期刊
MACROMOLECULAR CHEMISTRY AND PHYSICS
卷 221, 期 3, 页码 -出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/macp.201900421
关键词
alpha-helix; biocompatibility; biodegradation; lower critical solution temperature; stimuli-responsive polymers
资金
- National Natural Science Foundation of China [51873213]
- Open Project Foundation of Beijing National Laboratory for Molecular Sciences [BNLMS201840]
Biocompatible and biodegradable thermoresponsive polymers are of great interest in smart biomedical applications. Herein, triblock copolymers (6a and 6b) comprised of hydrophobic poly(propylene glycol) (PPG) and OEGylated polypeptides bearing Y-shaped or linear pendants are prepared by ring-opening polymerization of reactive N-carboxyanhydride monomers and subsequent side chain modification of polypeptides. OEGylated triblock copolymer bearing Y-shaped (6a) or linear pendants (6b) with similar main chain length and the same amount of oligo(ethylene glycol) (OEG) units are successfully prepared as verified by H-1 NMR, FTIR, and GPC. CD analysis reveals that 6a with Y-shaped OEG pendants shows thermal- or salt-induced destabilization of alpha-helical conformation in water. Both 6a and 6b show reversible lower critical solution temperature (LCST)-type phase transitions in DI H2O or PBS. Incorporation of a PPG segment leads to a significant decrease of the LCST-type cloud point temperature (T-cp). Consequently, 6a and 6b show T-cp to human body temperature at low polymer concentrations (<= 0.5 mg mL(-1) in PBS). Moreover, 6a and 6b show low in vitro cytotoxicity and biodegradability in the presence of proteinase K. The results indicate that the thermoresponsive properties of LCST-type polymers can be readily tuned by constructing Y-shaped pendants as well as incorporation of hydrophobic polymer building blocks.
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