Autonomous and Programmable Reorganization of DNA‐Based Polymers Using Redox Chemistry

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...

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Bibliographic Details
Published in:Chemistry : a European journal 2023-05, Vol.29 (30), p.e202300394-n/a
Main Authors: Gentile, Serena, Del Grosso, Erica, Prins, Leonard J., Ricci, Francesco
Format: Article
Language:English
Subjects:
Chemistry
Deoxyribonucleic acid
Disulfides
DNA
DNA - chemistry
DNA nanostructures
DNA nanotechnology
DNA polymers
Fuels
Kinetics
Monomers
Nanostructures - chemistry
Nanotechnology
Nucleic Acid Conformation
Oxidation-Reduction
Polymers
reconfiguration
redox chemistry
Reducing agents
Self-assembly
Tiles
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Summary: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. Programmable DNA assembly: Here we have rationally re‐engineered DNA tiles that can co‐assemble into tubular structures and can be orthogonally deactivated/re‐activated with redox‐controlled DNA fuel strands. By controlling the relative rate of re‐assembly of each tile, we can regulate the tiles distribution in the final co‐polymer. The approach can be coupled with enzymatic fuel‐degradation reactions and responds to external stimuli (i. e., pH) providing an additional level of control in the reconfiguration of DNA‐polymers.
ISSN:0947-6539
1521-3765
DOI:10.1002/chem.202300394