Merging transition metal-catalysis and electrochemistry for late stage functionalization of biologically active molecules

近年来，过渡金属催化的C-H官能化反应已被证明是革命性的，成千上万的出版物描述了无数的方案，包括交叉偶联反应，定向和非定向区域选择性C-C键形成（实现烷基化，烯基化和芳基化），以及复杂生物活性分子的选择性后期官能化。电化学自19世纪以来一直被使用，但直到最近才被大多数合成化学家视为晦涩难懂。在过去的15年里，电化学在合成界引起了新的兴趣，因为电化学设备变得更加标准化和易于使用，化学家们发现了利用电化学方法的令人兴奋的新型转化。与电化学相结合的过渡金属催化已成为C-H官能化的通用方法，并且处于研究理解的最前沿，能够实现以前未知的转化，同时消除对化学计量氧化剂和还原剂的需求，提高合成化学的可持续性。本论文详细介绍了为促进这一令人兴奋的现代化学领域所做的工作，通过开发电化学过渡金属催化的C-H功能化的新方法，用于生物活性分子的后期功能化

Transition-metal catalysed C-H functionalisation reactions have proven revolutionary in recent years, with thousands of publications describing myriad protocols including cross-coupling reactions, directed and non-directed regioselective C-C bond formation (achieving alkylation, alkenylation and arylation), and selective late-stage functionalisation of complex biologically active molecules. Electrochemistry has been utilised since the 1800s, but has largely been viewed by most synthetic chemists as obscure and inaccessible until only very recently. In the past 15 years, electrochemistry has enjoyed a surge of new-found interest within the synthesis community as electrochemistry equipment has become more standardised and accessible, with chemists discovering exciting novel transformations utilising electrochemical methods. Transition-metal catalysis integrated with electrochemistry has emerged as a versatile method for C-H functionalisation, and is at the forefront of research understanding, enabling previously unknown transformations while simultaneously removing the need for stoichiometric oxidants and reductants, improving the sustainability of synthetic chemistry. This thesis details work undertaken to contribute to this exciting modern field of chemistry, by developing new methods of electrochemical transition-metal catalysed C-H functionalisation for the late-stage functionalisation of biologically active molecules