Powering Artificial Enzymatic Cascades with Electrical Energy

We have developed a scalable platform that employs electrolysis for an in vitro synthetic enzymatic cascade in a continuous flow reactor. Both H 2 and O 2 were produced by electrolysis and transferred through a gas‐permeable membrane into the flow system. The membrane enabled the separation of the electrolyte from the biocatalysts in the flow system, where H 2 and O 2 served as electron mediators for the biocatalysts. We demonstrate the production of methylated N‐heterocycles from diamines with up to 99 % product formation as well as excellent regioselective labeling with stable isotopes. Our platform can be applied for a broad panel of oxidoreductases to exploit electrical energy for the synthesis of fine chemicals.