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Synthesis and self-assembly of temperature-responsive copolymers based on N-vinylpyrrolidone and triethylene glycol methacrylate.

ABSTRACT: Polyvinylpyrrolidone (PVP) is a biocompatible, water-soluble polymer with unique physicochemical properties and attractive biological features that has found widespread use in several industries. Owing to advances in controlled polymerisation techniques, PVP can be easily synthesised with robust control over its architecture. However, the synthesis of PVP copolymers, which can allow tailoring of its properties and expand the scope of this polymeric material, is challenging and rarely reported. Here, we demonstrate the synthesis of well-defined, temperature-responsive polyvinylpyrrolidone-co-poly(triethylene glycol methacrylate) (PVP-co-pTEGMA) block copolymers via successive Reversible Addition-Fragmentation chain Transfer (RAFT) and Activators ReGenerated by Electron Transfer Atom Transfer Radical Polymerisation (ARGET-ATRP) techniques. We show that PVP-co-pTEGMA block copolymers display temperature-responsive behaviour and self-assemble above their cloud point temperature (Tcp) to form spherical nanostructures of 100-200 nm in diameter. Finally, we demonstrate stabilisation of these assemblies below their Tcp by cross-linking through the PVP block.

SUBMITTER: Jumeaux C

PROVIDER: S-EPMC5408929 | biostudies-literature | 2015 May

REPOSITORIES: biostudies-literature

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Synthesis and self-assembly of temperature-responsive copolymers based on <i>N</i>-vinylpyrrolidone and triethylene glycol methacrylate.

Jumeaux Coline C Chapman Robert R Chandrawati Rona R Stevens Molly M MM

Polymer chemistry 20150501 22

Polyvinylpyrrolidone (PVP) is a biocompatible, water-soluble polymer with unique physicochemical properties and attractive biological features that has found widespread use in several industries. Owing to advances in controlled polymerisation techniques, PVP can be easily synthesised with robust control over its architecture. However, the synthesis of PVP copolymers, which can allow tailoring of its properties and expand the scope of this polymeric material, is challenging and rarely reported. H ...[more]

PMID: 28458725

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Project description:This paper introduces a new class of amphiphilic block copolymers created by combining two polymers: polylactic acid (PLA), a biocompatible and biodegradable hydrophobic polyester used for cargo encapsulation, and a hydrophilic polymer composed of oligo ethylene glycol chains (triethylene glycol methyl ether methacrylate, TEGMA), which provides stability and repellent properties with added thermo-responsiveness. The PLA-b-PTEGMA block copolymers were synthesized using ring-opening polymerization (ROP) and reversible addition-fragmentation chain transfer (RAFT) polymerization (ROP-RAFT), resulting in varying ratios between the hydrophobic and hydrophilic blocks. Standard techniques, such as size exclusion chromatography (SEC) and 1H NMR spectroscopy, were used to characterize the block copolymers, while 1H NMR spectroscopy, 2D nuclear Overhauser effect spectroscopy (NOESY), and dynamic light scattering (DLS) were used to analyze the effect of the hydrophobic PLA block on the LCST of the PTEGMA block in aqueous solutions. The results show that the LCST values for the block copolymers decreased with increasing PLA content in the copolymer. The selected block copolymer presented LCST transitions at physiologically relevant temperatures, making it suitable for manufacturing nanoparticles (NPs) and drug encapsulation-release of the chemotherapeutic paclitaxel (PTX) via temperature-triggered drug release mechanism. The drug release profile was found to be temperature-dependent, with PTX release being sustained at all tested conditions, but substantially accelerated at 37 and 40 °C compared to 25 °C. The NPs were stable under simulated physiological conditions. These findings demonstrate that the addition of hydrophobic monomers, such as PLA, can tune the LCST temperatures of thermo-responsive polymers, and that PLA-b-PTEGMA copolymers have great potential for use in drug and gene delivery systems via temperature-triggered drug release mechanisms in biomedicine applications.

Dataset Information

Synthesis and self-assembly of temperature-responsive copolymers based on N-vinylpyrrolidone and triethylene glycol methacrylate.

Publications

Synthesis and self-assembly of temperature-responsive copolymers based on <i>N</i>-vinylpyrrolidone and triethylene glycol methacrylate.

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