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WIREs Nanomed Nanobiotechnol
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Controlling self‐assembly of DNA‐polymer conjugates for applications in imaging and drug delivery

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Amphiphilic supramolecular structures such as micelles and vesicles can be formed through phase‐driven self‐assembly of monomer units having discrete hydrophilic and hydrophobic blocks. These structures show great promise for use in medical and biological applications, and incorporating DNA as the hydrophilic block of the amphiphilic monomers enables the creation of assemblies that also take advantage of the unique information storage and molecular recognition capabilities of DNA. Recently, significant advances have been made in the synthesis of DNA‐polymer conjugates (DPCs), controlling the morphology of DPC assemblies by altering monomer structure, and probing the effect of assembly on DNA stability and hybridization. Together, these investigations have laid the framework for using DPCs in drug delivery, cellular imaging, and other applications in materials science and chemistry. WIREs Nanomed Nanobiotechnol 2015, 7:282–297. doi: 10.1002/wnan.1309 This article is categorized under: Diagnostic Tools > Biosensing Biology-Inspired Nanomaterials > Lipid-Based Structures Biology-Inspired Nanomaterials > Nucleic Acid-Based Structures
DNA‐polymer conjugate (DPC) monomers can self‐assemble to provide a variety of architectures including micelles, vesicles, and tubes.
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Co‐assembly of FAM‐labeled micelles with DPC micelles encoding the nucleolin aptamer enables selective uptake by and imaging of cancer cells. (Reprinted with permission from Ref . Copyright 2014 American Chemical Society)
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Cellular imaging using DNA‐polymer conjugates (DPCs). (a) mRNA detection using molecular beacons; (b) ATP detection using aptamer beacons. In both DPC motifs, binding of the target moves the fluorophore away from the quencher, resulting in an increase in fluorescence emission.
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Addition of a complementary DNA strand compacts the hydrophobic core of the DPC, triggering release of paclitaxel.
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Hybridization of a PEG‐modified DNA strand increases the biocompatibility of DPC assemblies. The PEG‐modified strand can be removed by addition of a complementary nucleic acid.
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DNA properties can be altered by assembly into DPCs. (a) Terminal mismatches prevent aggregation at high ionic strength and (b) DPC assembly hinders cleavage of DNA by nucleases.
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Stimuli‐responsive changes to assembly morphology. (a) Enzymatic cleavage and addition of a complementary DNA strand enables switching between micelles and tubes (adapted with permission from Wiley). (b) Addition of a long complementary DNA strand transforms micelles into ladder structures (adapted with permission from Wiley). (c) Changing solvent polarity enables switching between micelles and tubes; (d) pH‐dependent formation of an i‐motif.
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DPCs are capable of disassembly or morphology change in response to reducing temperature below the LCST of the thermoresponsive polymer, re‐hybridizing one of the DNA strands to a complementary nucleic acid, or cleaving the disulfide bonds connecting the DNA to the polymer.
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As the monomer concentration is reduced below the CMC, the micelles dissociate. However, cross‐linking of the polymer segments stabilizes the micelle assemblies, preventing dissociation at low concentrations.
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General methods for the synthesis of DNA‐polymer conjugates (DPCs): (a) independent synthesis of DNA and polymer followed by solution‐phase conjugation; (b) attachment of the polymer to DNA during solid‐phase DNA synthesis; (c) incorporation of an initiator during solid‐phase DNA synthesis followed by polymer growth.
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Diagnostic Tools > Biosensing
Biology-Inspired Nanomaterials > Lipid-Based Structures
Biology-Inspired Nanomaterials > Nucleic Acid-Based Structures

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