Polyelectrolyte complex coacervation is an important process in nature and, in combination with synthetic variations in macromolecular architecture, provides new tools and versatility in the rational design of functional materials. Synthetic polyelectrolyte complexes (PECs) studied thus far have predominantly dealt with fully or strongly charged polyelectrolytes, i.e., those where all or a majority of monomer units are ionized, respectively. Meanwhile, theoretical studies suggest that linear charge density—or the fraction of ionic monomers <i>f</i>—can be used to tune the binodals of the associative phase separation as well as the internal structure and density of the PEC phase. A quantitative understanding of how PEC structure and properties change over a broad range of charge densities remains however experimentally unexplored. We have aimed to fill this gap and, in this talk, will share binodals and scattering profiles of PECs assembled from hydrophilic, near ideally random (co)polyelectrolytes with <i>f </i>= 0.30−1.0. Our experimental findings are contrasted with predictions from available scaling theory and molecular dynamics simulations to rationalize salient features.

Polyelectrolyte complex coacervation across a broad range of charge densities

ACS Spring 2022

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