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

该项目旨在将酶和过渡金属催化结合在一个协同过程中，利用酶的选择性与过渡金属的多功能性相结合，为芳香化合物的区域选择性元功能化提供一种生物/化学合成工具。这将通过开发能够将CO2固定在芳香化合物所需位置的酶羧化酶来实现。然后过渡金属催化剂将利用这一基团，以控制任何所需功能的安装，随后去除CO2基团。在这个过程中，二氧化碳作为一个无迹可循的指导基团，酶对其选择性安装是整个转化选择性的关键。该项目将采用最先进的酶进化技术，以开发一套酶羧化酶，这些酶羧化酶能够在广泛的底物范围内工作，并且在适合与过渡金属催化剂结合使用的条件下工作。

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.