| Abstract: | Stimuli‐responsive polypeptides are receiving much attention for drug delivery systems and tissue engineering scaffolds; however, it is challenging to construct multiple‐responsive polypeptides and one‐component polymeric hydrogels. Herein, a novel type of triple redox/temperature‐responsive diselenide‐containing poly(methoxydiethylene glycol‐l ‐glutamate) homopolypeptide was facilely synthesized by selenocystamine‐initiated ring‐opening polymerization in DMF at 30 °C, and their chemical structures and physical properties were fully characterized by means of 1H NMR, GPC, FT‐IR, WAXD, and CD. They self‐assembled into spherical micelles in aqueous solution, which possess a lower critical solution temperature, redox‐responsiveness inherited from diselenide bond, and the triple stimuli‐sensitive self‐assembly behaviors, as characterized by means of turbidity, DLS, TEM, and zeta potential measurements. The diselenide‐containing homopolypeptides formed supramolecular hydrogels at room temperature, exhibiting a thermal gel–sol transition. The rheological tests evidence that the mechanical modulus of the hydrogel is independent of angular frequency within 100 rad/s and at 25 °C, in which the storage modulus of G′ is order of magnitude greater than the loss modulus of G″, displaying a solid‐like elastic behavior. Moreover, the mechanical modulus of the hydrogel can be tuned by changing the chain length of the homopolypeptide, the 10‐mM 1,4‐dithiothreitol (DTT) reduction, and 1 mM H2O2 oxidation, respectively. Consequently, this work provides a simple strategy to fabricate triple‐stimuli responsive polypeptide micelles and one‐component hydrogels. © 2018 Wiley Periodicals, Inc. J. Polym. Sci., Part A: Polym. Chem. 2018 , 56, 1067–1077 |
