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Growing polyion complex micelles: kinetics and mechanism of electrostatic template polymerization and assembly. | LitMetric
Hypothesis : Electrostatic-templated polymerization (ETP) is a recently developed strategy for robust fabrication of stable polyion complex (PIC) micelles with regulated size and morphology, yet the kinetics and mechanism about this one pot process remain elusive.Experiments : In ETP method, ionic monomers are polymerized in the presence of an oppositely charged ionic-neutral diblock copolymer as template. We investigate the monomer conversion and electrostatic assembly as a function of time, under different polymerization conditions of ionic strength, pH, template/monomer molar ratio and the presence of a cross-linker.Findings : The template copolymer accelerates the monomer conversion and formation of PIC micelles dependent on ionic strength and pH. The process follows the "Pick-up" mechanism, where monomers first convert into oligomers which complex with template to induce further chain growth and electrostatic assembly. Introducing cross-linker hardly impacts the reaction kinetics and "Pick-up" route, while it creates PIC micelles containing cross-linked ionic network assembly with the template. Further removing the template by concentrated salt provides purified ionic nanogels. The disclosed findings not only provide a better understanding of the polymerization-assembly process, but also optimize the controls of electrostatic-templated polymerization for the rational design and fabrication of diverse PIC micelles and polyelectrolyte particles.
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