New Metal Catalysed Processes for the Rapid Construction of Functionalised Organic Architectures

由于在有机化学中使用金属介导的方法，在合成方面继续取得相当大的进展。近年来，斯特拉斯克莱德实验室内的一系列努力已经面向进一步的范围和合成效用的新金属介导的过程，直接应用于建立独特的成环策略和功能化的理想的有机框架。在这方面，最近，斯特拉斯克莱德的工作集中在新的手性镁双酰胺物种，（R2 N）2 Mg，作为不对称去质子化反应的潜在试剂。实际上，在制药和农业化学品加工方面，对映异构体富集产品的生产至关重要;这不仅是制造安全和适销对路的材料的关键，而且还导致在能源、溶剂和不需要的溶剂方面的浪费减少。除上述之外，最广泛应用的基于有机溶剂的方法之一是单步，环戊环化过程，Pauson-Khand（P-K）反应。近年来，我们实验室的研究一直集中在环化反应的发展上，试图找到更广泛适用的方法来促进这一重要的反应，并将此方法作为一系列天然产物系统合成中的中心转化。基于可靠的理论基础和一些非常有希望的初步结果，在本工作计划中，我们实验室正在开发的手性双酰胺镁试剂和Pauson-Khand方案都将作为关键的相互转化应用于合成具有潜在医学重要性和当前合成兴趣的要求高的分子结构。关于EPSRC组合，该计划的主要目标与催化，化学反应动力学和机制，合成有机化学的研究领域保持一致，并在医疗保健技术，物理科学和制造未来的主题中发挥重要作用。

Considerable advances in synthesis continue to be achieved due to the use of metal-mediated methods in organic chemistry. Over recent years, a series of endeavours within Strathclyde laboratories has been geared towards furthering the scope and synthetic utility of new metal-mediated processes for direct application towards the establishment of unique annulation strategies and functionalisation of desirable organic frameworks. In this respect and very recently, work at Strathclyde has focused on novel chiral magnesium bisamide species, (R2N)2Mg, as potential reagents for asymmetric deprotonation reactions. Indeed, in terms of pharmaceutical and agrochemical processes, the production of enantiomerically-enriched products is of paramount importance; not only is this key to the manufacture of safe and marketable materials but this also leads to less waste in terms of energy, solvents, and unwanted (enantiomeric) by-products.In addition to the above, one of the most widely applied organometal-based methods is the single-step, cyclopentannulation process, the Pauson-Khand (P-K) reaction. Over recent years, studies within our laboratories has been focused towards the development of this cyclisation, in attempts to find more widely applicable methods for facilitating this preparatively important reaction, and to applying this method as the central transformation within the syntheses of a spectrum of natural product systems.Based on sound theoretical underpinning and some highly promising preliminary results, within this programme of work both the chiral magnesium bisamide reagents and Pauson-Khand protocols being developed within our laboratory will find application as the key interconversion in the synthesis of demanding molecular architectures of potential medicinal importance and current synthetic interest. In relation to the EPSRC Portfolio, the main objectives of this programme align with and will address the Research Areas of Catalysis, Chemical Reaction Dynamics and Mechanism, and Synthetic Organic Chemistry and as of importance within the Themes of Healthcare Technologies, Physical Sciences, and Manufacturing the Future.