Redox-Switchable Binding Properties of the ATP-Aptamer

Yonatan Biniuri, Guo Feng Luo, Michael Fadeev, Verena Wulf, Itamar Willner*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review


In this study, we report on a redox-controllable and reversible complete "ON"/"OFF"-switchable aptamer binding to ATP. A series of methylene blue-modified ATP-aptamers was synthesized, revealing improved binding affinities toward ATP as compared to the nonmodified aptamer. These binding affinities were dependent on the conjugation site of the redox label on the aptamer scaffold. Importantly, we find that the oxidized methylene blue-modified aptamers bind to ATP with micromolar affinity, while the reduced form lacks binding affinity toward ATP, resulting in an unprecedented complete "ON"/"OFF" redox-controllable aptamer switch. We demonstrate the cyclic "ON"/"OFF" binding of ATP to the methylene blue-functionalized aptamer through cyclic oxidation and reduction of the redox label using both chemical and electrochemical means. Molecular dynamics and docking simulations were performed to account for the redox-switchable properties of the conjugated aptamers and to rationalize the enhanced binding affinities of the different aptamer designs.

Original languageEnglish
Pages (from-to)15567-15576
Number of pages10
JournalJournal of the American Chemical Society
Issue number39
StatePublished - 2 Oct 2019
Externally publishedYes


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