Thermoreversible and Injectable ABC Polypeptoid Hydrogels : Controlling the Hydrogel Properties through Molecular Design

A series of ABC triblock copolypeptoids [i.e., poly(N-allyl glycine)-b-poly(N-methyl glycine)-b-poly(N-decyl glycine) (AMD)] with well-defined structure and varying composition have been synthesized by sequential primary amine-initiated ring-opening polymerization of the corresponding N-substituted...

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Veröffentlicht in:Chemistry of materials : a publication of the American Chemical Society. - 1998. - 28(2016), 3 vom: 09. Feb., Seite 727-737
1. Verfasser: Xuan, Sunting (VerfasserIn)
Weitere Verfasser: Lee, Chang-Uk, Chen, Cong, Doyle, Andrew B, Zhang, Yueheng, Guo, Li, John, Vijay T, Hayes, Daniel, Zhang, Donghui
Format: Aufsatz
Sprache:English
Veröffentlicht: 2016
Zugriff auf das übergeordnete Werk:Chemistry of materials : a publication of the American Chemical Society
Schlagworte:Journal Article
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520 |a A series of ABC triblock copolypeptoids [i.e., poly(N-allyl glycine)-b-poly(N-methyl glycine)-b-poly(N-decyl glycine) (AMD)] with well-defined structure and varying composition have been synthesized by sequential primary amine-initiated ring-opening polymerization of the corresponding N-substituted N-carboxyanhydride monomers (Al-NCA, Me-NCA, and De-NCA). The ABC block copolypeptoids undergo sol-to-gel transitions with increasing temperature in water and biological media at low concentrations (2.5-10 wt %). The sol-gel transition is rapid and fully reversible with a narrow transition window, evidenced by the rheological measurements. The gelation temperature (Tgel) and mechanical stiffness of the hydrogels are highly tunable: Tgel in the 26.2-60.0 °C range, the storage modulus (G') and Young's modulus (E) in the 0.2-780 Pa and 0.5-2346 Pa range, respectively, at the physiological temperature (37 °C) can be readily accessed by controlling the block copolypeptoid composition and the polymer solution concentration. The hydrogel is injectable through a 24 gauge syringe needle and maintains their shape upon in contact with surfaces or water baths that are kept above the sol-gel transition temperature. The hydrogels exhibit minimal cytotoxicity toward human adipose derived stem cells (hASCs), evidenced from both alamarBlue and PicoGreen assays. Furthermore, quantitative PCR analysis revealed significant up-regulation of the Col2a1 gene and down-regulation of ANGPT1 gene, suggesting that the hydrogel exhibit biological activity in inducing chondrogenesis of hASCs. It was also demonstrated that the hydrogel can be used to quantitatively encapsulate water-soluble enzymes (e.g., horseradish peroxidase) by manipulating the sol-gel transition. The enzymatic activity of HRP remain unperturbed after encapsulation at 37 °C for up to 7 d, suggesting that the hydrogel does not adversely affect the enzyme structure and thereby the enzymatic activity. These results suggest that the polypeptoid hydrogel a promising synthetic platform for tissue engineering or protein storage applications 
650 4 |a Journal Article 
700 1 |a Lee, Chang-Uk  |e verfasserin  |4 aut 
700 1 |a Chen, Cong  |e verfasserin  |4 aut 
700 1 |a Doyle, Andrew B  |e verfasserin  |4 aut 
700 1 |a Zhang, Yueheng  |e verfasserin  |4 aut 
700 1 |a Guo, Li  |e verfasserin  |4 aut 
700 1 |a John, Vijay T  |e verfasserin  |4 aut 
700 1 |a Hayes, Daniel  |e verfasserin  |4 aut 
700 1 |a Zhang, Donghui  |e verfasserin  |4 aut 
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