When two oppositely charged hydrophilic block polyelectrolytes are mixed, they can self-assemble into micelles with polyelectrolyte cores and hydrophilic coronas. These double-hydrophilic aqueous assemblies are responsive to salt, temperature and pH, which makes them attractive carriers for hydrophilic genetic and medicinal material. For delivery applications, particle size is a critical parameter to control, but there are little to no systematic studies on how micelle size can be tuned as a function of neutral/charged block lengths. To precisely determine how distinct polyelectrolyte complex core micelles are influenced by charged and hydrophilic block length, we utilize a combination of controlled radical polymerizations and post-polymerization functionalization chemistry to grow a series of polymers that span a dozen charged and neutral block lengths. To determine the effect of charged block length, we use atom-transfer radical polymerization (ATRP) to grow blocks of the reactive monomer glycidyl methacrylate (GMA) from PEO macroinitiators. Similarly, to determine the effect of neutral block length, radical addition-fragmentation chain transfer (RAFT) is used to grow multiple lengths of dimethyl acrylamide (DMAA) from GMA macroinitiators. Using thiol-epoxy click chemistry, we quantitatively convert the epoxy groups on the glycidyl methacrylate units into analogous polyanions and polycations with the same backbone, linker, dispersity and length. Micelles formed from these pairings are then characterized by TEM, SAXS, SANS and DLS to determine aggregation number, complex core size, and hydrophilic corona thickness. The results from this model system can potentially elucidate universal structure-property relationships which could complement emerging scaling theories in the polyelectrolyte complexation community and enable the predictive design of polyelectrolyte complex micelles.

Effect of charged and hydrophobic block length on polyelectrolyte complex micelles through analogous block polyelectrolytes

Macromolecular Chemistry: The Second Century

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ACS Spring 2020 National Meeting & Expo

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.