Reversible multilayered vesicle-like structures with fluid hydrophobic and interpolyelectrolyte layers
Murmiliuk A. Filippov S.K. Rud O. Košovan P. Tošner Z. Radulescu A. Skandalis A. Pispas S. Šlouf M. Štěpánek M.
October 2021Academic Press Inc.
Journal of Colloid and Interface Science
2021#599313 - 325 pp.
Hydrophobic blocks of amphiphilic block copolymers often form glassy micellar cores at room temperature with a rigid structure that limits their applications as nanocapsules for targeted delivery. Nevertheless, we prepared and analyzed core/shell micelles with a soft core, formed by a self-assembled block copolymer consisting of a hydrophobic block and a polycation block, poly(lauryl acrylate)-block-poly(trimethyl-aminoethyl acrylate) (PLA-QPDMAEA), in aqueous solution. By light and small-angle neutron scattering, by transmission electron microscopy and by fluorescence spectroscopy, we showed that these core/shell micelles are spherical and cylindrical with a fluid-like PLA core and a positively charged outer shell and that they can encapsulate and release hydrophobic solutes. Moreover, after mixing these PLA-QPDMAEA core/shell micelles with another diblock copolymer, consisting of a hydrophilic block and a polyanion block, namely poly(ethylene oxide)-block-poly(methacrylic acid) (PEO-PMAA), we observed the formation of novel vesicle-like multicompartment structures containing both soft hydrophobic and interpolyelectrolyte (IPEC) layers. By combining small-angle neutron scattering with self-consistent field modeling, we confirmed the formation of these complex vesicle-like structures with a swollen PEO core, an IPEC inner layer, a PLA soft layer, an IPEC outer layer and a loose PEO corona. Thus, these multicompartment micelles with fluid and IPEC layers and a hydrophilic corona may be used as nanocapsules with several tunable properties, including the ability to control the thickness of each layer, the charge of the IPEC layers and the stability of the micelles, to deliver both hydrophobic and multivalent solutes.
Block polyelectrolytes , Core/shell particles , Electrostatic coassembly , Small-angle scattering
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Department of Physical and Macromolecular Chemistry, Faculty of Science, Charles University, Hlavova 8, 128 00, Prague 2, Czech Republic
Pharmaceutical Sciences Laboratory, Faculty of Science and Engineering, Åbo Akademi University, Turku, 20520, Finland
Forschungszentrum Jülich GmbH, Jülich Centre for Neutron Science@MLZ, Lichtenbergstraße 1, Garching, D-85747, Germany
Theoretical and Physical Chemistry Institute, National Hellenic Research Foundation, 48 Vassileos Constantinou Avenue, Athens, 11635, Greece
Institute of Macromolecular Chemistry, Czech Academy of Sciences, Heyrovského náméstí 2, Prague 6, 162 06, Czech Republic
Department of Chemistry and Chemical Technology, Al-Farabi Kazakh National University, Almaty, 050040, Kazakhstan
Department of Physical and Macromolecular Chemistry
Pharmaceutical Sciences Laboratory
Forschungszentrum Jülich GmbH
Theoretical and Physical Chemistry Institute
Institute of Macromolecular Chemistry
Department of Chemistry and Chemical Technology
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