新型手性含氮大环分子的不对称催化合成及在不对称催化反应中的应用

The design and synthesis of novel chiral ligands is the core research in the field of asymmetric catalysis. Due to the unique chemical and physical properties and rich metal coordination sites, the chiral macrocycles have emerged as a frontier and evolved into a hot topic of asymmetric catalysis in recent years. Now, it is highly desirable to develop new types of chiral macrocyclic ligands for asymmetric catalysis with high efficiency and high enantioselectivity. Unlike the traditional methods for the synthesis of chiral macrocycles, in this project, we will develop a new strategy for the design and synthesis of a novel series of chiral macrocyclic molecules via catalytic asymmetric hydrogenation. Moreover, the “macrocyclic effect” of achiral macrocycle substrates in asymmetric hydrogenation reaction will be studied. The synthesized chiral macrocycles will be characterized by using various instrumental techniques. Then, the synthesized chiral macrocyclic ligands will be utilized in enantioselective catalysis and nanocatalysis. In addition, the relationship between the structure of tunable chiral macrocyclic catalysis and the catalytic property will be systematically investigated. This research will further open up a new avenue for the fabrication and development of novel chiral macrocyclic ligands and promotes the development of supramolecular chemistry and asymmetric catalysis.

新型手性配体的设计合成是不对称催化研究的核心内容。近年来，手性大环配体由于其独特的化学特性和丰富的配位化学性能，引起了从事不对称催化合成工作者的广泛研究兴趣。发展一类全新骨架的、具有优异催化性能的手性大环配体分子一直是不对称催化研究的重要挑战。针对这一挑战性难题，本项目将突破传统手性大环分子的设计合成思路，拟建立与发展一种高效和实用的不对称催化氢化合成手性含氮大环化合物新策略，方便快捷地构筑一类结构新颖的手性含氮大环化合物。并系统研究非手性大环底物的“大环效应”在不对称氢化反应中的影响，揭示和总结出其影响规律和构效关系。在此基础上，详细研究所合成的手性含氮大环分子作为配体在不对称催化反应中的应用。此研究不仅为新型手性大环分子的构筑提供新的策略和途径，也为手性大环配体的设计拓展了思路，促进超分子化学和不对称催化研究的发展。