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Bottom-Up Assembly of DNA-Silica Nanocomposites into Micrometer-Sized Hollow Spheres.

ABSTRACT: Although DNA nanotechnology has developed into a highly innovative and lively field of research at the interface between chemistry, materials science, and biotechnology, there is still a great need for methodological approaches for bridging the size regime of DNA nanostructures with that of micrometer- and millimeter-sized units for practical applications. We report on novel hierarchically structured composite materials from silica nanoparticles and DNA polymers that can be obtained by self-assembly through the clamped hybridization chain reaction. The nanocomposite materials can be assembled into thin layers within microfluidically generated water-in-oil droplets to produce mechanically stabilized hollow spheres with uniform size distributions at high throughput rates. The fact that cells can be encapsulated in these microcontainers suggests that our concept not only contributes to the further development of supramolecular bottom-up manufacturing, but can also be exploited for applications in the life sciences.

SUBMITTER: Hu Y

PROVIDER: S-EPMC6900086 | biostudies-literature | 2019 Nov

REPOSITORIES: biostudies-literature

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Bottom-Up Assembly of DNA-Silica Nanocomposites into Micrometer-Sized Hollow Spheres.

Hu Yong Y Grösche Maximilian M Sheshachala Sahana S Oelschlaeger Claude C Willenbacher Norbert N Rabe Kersten S KS Niemeyer Christof M CM

Angewandte Chemie (International ed. in English) 20191018 48

Although DNA nanotechnology has developed into a highly innovative and lively field of research at the interface between chemistry, materials science, and biotechnology, there is still a great need for methodological approaches for bridging the size regime of DNA nanostructures with that of micrometer- and millimeter-sized units for practical applications. We report on novel hierarchically structured composite materials from silica nanoparticles and DNA polymers that can be obtained by self-asse ...[more]

PMID: 31625665

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Project description:A series of linear cationic diblock copolymer nanoparticles are prepared by polymerization-induced self-assembly (PISA) via reversible addition-fragmentation chain transfer (RAFT) aqueous dispersion polymerization of 2-hydroxypropyl methacrylate (HPMA) using a binary mixture of non-ionic and cationic macromolecular RAFT agents, namely poly(ethylene oxide) (PEO113, Mn = 4400 g mol-1; Mw/Mn = 1.08) and poly([2-(methacryloyloxy)ethyl]trimethylammonium chloride) (PQDMA125, Mn = 31?800 g mol-1, Mw/Mn = 1.19). A detailed phase diagram was constructed to determine the maximum amount of PQDMA125 stabilizer block that could be incorporated while still allowing access to a pure worm copolymer morphology. Aqueous electrophoresis studies indicated that zeta potentials of +35 mV could be achieved for such cationic worms over a wide pH range. Core cross-linked worms were prepared via statistical copolymerization of glycidyl methacrylate (GlyMA) with HPMA using a slightly modified PISA formulation, followed by reacting the epoxy groups of the GlyMA residues located within the worm cores with 3-aminopropyl triethoxysilane (APTES), and concomitant hydrolysis/condensation of the pendent silanol groups with the secondary alcohol on the HPMA residues. TEM and DLS studies confirmed that such core cross-linked cationic worms remained colloidally stable when challenged with either excess methanol or a cationic surfactant. These cross-linked cationic worms are shown to be much more effective bridging flocculants for 1.0 ?m silica particles at pH 9 than the corresponding linear cationic worms (and also various commercial high molecular weight water-soluble polymers.). Laser diffraction studies indicated silica aggregates of around 25-28 ?m diameter when using the former worms but only 3-5 ?m diameter when employing the latter worms. Moreover, SEM studies confirmed that the cross-linked worms remained intact after their adsorption onto the silica particles, whereas the much more delicate linear worms underwent fragmentation under the same conditions. Similar results were obtained with 4 ?m silica particles.

Dataset Information

Bottom-Up Assembly of DNA-Silica Nanocomposites into Micrometer-Sized Hollow Spheres.

Publications

Bottom-Up Assembly of DNA-Silica Nanocomposites into Micrometer-Sized Hollow Spheres.

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