Catalysis

Electrochemical Recycling of Adenosine Triphosphate in Biocatalytic Reaction Cascades

Authors

  • Serge Ruccolo Process Research and Development, Merck & Co., Inc. ,
  • Gilmar Brito Process Research and Development, Merck & Co., Inc. ,
  • Melodie Christensen Process Research and Development, Merck & Co., Inc. ,
  • Tetsuji Itoh Process Research and Development, Merck & Co., Inc. ,
  • Keith Mattern Process Research and Development, Merck & Co., Inc. ,
  • Kevin Stone Process Research and Development, Merck & Co., Inc. ,
  • Neil Strotman Process Research and Development, Merck & Co., Inc. ,
  • Alexandra Sun Process Research and Development, Merck & Co., Inc.

Abstract

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 and downstream purification. On the other hand, electrons are a cheap and green source of energy. We report a method that uses electricity to turn over enzymes for ATP generation. 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.

Content

Thumbnail image of BioechemATP_25052022.pdf

Supplementary material

Thumbnail image of Supporting Information_25042022.docx
Supporting information
Contains all supplementary materials: Chemicals and Materials, Enzyme Acquisition, Enzyme Purification, Analytical Instrumentation, Electrolysis Equipment, HPLC analytical method, Determination of Conversion and Faradaic Efficiency, UV-Vis Determination of FAD:PO ratio, Electrochemical Studies, Bioelectrochemical stoichiometric ATP formation, Bioelectrochemical glycosylation, Reaction scope, Amino acid and DNA sequences of the enzymes and References.