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Electrochemical-Mediated Gelation Of Catechol-Bearing Hydrogels Based On Multimodal Crosslinking.

ABSTRACT: Catechol-bearing polymers form hydrogel networks through cooperative oxidative crosslinking and coordination chemistry. Here we describe the kinetics of cation-dependent electrochemical-mediated gelation of precursor solutions composed of catechol functionalized four-arm poly(ethylene glycol) combined with select metal cations. The gelation kinetics, mechanical properties, crosslink composition, and self-healing capacity is a strong function of the valency and redox potential of metal ions in the precursor solution. Catechol-bearing hydrogels exhibit highly compliant mechanical properties with storage moduli ranging from G' = 0.1-5 kPa depending on the choice of redox active metal ions in the precursor solution. The gelation kinetics is informed by the net cell potential of redox active components in the precursor solution. Finally, redox potential of the metal ion precursor can differentially alter the effective density of crosslinks in networks and confer properties to hydrogels such as self-healing capacity. Taken together, this parametric study generates new insight to inform the design of catechol-bearing hydrogel networks formed by electrochemical-mediated multimodal crosslinking.

SUBMITTER: Mou C

PROVIDER: S-EPMC6675465 | biostudies-literature | 2019 Mar

REPOSITORIES: biostudies-literature

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Electrochemical-Mediated Gelation Of Catechol-Bearing Hydrogels Based On Multimodal Crosslinking.

Mou Chenchen C Ali Faisal F Malaviya Avishi A Bettinger Christopher J CJ

Journal of materials chemistry. B 20181213 10

Catechol-bearing polymers form hydrogel networks through cooperative oxidative crosslinking and coordination chemistry. Here we describe the kinetics of cation-dependent electrochemical-mediated gelation of precursor solutions composed of catechol functionalized four-arm poly(ethylene glycol) combined with select metal cations. The gelation kinetics, mechanical properties, crosslink composition, and self-healing capacity is a strong function of the valency and redox potential of metal ions in th ...[more]

PMID: 31372223

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Project description:Embedding nanomaterials into polymer hydrogels enables the design of functional materials with tailored chemical, mechanical, and optical properties. Nanocapsules that protect interior cargo and disperse readily through a polymeric matrix have drawn particular interest for their ability to integrate chemically incompatible systems and to further expand the parameter space for polymer nanocomposite hydrogels. The properties of polymer nanocomposite hydrogels depend on the material composition and processing route, which were explored systematically in this work. The gelation kinetics of network-forming polymer solutions with and without silica-coated nanocapsules bearing polyethylene glycol (PEG) surface ligands were investigated using in situ dynamic rheology measurements. Network-forming polymers comprised either 4-arm or 8-arm star PEG with terminal anthracene groups, which dimerize upon irradiation with ultraviolet (UV) light. The PEG-anthracene solutions exhibited rapid gel formation upon UV exposure (365 nm); gel formation was observed as a crossover from liquid-like to solid-like behavior during in situ small-amplitude oscillatory shear rheology. This crossover time was non-monotonic with polymer concentration. Far below the overlap concentration (c/c* ≪ 1), spatially separated PEG-anthracene molecules were subject to forming intramolecular loops over intermolecular cross-links, thereby slowing the gelation process. Near the polymer overlap concentration (c/c* ∼ 1), rapid gelation was attributed to the ideal proximity of anthracene end groups from neighboring polymer molecules. Above the overlap concentration (c/c* > 1), increased solution viscosities hindered molecular diffusion, thereby reducing the frequency of dimerization reactions. Adding nanocapsules to PEG-anthracene solutions resulted in faster gelation than nanocapsule-free PEG-anthracene solutions with equivalent effective polymer concentrations. The final elastic modulus of nanocomposite hydrogels increased with nanocapsule volume fraction, signifying synergistic mechanical reinforcement by nanocapsules despite not being cross-linked into the polymer network. Overall, these findings quantify the impact of nanocapsule addition on the gelation kinetics and mechanical properties of polymer nanocomposite hydrogels, which are promising materials for applications in optoelectronics, biotechnology, and additive manufacturing.

Dataset Information

Electrochemical-Mediated Gelation Of Catechol-Bearing Hydrogels Based On Multimodal Crosslinking.

Publications

Electrochemical-Mediated Gelation Of Catechol-Bearing Hydrogels Based On Multimodal Crosslinking.

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