Self-assembly of amphiphilic polymers is a promising strategy to design advanced nanomaterials.1 Among those copolymers, polypeptides are an emerging class of biomaterials.2 So far, the most economical and efficient process to prepare polypeptides is a one-step process based on the ring-opening polymerization of N-carboxyanhydride monomers (ROP, Scheme 1A).3 This controlled polymerization uses simple reagents and allows the preparation of polymers in both good yields and large quantities. However, NCA polymerizations suffer from significant limitations including tedious monomer purification steps,4 significant sensitivity to moisture,5 and processing in toxic organics solvents such as DMF that need to be subsequently removed.6 More importantly, the preparation of nanoassemblies from amphiphilic polypeptides requires a second step of nanoprecipitation (Scheme 1A), which entails the addition of a non-solvent for the hydrophobic segment to a copolymer solution in a common solvent for both blocks.7 This nanoprecipitation step is typically performed from toxic organic solvents, under relatively diluted conditions (&lt;1 wt%) and is sensitive to scale issues, overall hampering eventual regulatory approval.8 Specifically, we report aqueous ring-opening polymerization (ROP) of N-carboxyanhydrides (NCA) using a-amino-poly(ethylene oxide) macroinitiator to protect NCA monomers from hydrolysis through spontaneous in situ self-assembly (ISA). This ROPISA process (Scheme 1B) affords well-defined amphiphilic diblock copolymers that simultaneously form original anisotropic nano-objects.

Aqueous ring-opening polymerization-induced self-assembly (ROPISA) of N-carboxyanhydrides

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.