Stimuli-Responsive Hydrogels with Antibacterial Activity Assembled from Guanosine, Aminoglycoside, and a Bifunctional Anchor
Stimuli-Responsive Hydrogels with Antibacterial Activity Assembled from Guanosine, Aminoglycoside, and a Bifunctional Anchor
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由鸟苷、氨基糖苷和双功能锚组装而成的具有抗菌活性的刺激响应水凝胶。
DOI：
10.1002/adhm.201901329
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发表时间：
2019-12-09
影响因子：
10
通讯作者：
Zhang, Yadong
中科院分区：
文献类型：
--
作者：
Hu, Jingjing;Hu, Qianyu;Zhang, Yadong
具有特殊功能的多刺激响应型水凝胶在生物医学中的应用引起了人们的极大兴趣；然而，这些智能水凝胶通常需要预先合成具有多个配体的大分子构建块，并将生物活性物质整合到凝胶中。在这里，通过超分子组装和亚胺硼酸盐化学的结合，报道了一种具有强大抗菌活性的多刺激响应水凝胶。该水凝胶由包括氨基糖苷、鸟苷、钾离子在内的全小分子构筑块和一个同时含有硼酸和醛基的双功能锚链组成。鸟苷在钾离子存在下通过超分子组装形成四链，而双功能锚链通过动态亚胺硼酸化学将一类有效的抗生素氨基糖苷连接到四链上的顺式二醇基团，得到一种含有丰富抗生素的智能水凝胶。水凝胶对多种刺激很敏感，如热、酸、氧化剂、葡萄糖和冠醚，这些刺激促进了抗生素从凝胶中的释放。此外，所制备的水凝胶在体外和体内都显示出很强的抗菌活性。这一结果为利用全小分子构筑块通过简易化学方法制备具有多刺激响应性的抗菌水凝胶提供了新的选择。
Multistimuli-responsive hydrogels with specific functions have attracted great interest for biomedical applications; however, these smart hydrogels usually require the presynthesis of macromolecular building blocks with multiple ligands and the integration of bioactive cargoes into the gels. Here, a multistimuli-responsive hydrogel with potent antibacterial activity by a combination of supramolecular assembly and iminoboronate chemistry is reported. The hydrogel consists of all-small-molecule building blocks including aminoglycoside, guanosine, potassium ion, and a bifunctional anchor bearing both boronic acid and aldehyde groups. Guanosines form quadruplexes in the presence of potassium ions via supramolecular assembly, and the bifunctional anchor connects aminoglycosides, a class of potent antibiotics to cis-diol groups on quadruplexes via dynamic iminoboronate chemistry, yielding a smart hydrogel containing abundant antibiotics. The hydrogel is sensitive to multistimuli such as heat, acids, oxidants, glucose and crown ether, which promote the release of antibiotics from the gels. Moreover, the prepared hydrogels show potent antibacterial activities both in vitro and in vivo. The results provide a new option to prepare antibacterial hydrogels with multistimuli responsiveness via facile chemistry using all-small-molecule building blocks.