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

Research output: Contribution to journalArticleResearchpeer review

Authors

  • Valentina Jurkaš
  • Florian Weissensteiner
  • Piera De Santis
  • Stephan Vrabl
  • Frieda A. Sorgenfrei
  • Sarah Bierbaumer
  • Selin Kara
  • Robert Kourist
  • Pramod P. Wangikar
  • Christoph K. Winkler
  • Wolfgang Kroutil

External Research Organisations

  • University of Graz
  • Aarhus University
  • Graz University of Technology
  • Indian Institute of Technology Bombay (IITB)
  • BioTechMed Graz
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Details

Original languageEnglish
Article numbere202207971
JournalAngewandte Chemie - International Edition
Volume61
Issue number40
Early online date3 Aug 2022
Publication statusPublished - 26 Sept 2022
Externally publishedYes

Abstract

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.

Keywords

    Biocatalysis, Photocatalysis, Redox Chemistry, Reductions, Transmembrane Shuttling

ASJC Scopus subject areas

Cite this

Transmembrane Shuttling of Photosynthetically Produced Electrons to Propel Extracellular Biocatalytic Redox Reactions in a Modular Fashion. / Jurkaš, Valentina; Weissensteiner, Florian; De Santis, Piera et al.
In: Angewandte Chemie - International Edition, Vol. 61, No. 40, e202207971, 26.09.2022.

Research output: Contribution to journalArticleResearchpeer review

Jurkaš, V, Weissensteiner, F, De Santis, P, Vrabl, S, Sorgenfrei, FA, Bierbaumer, S, Kara, S, Kourist, R, Wangikar, PP, Winkler, CK & Kroutil, W 2022, 'Transmembrane Shuttling of Photosynthetically Produced Electrons to Propel Extracellular Biocatalytic Redox Reactions in a Modular Fashion', Angewandte Chemie - International Edition, vol. 61, no. 40, e202207971. https://doi.org/10.1002/anie.202207971, https://doi.org/10.1002/ange.202207971
Jurkaš, V., Weissensteiner, F., De Santis, P., Vrabl, S., Sorgenfrei, F. A., Bierbaumer, S., Kara, S., Kourist, R., Wangikar, P. P., Winkler, C. K., & Kroutil, W. (2022). Transmembrane Shuttling of Photosynthetically Produced Electrons to Propel Extracellular Biocatalytic Redox Reactions in a Modular Fashion. Angewandte Chemie - International Edition, 61(40), Article e202207971. https://doi.org/10.1002/anie.202207971, https://doi.org/10.1002/ange.202207971
Jurkaš V, Weissensteiner F, De Santis P, Vrabl S, Sorgenfrei FA, Bierbaumer S et al. Transmembrane Shuttling of Photosynthetically Produced Electrons to Propel Extracellular Biocatalytic Redox Reactions in a Modular Fashion. Angewandte Chemie - International Edition. 2022 Sept 26;61(40):e202207971. Epub 2022 Aug 3. doi: 10.1002/anie.202207971, 10.1002/ange.202207971
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abstract = "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.",
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note = "Funding Information: This project has received funding from the European Union's Horizon 2020 research and innovation program under the Marie Sk{\l}odowska‐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 Sk{\l}odowska-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: {\textcopyright} 2022 The Authors. Angewandte Chemie International Edition published by Wiley-VCH GmbH.",
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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.

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KW - Reductions

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