Abstract
We report on the preparation of novel and multifunctional hybrid spherical-shaped nanostructures involving a double-hydrophilic block copolymer, namely the neutral cationic poly[oligo(ethylene glycol) methacrylate]-b-poly[(vinyl benzyl trimethylammonium chloride)] (POEGMA-b-PVBTMAC) diblock copolymer, initially complexed with hydrophilic anionic magnetic nanoparticles (MNPs), and subsequently, with short deoxyribonucleic acid (113 bases DNA). The POEGMA-b-PVBTMAC copolymer, the copolymer/MNPs and the copolymer/MNPs/DNA tricomponent hybrid electrostatic complexes were studied by dynamic/electrophoretic light scattering (DLS/ELS) and cryogenic transmission electron microscopy (cryo-TEM) techniques for the determination of their structure and solution properties. The MNPs were complexed efficiently with the oppositely charged diblock chains, leading to well-defined hybrid organic–inorganic spherical-shaped nanostructures. A significant aggregation tendency of the MNPs is noticed in cryo-TEM measurements after the electrostatic complexation of DNA, implying an accumulation of the DNA macromolecules on the surface of the hybrid tricomponent complexes. Magnetophoretic experiments verified that the MNPs maintain their magnetic properties after the complexation initially with the copolymer, and subsequently, within the block polyelectrolyte/MNPs/DNA nanostructures.
Highlights
Polymeric theranostics that can deliver imaging and therapeutic agents simultaneously are being intensively developed to achieve dual-functionality for the treatment of threatening disorders.A plethora of scientific papers has been published to provide multi-functionality in treatment applications [1,2,3,4,5,6,7,8]
We developed multifunctional hybrid spherical-shaped nanostructures utilizing a biocompatible double hydrophilic block copolymers (DHBCs) synthesized by Reversible Addition–Fragmentation Chain Transfer (RAFT) polymerization, namely the poly[oligo(ethylene glycol) methacrylate]-b-poly[(vinyl benzyl trimethylammonium chloride)] (POEGMA-b-PVBTMAC), as the base for electrostatic complexation initially with hydrophilic magnetic nanoparticles (MNPs), and subsequently, incorporating a short DNA
DLS and X-ray diffraction (XRD) measurements implemented to assess the size and the crystalline structure of the CoFe2 O4 NPs are presented in the Supplementary Material (SM) in Figures S1 and S2 [41]
Summary
Polymeric theranostics that can deliver imaging and therapeutic agents simultaneously are being intensively developed to achieve dual-functionality for the treatment of threatening disorders. A polyelectrolyte block incorporated in DHBCs has the ability to interact/complex with oppositely charged components, such as imaging agents or biomacromolecules, while the neutral hydrophilic blocks promote solubilization in water and provide stabilization of the formed hybrid nanostructures in aqueous dispersions [17,18,19]. Magnetic nanoparticles (MNPs) have been used in a multitude of biomedical applications including magnetic resonance imaging (as negative contrast agents), gene therapy, targeted drug delivery, and magnetic hyperthermia treatment (under alternating magnetic fields) [22,23,24,25,26], rendering them ideal for the design of hybrid nanostructures based on polymers. We developed multifunctional hybrid spherical-shaped nanostructures utilizing a biocompatible DHBC synthesized by Reversible Addition–Fragmentation Chain Transfer (RAFT) polymerization, namely the poly[oligo(ethylene glycol) methacrylate]-b-poly[(vinyl benzyl trimethylammonium chloride)] (POEGMA-b-PVBTMAC), as the base for electrostatic complexation initially with hydrophilic MNPs, and subsequently, incorporating a short DNA. The structure of both MNPs-hybrid complexes and magnetopolyplexes was determined by cryogenic transmission electron microscopy measurements (cryo-TEM)
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