Modelling Photosynthesis with ZnII-Protoporphyrin All-DNA G-Quadruplex/Aptamer Scaffolds

Guo Feng Luo, Yonatan Biniuri, Wei Hai Chen, Jianbang Wang, Ehud Neumann, Henri Baptiste Marjault, Rachel Nechushtai, Martin Winkler, Thomas Happe, Itamar Willner*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

19 Scopus citations

Abstract

All-DNA scaffolds act as templates for the organization of photosystem I model systems. A series of DNA templates composed of ZnII-protoporphyrin IX (ZnIIPPIX)-functionalized G-quadruplex conjugated to the 3′- or 5′-end of the tyrosinamide (TA) aptamer and ZnIIPPIX/G-quadruplex linked to the 3′- and 5′-ends of the TA aptamer through a four-thymidine bridge. Effective photoinduced electron transfer (ET) from ZnIIPPIX/G-quadruplex to bipyridinium-functionalized tyrosinamide, TA-MV2+, bound to the TA aptamer units is demonstrated. The effectiveness of the primary ET quenching of ZnIIPPIX/G-quadruplex by TA-MV2+ controls the efficiency of the generation of TA-MV+.. The photosystem-controlled formation of TA-MV+. by the different photosystems dictates the secondary activation of the ET cascade corresponding to the ferredoxin-NADP+ reductase (FNR)-catalysed reduction of NADP+ to NADPH by TA-MV+., and the sequestered alcohol dehydrogenase catalysed reduction of acetophenone to 1-phenylethanol by NADPH.

Original languageAmerican English
Pages (from-to)9163-9170
Number of pages8
JournalAngewandte Chemie - International Edition
Volume59
Issue number23
DOIs
StatePublished - 2 Jun 2020

Bibliographical note

Publisher Copyright:
© 2020 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim

Keywords

  • artificial photosynthesis
  • electron transfer
  • energy conversion
  • ferredoxin-NADP reductase
  • nanobiotechnology

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