Reaction Engineering and Comparison of Electroenzymatic and Enzymatic ATP Regeneration Systems

TL;DR

This paper develops an electroenzymatic ATP regeneration system that enhances biocatalytic efficiency, surpassing traditional methods, and broadens application scope through enzyme system expansion.

Contribution

It introduces a novel electroenzymatic ATP regeneration method with superior performance metrics and compares it to existing systems, also expanding functionality with a new enzyme.

Findings

Achieved 84% yield of mevalonate phosphate

Total turnover number for ADP reached 68

System outperforms many enzymatic ATP regeneration methods

Abstract

Adenosine-5'-triphosphate (ATP) plays a crucial role in many biocatalytic reactions and its regeneration can influence the performance of a related enzymatic reaction significantly. Here, we established an electrochemically coupled ATP regeneration by pyruvate oxidase and acetate kinase (ACK) for the phosphorylation of mevalonate catalyzed by mevalonate kinase. A yield of 84% for the product mevalonate phosphate was reached and a total turnover number for ADP of 68. These metrics are promising for the development of an economic feasible bioprocess and surpass many other enzymatic ATP regeneration systems. A comparison was made to polyphosphate kinases (PPKs), ACK, pyruvate kinase, and creatine kinase in terms of the phosphate donor properties and biocatalytic metrics of exemplary reactions. Furthermore, our system was expanded by a PPK that enables the phosphorylation of AMP, which can broaden the spectrum of applications even further.