通过苯并恶硼烷和羟基之间的动态共价键形成的可注射、自修复和多重响应水凝胶。

Injectable, Self-Healing, and Multi-Responsive Hydrogels via Dynamic Covalent Bond Formation between Benzoxaborole and Hydroxyl Groups.

机构信息

School of Ophthalmology & Optometry, Eye Hospital , Wenzhou Medical University , Wenzhou , Zhejiang 325027 , China.

Department of Chemical and Materials Engineering , University of Alberta , Edmonton , Alberta T6G 2G6 , Canada.

出版信息

Biomacromolecules. 2019 Feb 11;20(2):1028-1035. doi: 10.1021/acs.biomac.8b01652. Epub 2019 Jan 11.

Abstract

Hydrogels that are injectable, self-healing, and multiresponsive are becoming increasingly relevant for a wide range of applications. In this work, we have successfully developed a novel approach in the fabrication of smart hydrogels with all the above properties. A symmetrical ABA triblock copolymer was first synthesized via atom transfer radical polymerization with a temperature responsive middle block and two permanently hydrophilic glycopolymer chains on both ends. Hydrogels were subsequently constructed by mixing the triblock copolymer with another linear hydrophilic copolymer bearing benzoxaborole groups. The interactions of the benzoxaborole groups with the sugar hydroxyl groups allowed the formation of dynamic covalent bonds. The resulting hydrogels exhibited temperature, pH, and sugar responsiveness. Rheological studies confirmed that the mechanical property can be tuned by changing the pH as well as the galactose/benzoxaborole molar ratio. Furthermore, the hydrogels showed excellent self-healing ability and shear-thinning performance due to the inherent well-known dynamic covalent bonds of boronic esters. Therefore, these types of hydrogels can have excellent biomedical applications.

摘要

可注射、自修复和多重响应的水凝胶在广泛的应用中变得越来越重要。在这项工作中,我们成功地开发了一种新的方法来制备具有所有上述特性的智能水凝胶。首先通过原子转移自由基聚合合成了一种对称的 ABA 三嵌段共聚物,该共聚物具有温度响应性的中间嵌段和两个永久亲水糖聚合物链在两端。随后通过将三嵌段共聚物与另一个带有苯并恶唑基团的线性亲水性共聚物混合来构建水凝胶。苯并恶唑基团与糖羟基之间的相互作用允许形成动态共价键。所得水凝胶表现出温度、pH 和糖响应性。流变学研究证实,通过改变 pH 值以及半乳糖/苯并恶唑摩尔比可以调节机械性能。此外,由于硼酸酯固有的众所周知的动态共价键,水凝胶表现出优异的自修复能力和剪切稀化性能。因此,这类水凝胶可以有很好的生物医学应用。

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