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Transmembrane Shuttling of Photosynthetically Produced Electrons to Propel Extracellular Biocatalytic Redox Reactions in a Modular Fashion

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  • Valentina Jurkas, University of Graz
  • ,
  • Florian Weissensteiner, University of Graz
  • ,
  • Piera De Santis, University of Graz
  • ,
  • Stephan Vrabl, University of Graz
  • ,
  • Frieda A. Sorgenfrei, University of Graz
  • ,
  • Sarah Bierbaumer, University of Graz
  • ,
  • Selin Kara
  • Robert Kourist, Graz University of Technology
  • ,
  • Pramod P. Wangikar, Indian Institute of Technology (BHU), Varanashi
  • ,
  • Christoph K. Winkler, University of Graz
  • ,
  • Wolfgang Kroutil, University of Graz

Many biocatalytic redox reactions depend on the cofactor NAD(P)H, which may be provided by dedicated recycling systems. Exploiting light and water for NADPH-regeneration as it is performed, e.g. by cyanobacteria, is conceptually very appealing due to its high atom economy. However, the current use of cyanobacteria is limited, e.g. by challenging and time-consuming heterologous enzyme expression in cyanobacteria as well as limitations of substrate or product transport through the cell wall. Here we establish a transmembrane electron shuttling system propelled by the cyanobacterial photosynthesis to drive extracellular NAD(P)H-dependent redox reactions. The modular photo-electron shuttling (MPS) overcomes the need for cloning and problems associated with enzyme- or substrate-toxicity and substrate uptake. The MPS was demonstrated on four classes of enzymes with 19 enzymes and various types of substrates, reaching conversions of up to 99 % and giving products with >99 % optical purity.

Original languageEnglish
Article numbere202207971
JournalAngewandte Chemie
Volume61
Issue40
Number of pages10
ISSN0044-8249
DOIs
Publication statusPublished - Oct 2022

Bibliographical note

© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.

    Research areas

  • Biocatalysis, Photocatalysis, Redox Chemistry, Reductions, Transmembrane Shuttling

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