Directional Preference of DNA-Mediated Electron Transfer in Gold-Tethered DNA Duplexes: Is DNA a Molecular Rectifier?

László Kékedy-Nagy, Elena E. Ferapontova*

*Corresponding author for this work

Research output: Contribution to journal/Conference contribution in journal/Contribution to newspaperJournal articleResearchpeer-review

Abstract

Electrical properties of self-assembling DNA nanostructures underlie the paradigm of nanoscale bioelectronics, and as such require clear understanding. DNA-mediated electron transfer (ET) from a gold electrode to DNA-bound Methylene Blue (MB) shows directional preference, and it is sequence-specific. During the electrocatalytic reduction of [Fe(CN) 6 ] 3− catalyzed by DNA-bound MB, the ET rate constant for DNA-mediated reduction of MB reaches (1.32±0.2)10 3 and (7.09±0.4)10 3 s −1 for (dGdC) 20 and (dAdT) 25 duplexes. The backward oxidation process is less efficient, making the DNA duplex a molecular rectifier. Lower rates of ET via (dGdC) 20 agree well with its disturbed π-stacked sub-molecular structure. Such direction- and sequence-specific ET may be implicated in DNA oxidative damage and repair, and be relevant to other polarized surfaces, such as cell membranes and biomolecular interfaces.

Original languageEnglish
JournalAngewandte Chemie - International Edition
Volume58
Issue10
Pages (from-to)3048-3052
Number of pages5
ISSN1433-7851
DOIs
Publication statusPublished - 2019

Keywords

  • DNA
  • electrocatalysis
  • electron transfer
  • gold electrodes
  • Methylene Blue

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