Self-Healing Hydrogel with a Double Dynamic Network Comprising Imine and Borate Ester Linkages

Self-Healing Hydrogel with a Double Dynamic Network Comprising Imine and Borate Ester Linkages
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具有包含亚胺和硼酸酯键的双动态网络的自修复水凝胶

DOI:
10.1021/acs.chemmater.9b01301
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发表时间:
2019-08-13
影响因子:
8.6
通讯作者:
Tao, Lei
Tao, Lei
中科院分区:
材料科学2区
文献类型:
--
作者:
Li, Yongsan;Yang, Lei;Tao, Lei

文献摘要

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一种具有双动态网络(DDN)性质的自修复水凝胶,该双动态网络(DDN)是通过使用单一的聚合物交联剂通过两个动态连接(亚胺和硼酸酯)制备的。利用四组分的乌吉反应,在链的两端分别带有苯甲醛和苯基硼酸基,可方便地合成多官能团聚乙二醇(MF-PEG)。在温和的条件下(pH值约为7,25℃),这种微球与聚乙烯醇同时通过硼酸酯和乙二醇壳聚糖通过亚胺进行交联,在几秒钟内生成了具有独特DDN结构的自愈水凝胶。由于互补的互穿动态网络,所制备的水凝胶显示出更高的强度和粘附性。DDN水凝胶具有良好的生物相容性,并在小鼠体内实验中得到应用。该水凝胶注射成功地输送了一种抗肿瘤药物,与传统的输送方式相比,取得了更好的性能。据我们所知,这是首次利用UGI反应制备DDN自愈水凝胶的报道。在此,我们提出了一种简单的制备具有改进性能的自愈合材料的总体策略。该策略还为结合动态化学反应和多组分反应合成多功能/增强材料开辟了一条新的途径。
A self-healing hydrogel enriched with properties from a double-dynamic network (DDN) that has been prepared via two dynamic linkages (imine and borate ester) by using a single polymeric cross-linker. The four-component Ugi reaction was used for easily synthesizing multifunctional poly(ethylene glycol) (MF-PEG) with a benzaldehyde group and phenylboronic acid group at each end of the chain. This MF-PEG simultaneously cross-linked with poly(vinyl alcohol) through the borate ester and glycol chitosan via an imine to generate a self-healing hydrogel with a unique DDN structure in seconds under mild conditions (pH approximate to 7, 25 degrees C). The prepared hydrogel showed enhanced strength and mucoadhesive abilities because of the complimentary interpenetrating dynamic networks. The DDN hydrogel showed satisfying biocompatibility and was further used in an in vivo mouse model. The hydrogel was injected to successfully deliver an antitumor drug and achieved a superior performance compared to traditional delivery methods. To the best of our knowledge, this is the first report of using the Ugi reaction to prepare a DDN self-healing hydrogel. We hereby propose a general strategy for the facile preparation of self-healing materials with improved properties. The strategy also opens a new avenue for synthesizing multifunctional/reinforced materials with the combination of dynamic chemistry and multicomponent reactions.