New Ruthenium Catalysts for C-C bond Formation: A Combined Experimental and Theoretical Approach

新型化合物的制备是现代社会各种重要材料发展的重要组成部分，如医药、农用制剂、塑料等。这些应用中的大多数化合物都是以碳元素为基础的，需要新的有效方法来形成新的碳-碳和碳-X(其中X是不同的元素)。最重要的是，在形成新的碳-碳和碳-X键的现代技术中，使用过渡金属化合物作为催化剂(即，提高给定反应的速度和可能的效率的添加剂)。基于一系列金属，特别是钯、Ru和钼，开发出了成功和广泛使用的催化剂，在这一领域的工作使理查德·施罗克、罗伯特·格拉布斯和伊夫·肖文获得了2005年诺贝尔奖。该项目的目的是深入了解一系列较少使用的催化剂。我们将要开发的化合物已经被证明能够帮助形成一系列新的碳-碳和碳-X键，然而，它们有几个缺点--例如经常需要大量的催化剂，并且必须使用高温。该项目将需要深入研究利益反应的基本步骤，这将使用双管齐下的攻击。首先，将进行一系列实验研究，为这些反应的性质提供直接证据。其次，同时，将使用一系列高水平的理论计算来从不同的角度提供见解。这个项目成功的关键将是理论和实验方案之间的协同作用，因为每个方案都将提供有关正在研究的反应的重要信息，并为另一个方案的发展提供信息。最终，这项研究将导致开发新的催化剂和新的合成反应，使新化合物的形成变得容易，并应用于例如制药和农业工业。

The preparation of novel chemical compounds forms a fundamental part of the development of a wide range of important materials in modern society such as pharmaceuticals, agricultural agents, plastics etc. The majority of compounds for these applications are based on the element carbon and new and efficient ways to form new carbon-carbon and carbon-X (where X is a different element) are required. Foremost amongst the modern techniques to form new carbon-carbon and carbon-X bonds use transition metal compounds as catalysts (i.e. additives which increase the speed and possibly the efficiency of a given reaction). Successful and widely used catalysts have been developed based on a range of metals, notably palladium, ruthenium and molybdenum, and work in this area resulted in the award of the 2005 Noble Prize to Richard Schrock, Robert Grubbs and Yves Chauvin. The aim of this project is to develop an in-depth understanding of a series of less well used catalysts. The compounds which we will develop have been shown to be capable of assisting in the formation of a range of new carbon-carbon and carbon-X bonds, however, they have several drawbacks - such as a large amount of catalyst is often required and high temperatures must be employed. The project will entail an in-depth study of the fundamental steps of the reactions of interest which will use a two pronged attack. Firstly a series of experimental studies will be performed which will provide direct evidence about the nature of these reactions. Secondly, and simultaneously, a series of high-level theoretical calculations will be employed to provide insight from a different perspective. The key to the success of this project will be the synergy between the theoretical and experimental programmes as each will provide important information about the reactions under study and inform the development of the other.Ultimately, this research will result in the development of new catalysts and new synthetic reactions that will enable the facile formation of new compounds with applications in, for example, the pharmaceutical and agricultural industries.