Chemo- and biocatalytic cascades for the production of industrially relevant molecules

将生物催化和传统化学催化剂结合到一锅级联反应中，可以实现单独使用一种催化体系无法实现的高效分子转化。它们允许快速建立分子复杂性，同时减少与分离和纯化中间体相关的时间、精力和浪费。副产物和不稳定或危险中间体的问题也可以避免，反应通常可以在水介质中进行。在这项工作中，级联反应将被开发，允许访问工业相关的基序。第一个项目使用腈酶与光催化脱羧功能化相结合，从腈开始生产氟化和三氟甲基化化合物。剩下的工作集中在利用酶级联形成酰胺键，包括酰胺键合成酶、atp抓住连接酶和腈酶。

Combining biocatalysis and traditional chemical catalysts into one-pot cascade reactions allows efficient molecular transformations that could not be achieved using one catalytic regime alone. They allow rapid build-up of molecular complexity whilst reducing the time, effort, and waste associated with isolation and purification of intermediates. Problems with side-products and unstable or dangerous intermediates can also be circumvented, and reactions can often be carried out in aqueous media. In this work, cascade reactions will be developed which allow access to industrially relevant motifs. The first project uses nitrilase enzymes combined with photocatalytic decarboxylative functionalisations to produce fluorinated and trifluoromethylated compounds, starting from nitriles. The remainder of the work focuses on the formation of amide bonds using enzymatic cascades which include amide bond synthetases, ATP-grasp ligases, and nitrilases.