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Tunable Coacervation of Well-Defined Homologous Polyanions and Polycations by Local Polarity.

ABSTRACT: The ionic complexation of polyelectrolytes is an important mechanism underlying many important biological processes and technical applications. The main driving force for complexation is electrostatic, which is known to be affected by the local polarity near charge centers, but the impact of which on the complexation of polyelectrolytes remains poorly explored. We developed a homologous series of well-defined polyelectrolytes with identical backbone structures, controlled molecular weights, and tunable local polarity to modulate the solvation environment near charged groups. A multitude of systematic, accurate phase diagrams were obtained by spectroscopic measurements of polymer concentrations via fluorescent labeling of polycations. These phase diagrams unambiguously revealed that the liquidlike coacervation is more stable against salt addition at reduced local polarity over a wide range of molecular weights. These trends were quantitatively captured by a theory of complexation that incorporates the effects of dispersion interactions, charge connectivity, and reversible ion-binding, providing the microscopic design rules for tuning molecular parameters and local polarity.

SUBMITTER: Lou J

PROVIDER: S-EPMC6439447 | biostudies-literature | 2019 Mar

REPOSITORIES: biostudies-literature

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Tunable Coacervation of Well-Defined Homologous Polyanions and Polycations by Local Polarity.

Lou Junzhe J Friedowitz Sean S Qin Jian J Xia Yan Y

ACS central science 20190206 3

The ionic complexation of polyelectrolytes is an important mechanism underlying many important biological processes and technical applications. The main driving force for complexation is electrostatic, which is known to be affected by the local polarity near charge centers, but the impact of which on the complexation of polyelectrolytes remains poorly explored. We developed a homologous series of well-defined polyelectrolytes with identical backbone structures, controlled molecular weights, and ...[more]

PMID: 30937382

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Project description:Design, synthesis, and application of cyclodextrin (CD) containing thermoresponsive hydrogels fabricated from thiol-reactive telechelic polymers are reported. Hydrophilic polymers containing 2-hydroxyethyl methacrylate and/or di(ethylene glycol)methylether methacrylate monomers as side chains and thiol-reactive groups at chain ends were synthesized. A series of hydrogels was fabricated using thiol-ene conjugation of these thiol-reactive polymers with multivalent thiol-containing CDs as crosslinkers. Clear and transparent hydrogels were obtained with good conversion (79-89%) by utilizing the "nucleophilic" and "radical" thiol-ene "click" reactions. Analysis of the amount of residual thiol groups in these hydrogels using Ellman's reagent suggested that gels with a moderately well-defined network structure were obtained. Hydrogels fabricated using different telechelic polymers were examined for their properties such as morphology, equilibrium water uptake, and rheological characteristics. Cytocompatibility of these hydrogels was ascertained by a cell viability assay that demonstrated low toxicity toward fibroblast cells. Thereafter, the CD-containing hydrogels were evaluated for the loading and controlled release of puerarin, an antiglaucoma drug. Utilization of thermoresponsive polymers as the matrix for these hydrogels allows use of temperature as a stimulus to modulate the drug release. A slower and more sustained drug release was observed at physiological temperatures compared to ambient conditions. The effect of temperature on the elasticity of the hydrogel was investigated rheologically to demonstrate that the collapse of the network structure occurs near physiological temperatures. The increased hydrophobicity and compactness of the gel matrix at higher temperatures results in a slower drug release. The strategy employed here demonstrates that tuning the matrix composition of hydrogels with well-defined network structures through appropriate choice of responsive copolymers allows design of materials with control of their physical properties and drug-release behavior.

Dataset Information

Tunable Coacervation of Well-Defined Homologous Polyanions and Polycations by Local Polarity.

Publications

Tunable Coacervation of Well-Defined Homologous Polyanions and Polycations by Local Polarity.

Similar Datasets

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