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

碳-碳键的有效形成是有机分子合成的核心目标，这在整个社会的许多应用中都是必需的。虽然采用两种含有碳-金属或碳-卤素键的官能化起始材料的传统合成方法已经非常成功，但最近的研究集中在直接从两个碳-氢（C-H）键形成碳-碳键。这种C-H官能化反应具有更短的靶分子路线的优点（因为避免了官能化前体的预先制备）和产生更少的化学废物（因为在起始材料中存在的原子的较高比例最终在产物中）。在该研究方案中，我们的目标是开发通过由两个碳-氢键形成两个碳-碳键来形成环状（含环）有机分子的新方法。这些反应将通过少量的基于钌、铑、钯、镍或其他金属的金属催化剂来促进。以这种方式，可以快速且有效地制备多种可能有用的有机分子。这些反应中的许多具有形成多于一种产物的潜力，并且为了使效率最大化，将确定催化剂和反应条件以选择性地任意形成这些产物中的每一种。此外，一些反应有可能形成手性产物（具有不可重叠镜像的化合物）。在这些情况下，我们将确定手性催化剂，使选择性形成一个对映异构体超过其他。这方面是很重要的，因为功能分子（如药物或农用化学品）的不同对映体往往表现出不同的行为。这项研究将提供有价值的信息，可能有利于所有参与有机化合物合成的研究人员。我们希望能够建立可以在最初未预料到的情况下应用的概念，最终为科学和社会做出积极贡献。

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.