摘要/Abstract
烯烃的不对称氢官能团化是一个重要的研究方向.从简单的烯烃原料出发,通过该方法可以高效构建手性分子.多取代烯烃的不对称氢官能团化仍然是一个挑战.一方面,烯烃有两个反应位点,反应的区域选择性需要进行有效的控制.另一方面,如果反应生成了多个手性中心,则涉及到非对映选择性的控制.此外,还需要控制反应的对映选择性.因此,此类研究的关键在于如何发展有效的催化体系,以同时实现区域选择性、非对映选择性及对映选择性的高效控制.针对这一问题,我们采用配位辅助策略,利用底物中的配位基团及烯烃与金属中心形成双位点配位模式,从而有效控制烯烃转化的区域选择性及立体选择性.以烯烃不对称炔氢化作为模型转化,以研究多取代烯烃催化不对称转化中的选择性控制.
关键词: 烯烃转化, 不对称催化, 选择性, 配位辅助, 过渡金属催化
Catalytic asymmetric hydrofunctionalization of alkene is an important research field, which enables efficient construction of chiral molecules from readily available starting materials. Asymmetric hydrofunctionalization of multiple substituted alkenes represents a significant challenge to organic chemists because this process involves the simutaneous control of regio-, diastereo-, and enantio-selectivities. The key to solve this challenge is to identify novel catalyst systems to exert powerful regio- and stereo-control. Recently, by taking advantage of substrate-directed strategy, we have developed a number of alkene functionalization methods with excellent regio-, diastereo-, and enantio-selectivities. In particular, we focus on catalytic asymmetric hydroalkynylation of alkenes as a model transformation to analyze the factors that control the selectivity.
Key words: alkene functionalization, asymmetric catalysis, selectivity, substrate-directed strategy, transition metal catalysis
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