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Photopolymerizable nanogels as macromolecular precursors to covalently crosslinked water-based networks.

ABSTRACT: We present a strategy for directly and efficiently polymerizing aqueous dispersions of reactive nanogels into covalently crosslinked polymer networks with properties that are determined by the initial chemical and physical nanogel structure. This technique can extend the range of achievable properties and architectures for networks formed in solution, particularly in water where monomer selection for direct polymerization and the final network properties are quite limited. Nanogels were initially obtained from a solution polymerization of a hydrophilic monomethacrylate and either a hydrophilic PEG-based dimethacrylate or a more hydrophobic urethane dimethacrylate, which produced globular particles with diameters of 10-15 nm with remarkably low polydispersity in some cases. Networks derived from a single type of nanogel or a blend of nanogels with different chemistries when dispersed in water gelled within minutes when exposed to low intensity UV light. Modifying the nanogel structure changes both covalent and non-covalent secondary interactions in the crosslinked networks and reveals critical design criteria for the development of networks from highly internally branched, nanoscale prepolymer precursors.

SUBMITTER: Dailing EA

PROVIDER: S-EPMC4502958 | biostudies-literature | 2015 Jul

REPOSITORIES: biostudies-literature

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Photopolymerizable nanogels as macromolecular precursors to covalently crosslinked water-based networks.

Dailing Eric A EA Setterberg Whitney K WK Shah Parag K PK Stansbury Jeffrey W JW

Soft matter 20150701 28

We present a strategy for directly and efficiently polymerizing aqueous dispersions of reactive nanogels into covalently crosslinked polymer networks with properties that are determined by the initial chemical and physical nanogel structure. This technique can extend the range of achievable properties and architectures for networks formed in solution, particularly in water where monomer selection for direct polymerization and the final network properties are quite limited. Nanogels were initiall ...[more]

PMID: 26075300

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Project description:This paper reports a series of photopolymerizable polysiloxane-modified nanogels for regulating surface microstructure and gradient property of polymers, which were synthesized by solution polymerization under different feed ratios of a methacrylate-modified polysiloxane, urethane dimethacrylate (UDMA) and isobornyl methacrylate (IBMA) in the presence of a thiol chain transfer agent. The nanogel structure and composition were characterized by proton nuclear magnetic resonance (1H-NMR), Fourier transform-infrared spectroscopy (FT-IR), transmission electron microscope (TEM), gel permeation chromatography (GPC) and differential scanning calorimetry (DSC). The dispersion of these nanogels in triethylene glycol dimethacrylate (TEGDMA) can reduce the onset and magnitude of shrinkage stress during polymerization without compromise to mechanical properties of the resulting polymers. Most importantly, as demonstrated by elemental analysis and X-ray photoelectron spectroscopy (XPS), the nanogels exhibit good self-floating ability in the monomer/polymer matrix and the increase of polysiloxane content in the nanogel can enhance the self-floating capability due to the lower surface tension and energy associated with the polysiloxane component. As a result, the polysiloxane-modified nanogels can spontaneously form a concentration gradient that can be locked in upon photopolymerization leading to a well-controlled heterogeneous polymer that presents a gradient change in thermal stability. With the increase of polysiloxane content, the thermal stability of the polymer was improved significantly. Furthermore, the enrichment of the nanogel on the surface resulting from the good self-floating ability can reduce the dispersion surface energy of gradient polymer film and generate a more hydrophobic surface with altered surface microstructure. These photopolymerizable polysiloxane-modified nanogels are demonstrated to have potential broad application in the preparation of gradient polymer with controlled surface properties.

Dataset Information

Photopolymerizable nanogels as macromolecular precursors to covalently crosslinked water-based networks.

Publications

Photopolymerizable nanogels as macromolecular precursors to covalently crosslinked water-based networks.

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