Silver-catalyzed C-H activation: design and development of novel catalytic systems for synthetic chemistry

该项目旨在将酶催化和过渡金属催化结合在一个协同过程中，利用酶的选择性和过渡金属的多功能性，为芳香族化合物的区域选择性歧化提供生物/化学合成工具。这将通过开发能够将二氧化碳固定在芳香化合物的所需位置的酶羧化酶来实现。然后，过渡金属催化剂将利用该基团来控制任何所需官能团的安装，然后去除二氧化碳基团。在这个过程中，CO2作为一个无痕迹的导向基团，其通过酶的选择性安装是整个转化的选择性的关键。该项目将采用最先进的酶进化技术，以开发一套能够在广泛的底物范围内工作，并在符合条件下与过渡金属催化剂一起使用的酶羧基酶。

This project aims at the marriage of enzymatic and transition metal catalysis in a synergistic process that exploits enzyme selectivity in combination with transition metal versatility, in order to afford a bio/chemosynthetic tool for the regioselective meta-functionalisation of aromatic compounds. This will be achieved by developing enzyme carboxylases capable of fixing CO2 at desired positions of aromatic compounds. This group will then be exploited by transition metal catalysts in order to control the installation of any desired functionality, followed by the removal of the CO2 group. In this process CO2 is acting as a traceless directing group whose selective installation by an enzyme is key to the selectivity of the overall transformation. This project will employ state-of-the-art enzyme evolution techniques in order to develop a set of enzyme carboxylases capable of operating on a broad substrate scope and under conditions amenable to their use in conjunction with transition metal catalysts.