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，在社会上的许多应用中都是必需的。例如，传统的合成方法采用两种含有碳-金属或碳-卤素键的功能化起始材料，已经非常成功，而最近的研究则集中在直接由两个碳氢键形成碳-碳键。这样的碳氢功能化反应具有到目标分子的路线较短（因为避免了预先制备功能化前体）和产生较少化学废物的优点（因为初始材料中存在的更高比例的原子最终进入了产品）。在这个研究项目中，我们的目标是开发新的方法，通过两个碳氢键形成两个碳碳键来形成环状（含环）有机分子。这些反应可以通过少量的钌、铑、钯、镍或其他金属催化剂来促进。通过这种方法，可以快速有效地制备各种可能有用的有机分子。这些反应中的许多都有可能形成不止一种产物，为了最大限度地提高效率，将确定催化剂和反应条件，以选择性地形成每种产物。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，我们将识别手性催化剂，使一种对映体的选择性形成。这方面很重要，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。这项研究将为所有从事有机化合物合成的研究人员提供有价值的信息。我们希望能够建立能够应用于最初意想不到的环境的概念，最终为科学和社会提供积极的贡献。

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.