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Polyelectrolyte Complexation of Oligonucleotides by Charged Hydrophobic—Neutral Hydrophilic Block Copolymers

Institute for Molecular Engineering, University of Chicago, Chicago, IL 60637, USA
Institute for Molecular Engineering at Argonne National Laboratory, Lemont, IL 60439, USA
Departments of Biology and Physics, Swarthmore College, Swarthmore, PA 19081, USA
Author to whom correspondence should be addressed.
Polymers 2019, 11(1), 83;
Received: 10 December 2018 / Revised: 1 January 2019 / Accepted: 2 January 2019 / Published: 7 January 2019
PDF [5846 KB, uploaded 7 January 2019]


Polyelectrolyte complex micelles (PCMs, core-shell nanoparticles formed by complexation of a polyelectrolyte with a polyelectrolyte-hydrophilic neutral block copolymer) offer a solution to the critical problem of delivering therapeutic nucleic acids, Despite this, few systematic studies have been conducted on how parameters such as polycation charge density, hydrophobicity, and choice of charged group influence PCM properties, despite evidence that these strongly influence the complexation behavior of polyelectrolyte homopolymers. In this article, we report a comparison of oligonucleotide PCMs and polyelectrolyte complexes formed by poly(lysine) and poly((vinylbenzyl) trimethylammonium) (PVBTMA), a styrenic polycation with comparatively higher charge density, increased hydrophobicity, and a permanent positive charge. All of these differences have been individually suggested to provide increased complex stability, but we find that PVBTMA in fact complexes oligonucleotides more weakly than does poly(lysine), as measured by stability versus added salt. Using small angle X-ray scattering and electron microscopy, we find that PCMs formed from both cationic blocks exhibit very similar structure-property relationships, with PCM radius determined by the cationic block size and shape controlled by the hybridization state of the oligonucleotides. These observations narrow the design space for optimizing therapeutic PCMs and provide new insights into the rich polymer physics of polyelectrolyte self-assembly. View Full-Text
Keywords: polyelectrolytes; complex coacervation; oligonucleotides; phase separation; nanoparticles polyelectrolytes; complex coacervation; oligonucleotides; phase separation; nanoparticles

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This is an open access article distributed under the Creative Commons Attribution License which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited (CC BY 4.0).

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Marras, A.E.; Vieregg, J.R.; Ting, J.M.; Rubien, J.D.; Tirrell, M.V. Polyelectrolyte Complexation of Oligonucleotides by Charged Hydrophobic—Neutral Hydrophilic Block Copolymers. Polymers 2019, 11, 83.

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