TY - JOUR
T1 - Transmembrane Shuttling of Photosynthetically Produced Electrons to Propel Extracellular Biocatalytic Redox Reactions in a Modular Fashion
AU - Jurkaš, Valentina
AU - Weissensteiner, Florian
AU - De Santis, Piera
AU - Vrabl, Stephan
AU - Sorgenfrei, Frieda A.
AU - Bierbaumer, Sarah
AU - Kara, Selin
AU - Kourist, Robert
AU - Wangikar, Pramod P.
AU - Winkler, Christoph K.
AU - Kroutil, Wolfgang
N1 - Funding Information:
This project has received funding from the European Union's Horizon 2020 research and innovation program under the Marie Skłodowska‐Curie grant agreement No 764920. S.B. acknowledge the Austrian Science Fund (FWF) for funding within the project CATALOX (DOC 46‐B21). The COMET center: acib: Next Generation Bioproduction is funded by BMK, BMDW, SFG, Standortagentur Tirol, Government of Lower Austria und Vienna Business Agency in the framework of COMET—Competence Centers for Excellent Technologies. The COMET‐Funding Program is managed by the Austrian Research Promotion Agency FFG. The University of Graz and the Field of Excellence BioHealth are acknowledged for financial support. J. Schrittwieser is acknowledged for providing substrate.
Funding Information:
This project has received funding from the European Union's Horizon 2020 research and innovation program under the Marie Skłodowska-Curie grant agreement No 764920. S.B. acknowledge the Austrian Science Fund (FWF) for funding within the project CATALOX (DOC 46-B21). The COMET center: acib: Next Generation Bioproduction is funded by BMK, BMDW, SFG, Standortagentur Tirol, Government of Lower Austria und Vienna Business Agency in the framework of COMET—Competence Centers for Excellent Technologies. The COMET-Funding Program is managed by the Austrian Research Promotion Agency FFG. The University of Graz and the Field of Excellence BioHealth are acknowledged for financial support. J. Schrittwieser is acknowledged for providing substrate.
Publisher Copyright:
© 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.
PY - 2022/10/4
Y1 - 2022/10/4
N2 - 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.
AB - 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.
KW - Biocatalysis
KW - Photocatalysis
KW - Redox Chemistry
KW - Reductions
KW - Transmembrane Shuttling
UR - http://www.scopus.com/inward/record.url?scp=85137031837&partnerID=8YFLogxK
U2 - 10.1002/anie.202207971
DO - 10.1002/anie.202207971
M3 - Article
C2 - 35921249
AN - SCOPUS:85137031837
SN - 1433-7851
VL - 61
JO - Angewandte Chemie - International Edition
JF - Angewandte Chemie - International Edition
IS - 40
M1 - e202207971
ER -