Adenosine
triphosphate (ATP) provides the driving force necessary
for critical biological functions in all living organisms. In synthetic
biocatalytic reactions, this cofactor is recycled in situ using high-energy stoichiometric reagents, an approach that generates
waste and poses challenges with enzyme stability. On the other hand,
an electrochemical recycling system would use electrons as a convenient
source of energy. We report a method that uses electricity to turn
over enzymes for ATP generation in a simplified cellular respiration
mimic. The method is simple, robust, and scalable, as well as broadly
applicable to complex enzymatic processes including a four-enzyme
biocatalytic cascade in the synthesis of the antiviral molnupiravir.