Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 59, Issue 47, Pages 21058-21063Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202008007
Keywords
DNA devices; DNA nanotechnology; redox cycles; supramolecular chemistry; temporal control
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Funding
- European Research Council, ERC [336493]
- Associazione Italiana per la Ricerca sul Cancro, AIRC [14420]
- Italian Ministry of Health [GR-2010-2317212]
- Italian Ministry of University and Research (Project of National Interest, PRIN) [2012CTAYSY]
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Nature employs sulfur switches, that is, redox-active disulfides, to kinetically control biological pathways in a highly efficient and reversible way. Inspired by this mechanism, we describe herein a DNA-based synthetic nanodevice that acts as a sulfur switch and can be temporally controlled though redox regulation. To do this, we rationally designed disulfide DNA strands (modulators) that hybridize to a ligand-binding DNA nanodevice and act as redox-active allosteric regulators inducing the nanodevice to release or load its ligand. Upon reduction, the allosteric modulator spontaneously de-hybridizes from the nanodevice and, as a result, its effect is transient. The system is reversible and has an unprecedented high tolerance to waste products and displays transient behavior for over 40 cycles without significant loss of efficiency. Kinetic control of DNA-based ligand-binding nanodevices through purely chemical reactions paves the way for temporal regulation of more complex chemical pathways.
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