Preparation and Characterization of Attractive Poly(amino acid) Hydrogels Based on 2-Ureido-4[1 H ]-Pyrimidinone
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ARTICLE
POLYMER SCIENCE
https://doi.org/10.1007/s10118-021-2498-y Chinese J. Polym. Sci.
Preparation and Characterization of Attractive Poly(amino acid) Hydrogels Based on 2-Ureido-4[1H]-Pyrimidinone Zhen Shi†, Qi Wang†, Gui-Fei Li*, Yu-Feng Shou, Hong-Jie Zong, Shi-Feng Yan, Kun-Xi Zhang, and Jing-Bo Yin* Department of Polymer Materials, School of Materials Science and Engineering, Shanghai University, Shanghai 200444, China
Electronic Supplementary Information Abstract Self-healing hydrogels with the shear-thinning property are novel injectable materials and are superior to traditional injectable hydrogels. The self-healing hydrogels based on 2-ureido-4[1H]-pyrimidinone (UPy) have recently received extensive attention due to their dynamic reversibility of UPy dimerization. However, generally, UPy-based self-healing hydrogels exhibit poor stability, cannot degrade in vivo and can hardly be excreted from the body, which considerably limit their bio-application. Here, using poly(l-glutamic acid) (PLGA) as biodegradable matrix, branching α-hydroxy-ω-amino poly(ethylene oxide) (HAPEO) as bridging molecule to introduce UPy, and ethyl acrylate polyethylene glycol (MAPEG) to introduce double bond, the hydrogel precursors (PMHU) are prepared. A library of the self-healing hydrogels has been achieved with well self-healable and shear-thinning properties. With the increase of MAPEG grafting ratio, the storage modulus of the self-healing hydrogels decreases. The self-healing hydrogels are stable in solution only for 6 h, hard to meet the requirements of tissue regeneration. Consequently, ultraviolet (UV) photo-crosslinking is involved to obtain the dual crosslinking hydrogels with enhanced mechanical properties and stability. When MAPEG grafting ratio is 35.5%, the dual crosslinking hydrogels can maintain the shape in phosphate-buffered saline solution (PBS) for at least 8 days. Loading with adipose-derived stem cell spheroids, the self-healing hydrogels are injected and self-heal to a whole, and then they are crosslinked in situ via UV-irradiation, obtaining the dual crosslinking hydrogels/cell spheroids complex with cell viability of 86.7%±6.0%, which demonstrates excellent injectability, subcutaneous gelatinization, and biocompatibility of hydrogels as cell carriers. The novel PMHU hydrogels crosslinked by quadruple hydrogen bonding and then dual photo-crosslinking of double bond are expected to be applied for minimal invasive surgery or therapies in tissue engineering. Keywords 2-Ureido-4[1H]-pyrimidinone (UPy); Poly(l-glutamic acid) (PLGA); Self-healable; Photo-crosslinking Citation: Shi, Z.; Wang, Q.; Li, G. F.; Shou, Y. F.; Zong, H. J.; Yan, S. F.; Zhang, K. X.; Yin, J. B. Preparation and characterization of attractive poly(amino acid) hydrogels based on 2-ureido-4[1H]-pyrimidinone. Chinese J. Polym. Sci. https://doi.org/10.1007/s10118-021-2498-y
INTRODUCTION Self-healing hydrogels with the shear-thinning property are promising injectable materials, showing great advantages in minimally invasive trea
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