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. 2023 Dec 18;16(24):7702.
doi: 10.3390/ma16247702.

Anionic Hyperbranched Amphiphilic Polyelectrolytes as Nanocarriers for Antimicrobial Proteins and Peptides

Anastasia Balafouti  1   2 , Aleksander Forys  3 , Barbara Trzebicka  3 , Angelica Maria Gerardos  1   2 , Stergios Pispas  1
Affiliations

Anionic Hyperbranched Amphiphilic Polyelectrolytes as Nanocarriers for Antimicrobial Proteins and Peptides

Anastasia Balafouti et al. Materials (Basel). .

Abstract

This manuscript presents the synthesis of hyperbranched amphiphilic poly (lauryl methacrylate-co-tert-butyl methacrylate-co-methacrylic acid), H-P(LMA-co-tBMA-co-MAA) copolymers via reversible addition fragmentation chain transfer (RAFT) copolymerization of tBMA and LMA, and their post-polymerization modification to anionic amphiphilic polyelectrolytes. The focus is on investigating whether the combination of the hydrophobic characters of LMA and tBMA segments, as well as the polyelectrolyte and hydrophilic properties of MAA segments, both distributed within a unique hyperbranched polymer chain topology, would result in intriguing, branched copolymers with the potential to be applied in nanomedicine. Therefore, we studied the self-assembly behavior of these copolymers in aqueous media, as well as their ability to form complexes with cationic proteins, namely lysozyme (LYZ) and polymyxin (PMX). Various physicochemical characterization techniques, including size exclusion chromatography (SEC) and proton nuclear magnetic resonance (1H-NMR), verified the molecular characteristics of these well-defined copolymers, whereas light scattering and fluorescence spectroscopy techniques revealed promising nanoparticle (NP) self- and co-assembly properties of the copolymers in aqueous media.

Keywords: amphiphilic copolymers; hyperbranched; nanoparticles; polyelectrolytes; protein complexation; self-assembly.

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Conflict of interest statement

The authors declare no conflict of interest.

Figures

Scheme 1
Scheme 1
Synthesis of the HHC via RAFT polymerization and post-modification hydrolysis.
Figure 1
Figure 1
SEC traces of the precursor HCs.
Figure 2
Figure 2
1H-NMR spectra of the precursor HCs (Hydrogen peak assignments are represented by the letters).
Figure 3
Figure 3
1H-NMR spectra in CDCl3 and d8-THF (a) and FT-IR ATR spectra (b) of HC 2 before and after 24 h hydrolysis (The letters in 1H-NMR spectra represent hydrogen peak assignments and the star (*) symbols are attributed to CDCL3 and d8-THF).
Figure 4
Figure 4
Size distributions from DLS analysis performed in THF at c = 10−2 g/mL for the different HC polymers.
Figure 5
Figure 5
CAC determination for HHC 1 (a) and HHC 3 (b) copolymers.
Figure 6
Figure 6
Comparison of size distributions from DLS analysis of the (a) HCs after 24 h hydrolysis in aqueous media and (b) the HHCs in aqueous media. (c = 5 × 10−4 g/mL).
Figure 7
Figure 7
Cryo-TEM images from HHC 1 copolymer solutions showing NPs of (a) Rh ≤ 47 nm, (b) Rh ≤ 108 nm and (c) Rh ≤ 30 nm.
Figure 8
Figure 8
Cryo-TEM images from HHC 3 copolymer solutions showing NPs of (a) Rh = 23 nm and (b) Rh ≤ 56 nm.
Figure 9
Figure 9
Comparison of size distributions from DLS analysis of the HHC–LYZ complexes obtained from (a) HHC 2 and (b) HHC 3 copolymers.
Figure 10
Figure 10
Cryo-TEM images from HHC 3:LYZ = 1:1.5 complexes showing NPs of (a) Rh ≤ 138 nm and (b) Rh ≤ 68 nm.
Figure 11
Figure 11
Cryo-TEM images from HHC 3:LYZ = 1:1 complexes showing NPs of (a) Rh ≤ 135 nm, (b) Rh = 177 nm and (c) Rh ≤ 104 nm.
Figure 12
Figure 12
Fluorescence spectra of HHC–LYZ complexes for (a) HHC 2 and (b) HHC 3 copolymers.
Figure 13
Figure 13
Photograph of solutions of HHC1:PMX complexes with a charge ratio of 1:2 to 8:1 (left to right).
Figure 14
Figure 14
Comparison of size distributions from DLS analysis of the HHC–PMX complexes obtained from (a) HHC 1 and (b) HHC 3 copolymers.
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