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Antifreeze and Rheological Properties of Injectable Triblock Copolymer Hydrogels with Supramolecular Junctions

Authors
Choi, JewonKim, SeyoungMun, Huy JuYoo, JinChoi, Soo-HyungChar, Kookheon
Issue Date
1-Jun-2022
Publisher
John Wiley & Sons Ltd.
Keywords
antifreeze hydrogels; injectability; self-healing; supramolecular interactions; triblock copolymer
Citation
Macromolecular Rapid Communications, v.43, no.12
Journal Title
Macromolecular Rapid Communications
Volume
43
Number
12
URI
https://scholarworks.bwise.kr/hongik/handle/2020.sw.hongik/21058
DOI
10.1002/marc.202100618
ISSN
1022-1336
Abstract
ABC triblock copolymers composed of hydrophobic poly(epsilon-caprolactone) (PCL), zwitterionic poly(carboxybetaine methacrylate) midblock, and P(PEGMA-UPy0.15) containing supramolecular ureidopyrimidinone moieties, poly(epsilon-caprolactone-block-carboxybetaine methacrylate-block-[poly(ethylene glycol) methyl ether methacrylate-co-(alpha-methacryloyl-omega-(6-(3-(6-methyl-4-oxo-1,4-dihydropyrimidin-2-yl)ureido)hexylcarbamoyloxy)poly(ethylene glycol))]), are investigated to achieve multifunctional antifreeze hydrogels. The PCL and P(PEGMA-UPy0.15) blocks induce the formation of physical network with a hierarchical nanostructure comprising hydrophobic PCL cores and supramolecular junctions, respectively. The super-hydrophilic nature of polyzwitterion midblocks and the confinement effect of the supramolecular junctions enhance the antifreeze performance, where the majority of water molecules remains supercooled below sub-zero temperature. The hydrogel relaxation characterized over a wide range of timescale reveals that the facile dynamics of the supramolecular junctions lead to the self-healing and injectability of the hydrogels. In conjunction with the biodegradable PCL cores, the antifreeze and rheological characteristics of the triblock copolymer hydrogels provide significant potential to use for cryo-preservable and bio-injectable drug storage and delivery.
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