Artificial Photosynthesis with Electron Acceptor/Photosensitizer-Aptamer Conjugates

Guo Feng Luo, Yonatan Biniuri, Wei Hai Chen, Ehud Neumann, Michael Fadeev, Henri Baptiste Marjault, Anjan Bedi, Ori Gidron, Rachel Nechushtai, David Stone, Thomas Happe, Itamar Willner*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

12 Scopus citations

Abstract

Sequence-specific aptamers act as functional scaffolds for the assembly of photosynthetic model systems. The Ru(II)-tris-bipyridine photosensitizer is conjugated by different binding modes to the antityrosinamide aptamer to yield a set of photosensitizer-aptamer binding scaffolds. The N-methyl-N′-(3-aminopropane)-4,4′-bipyridinium electron acceptor, MV2+, is covalently linked to tyrosinamide, TA, to yield the conjugate TA-MV2+. The tyrosinamide unit in TA-MV2+ acts as a ligand for anchoring TA-MV2+ to the Ru(II)-tris-bipyridine-aptamer scaffold, generating the diversity of photosensitizer-aptamer/electron acceptor supramolecular conjugates. Effective electron transfer quenching in the photosynthetic model systems is demonstrated, and the quenching efficiencies are controlled by the structural features of the conjugates. The redox species generated by the photosensitizer-aptamer/electron acceptor supramolecular systems mediate the ferredoxin-NADP+ reductase, FNR, catalyzed synthesis of NADPH, and the Pt-nanoparticle-catalyzed evolution of hydrogen (H2). The novelty of the study rests on the unprecedented use of aptamer scaffolds as functional units for organizing photosynthetic model systems.

Original languageAmerican English
Pages (from-to)6621-6628
Number of pages8
JournalNano Letters
Volume19
Issue number9
DOIs
StatePublished - 11 Sep 2019

Bibliographical note

Publisher Copyright:
© 2019 American Chemical Society.

Keywords

  • Electron transfer
  • H-evolution
  • NADPH
  • biocatalysis
  • nucleic acid

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