Autonomous and programmable reorganization of DNA-based polymers using redox chemistry

14 July 2022, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

We demonstrate here a strategy that allows the programmable and autonomous reorganization of self-assembled DNA polymers using redox chemistry. We have rationally designed different DNA monomers (tiles) that can co-assemble into tubular structures. The tiles can be orthogonally activated/deactivated with disulfide-linked DNA fuel strands that are degraded over time upon reduction because of the presence of a reducing agent in the system. The concentration of the disulfide fuels determines the activation kinetics of each DNA tile, which controls the degree of order/disorder in the formed co-polymer. The disulfide-reduction pathway can be employed together with enzymatic fuel-degradation pathways providing an additional level of control in the re-organization of DNA structures. Taking advantage of the different pH-sensitivities of disulfide-thiol and enzymatic reactions, we show that we can control the order in DNA-based co-polymers as a function of pH.

Keywords

DNA Nanotechnology
self-assembly
disulfide
supramolecular chemistry
polymers

Supplementary materials

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Supporting Information
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Experimental procedures, simulations and predictions, supplementary figures
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