ambient CO2 as feedstock with the catalysis of functionalized polyoxometalate under mild conditions. The construction of high-value oxazolidin-2-ones and isochromans scaffolds will be realized employing cheap, ambient pressure of CO2 as starting material. The reaction parameters such as ligands, solvents, additives, temperature, and reaction time will be investigated to avoid drastic conditions. More importantly, the structure-activity relationship of the catalytic system will be studied using NMR and different spectroscopic technologies. The mechanism of the dual activation of substrates and CO2 by the functionalized polyoxometalate will be explored with isotopic labeling experiments and quantum chemistry methods..This project will establish the catalytic CO2 transformation methods under ambient condition circumventing the use of high-pressure apparatus and toxic carboxylative reagents. We anticipate that this study will lead to new knowledge in polyoxometalate catalysis and industrial fixation of CO2, and also provide effective methods for oxazolidin-2-ones and isochromans synthesis.

二氧化碳（CO2）既是主要的温室气体，也是地球上最多的碳源，将其转化为高附加值的化学品具有重大意义。CO2的化学转化通常需要高温、高压等苛刻条件，且产品结构十分局限。本项目针对以上问题，基于CO2的活化原理，设计合成高效的功能化多金属氧簇催化剂，优化配体、溶剂、温度、时间等实验参数，建立常压下催化转化CO2的新方法，构建具有重要价值的噁唑啉酮和异色满杂环化合物。通过现代核磁技术、光谱技术，重点研究多金属氧簇催化剂的组成、结构与催化性能之间的构效关系规律；结合同位素标记实验、量子化学计算等手段，研究多金属氧簇催化剂对CO2和有机反应底物双重活化的机理，为CO2的资源化利用提供科学依据和技术支撑。.本项目拓展多金属氧簇的催化应用的新领域、发展常压条件下CO2的催化转化方法；避免使用高压设备和有毒害的羰基化试剂，提供温和条件下合成噁唑啉酮和异色满的新方法，为CO2的工业化应用提供新思路。

杂多酸是一类廉价、绿色、易于合成的多金属氧簇。本项目设计合成绿色的功能化多金属氧簇催化剂，通过优化配体、溶剂、温度、时间等实验参数，建立温和条件下有机反应的催化转化新方法，构建具有重要价值的化合物。并通过现代核磁技术、光谱技术，研究多金属氧簇催化剂的组成、结构与催化性能之间的构效关系规律；结合同位素标记实验、量子化学计算等手段，研究多金属氧簇催化剂对有机反应底物活化的机理，为杂多酸的资源化利用提供科学依据和技术支撑。