Issue 11, 2023

Preparation of polymer nanoparticle-based complex coacervate hydrogels using polymerisation-induced self-assembly derived nanogels

Abstract

This paper reports a generic method to prepare polymer nanoparticle-based complex coacervate (PNCC) hydrogels by employing rationally designed nanogels synthesised by reversible addition-fragmentation chain-transfer (RAFT)-mediated polymerisation-induced self-assembly (PISA). Specifically, a poly(potassium 3-sulfopropyl methacrylate) (PKSPMA) macromolecular chain-transfer agent (macro-CTA) was synthesised via RAFT solution polymerisation followed by chain-extension with a statistical copolymer of benzyl methacrylate (BzMA) and methacrylic acid (MAA) at pH 2. Thus, pH-responsive nanoparticles (NPs) comprising a hydrophobic polyacid core-forming block and a sulfonate-functional stabiliser block were formed. With the introduction of methacrylic acid into the core of the NPs, they become swollen with increasing pH, as judged by dynamic light scattering (DLS), indicating nanogel-type behaviour. PNCC hydrogels were prepared by simply mixing the PISA-derived nanogels and cationic branched polyethyleneimine (bPEI) at 20% w/w. In the absence of MAA in the core of the NPs, gel formation was not observed. The mass ratio between the nanogels and bPEI affected resulting hydrogel strength and a mixture of bPEI and PKSPMA68-P(BzMA0.6-stat-MAA0.4)300 NPs with a mass ratio of 0.14 at pH ∼7 resulted in a hydrogel with a storage modulus of approximately 2000 Pa, as determined by oscillatory rheology. This PNCC hydrogel was shear-thinning and injectable, with recovery of gel strength occurring rapidly after the removal of shear.

Graphical abstract: Preparation of polymer nanoparticle-based complex coacervate hydrogels using polymerisation-induced self-assembly derived nanogels

Supplementary files

Article information

Article type
Paper
Submitted
23 11月 2022
Accepted
22 2月 2023
First published
23 2月 2023
This article is Open Access
Creative Commons BY license

Soft Matter, 2023,19, 2074-2081

Preparation of polymer nanoparticle-based complex coacervate hydrogels using polymerisation-induced self-assembly derived nanogels

R. Du and L. A. Fielding, Soft Matter, 2023, 19, 2074 DOI: 10.1039/D2SM01534J

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