Unimolecular Micelles from Randomly Grafted Arborescent Copolymers with Different Core Branching Densities: Encapsulation of Doxorubicin and In Vitro Release Study.

Materials (Basel)

Department of Chemistry, Institute for Polymer Research, University of Waterloo, 200 University Ave. W., Waterloo, ON N2L 3G1, Canada.

Published: March 2023

A series of amphiphilic arborescent copolymers of generations G1 and G2 with an arborescent poly(γ-benzyl L-glutamate) (PBG) core and poly(ethylene oxide) (PEO) chain segments in the shell, PBG--PEO, were synthesized and evaluated as drug delivery nanocarriers. The PBG building blocks were generated by ring-opening polymerization of γ-benzyl L-glutamic acid carboxyanhydride (Glu-NCA) initiated with -hexylamine. Partial or full deprotection of the benzyl ester groups followed by coupling with PBG chains yielded a comb-branched (arborescent polymer generation zero or G0) PBG structure. Additional cycles of deprotection and grafting provided G1 and G2 arborescent polypeptides. Side chains of poly(ethylene oxide) were then randomly grafted onto the arborescent PBG substrates to produce amphiphilic arborescent copolymers. Control over the branching density of G0PBG was investigated by varying the length and the deprotection level of the linear PBG substrates used in their synthesis. Three G0PBG cores with different branching densities, varying from a compact and dense to a loose and more porous structure, were thus synthesized. These amphiphilic copolymers behaved similar to unimolecular micelles in aqueous solutions, with a unimodal number- and volume-weighted size distributions in dynamic light scattering measurements. It was demonstrated that these biocompatible copolymers can encapsulate hydrophobic drugs such as doxorubicin (DOX) within their hydrophobic core with drug loading efficiencies of 42-65%. Sustained and pH-responsive DOX release was observed from the unimolecular micelles, which suggests that they could be useful as drug nanocarriers for cancer therapy.

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http://www.ncbi.nlm.nih.gov/pmc/articles/PMC10053569PMC
http://dx.doi.org/10.3390/ma16062461DOI Listing

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