One-Pot Synthesis of Oxidation-Sensitive Supramolecular Gels and Vesicles
Metadatos
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American Chemical Society
Date
2021-11-11Referencia bibliográfica
Biomacromolecules 2021, 22, 5052−5064. [https://doi.org/10.1021/acs.biomac.1c01039]
Patrocinador
Royal Society of London European Commission 2017-NF171487; EU H2020 MSCA-IF-792957 European Research Council (ERC) European Commission CheSSTaG 769798; UK Research & Innovation (UKRI); Engineering & Physical Sciences Research Council (EPSRC) EP/N026322/1; Jeol and DENS Solutions; UK's ESPRC EP/N026322/1; Spanish State Research Agency (Spanish Ministry of Science and Innovation) IJC2018-037951-IRésumé
Polypeptide-based nanoparticles offer unique advantages from a nanomedicine perspective such as biocompatibility,
biodegradability, and stimuli-responsive properties to (patho)physiological conditions. Conventionally, self-assembled polypeptide
nanostructures are prepared by first synthesizing their constituent amphiphilic polypeptides followed by postpolymerization selfassembly.
Herein, we describe the one-pot synthesis of oxidation-sensitive supramolecular micelles and vesicles. This was achieved
by polymerization-induced self-assembly (PISA) of the N-carboxyanhydride (NCA) precursor of methionine using poly(ethylene
oxide) as a stabilizing and hydrophilic block in dimethyl sulfoxide (DMSO). By adjusting the hydrophobic block length and
concentration, we obtained a range of morphologies from spherical to wormlike micelles, to vesicles. Remarkably, the secondary
structure of polypeptides greatly influenced the final morphology of the assemblies. Surprisingly, wormlike micellar morphologies
were obtained for a wide range of methionine block lengths and solid contents, with spherical micelles restricted to very short
hydrophobic lengths. Wormlike micelles further assembled into oxidation-sensitive, self-standing gels in the reaction pot. Both
vesicles and wormlike micelles obtained using this method demonstrated to degrade under controlled oxidant conditions, which
would expand their biomedical applications such as in sustained drug release or as cellular scaffolds in tissue engineering.