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H. Wu et al Mechanism of Dissociation Kinetics in Polyelectrolyte Complex Micelles.pdf (2.76 MB)
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Mechanism of Dissociation Kinetics in Polyelectrolyte Complex Micelles

preprint
submitted on 27.08.2019 and posted on 28.08.2019 by Hao Wu, Jeffrey Ting, Matthew Tirrell

Polyelectrolyte-based nanoscale self-assemblies, such as micelles, possess diverse desirable attributes such as capability for sequestering and protecting biomacromolecules against inhospitable environments, responsiveness to external stimuli, and tunability of physical behavior. However, little is known on the mechanisms of dissociation when micelles encounter and respond to environmental changes. Using salt-jump, time-dependent, light scattering, the pathway of dissociation is observed in polyelectrolyte complex micelles that have complex cores and neutral coronas. The micelle dissociation kinetics appear to be a three-staged process, in good agreement with the scattering data. Using kinetic models of amphiphilic block copolymer micelles in polyelectrolyte complexation-driven micelles, we derive an analytical expression for dissociation relaxation rates as a function of solvent temperature, salt concentration, and the length of the charged polymer blocks. The theoretical predictions are compatible with the experimental data from light scattering experiments. This study demonstrates experimentally the relaxation kinetics of polyelectrolyte complex micelle dissociation and illustrates the underlying mechanism governing the dissociation kinetics. It is anticipated that these findings can be generalized to other electrostatic interaction-driven self-assemblies to better understand the relationship among the kinetics of dissociation, constituent polymer properties, and environmental parameters.

Funding

NIST-CHiMaD

History

Email Address of Submitting Author

wuhao@uchicago.edu

Institution

University of Chicago

Country

United States

ORCID For Submitting Author

0000-0001-6276-6114

Declaration of Conflict of Interest

The authors declare no conflict of interest.

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