New Catalytic C-H Functionalisations and Oxidative Annulations for Chemical Synthesis

点击翻译按钮获取中文摘要

The efficient formation of carbon-carbon bonds is a central objective in the synthesis of organic molecules, which are required in numerous applications across society. While traditional synthetic methods employing two functionalised starting materials containing carbon-metal or carbon-halogen bonds, for example, have been highly successful, more recent research has focused on forming carbon-carbon bonds directly from two carbon-hydrogen (C-H) bonds. Such C-H functionalisation reactions have the advantages of shorter routes to target molecules (as prior preparation of functionalised precursors is avoided) and the generation of less chemical waste (since a higher proportion of atoms present in the starting materials ends up in the products).In this research programme, we aim to develop new methods to form cyclic (ring-containing) organic molecules by the formation of two carbon-carbon bonds from two carbon-hydrogen bonds. These reactions will be promoted by small quantities of metal catalysts based around ruthenium, rhodium, palladium, nickel, or other metals. In this way, a diverse range of potentially useful organic molecules may be prepared rapidly and efficiently. Many of these reactions have the potential to form more than one product, and in order to maximise efficiency, catalysts and reaction conditions will be identified to form each of those products selectively, at will. Furthermore, some of the reactions have the potential to form chiral products (compounds that have non-superimposable mirror images). In these cases, we will identify chiral catalysts that enable the selective formation of one enantiomer over the other. This aspect is important, since different enantiomers of functional molecules (such as medicines or agrochemicals) often display different behaviours.This research will provide valuable information that could be of benefit to all researchers involved in the synthesis of organic compounds. We hope to be able to establish concepts that can be applied in initially unanticipated contexts, ultimately providing positive contributions to science and society.