Nanofilamentous Virus-Based Dynamic Hydrogels with Tunable Internal Structures, Injectability, Self-Healing, and Sugar Responsiveness at Physiological pH
Nanofilamentous Virus-Based Dynamic Hydrogels with Tunable Internal Structures, Injectability, Self-Healing, and Sugar Responsiveness at Physiological pH
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基于纳米丝病毒的动态水凝胶，具有可调节的内部结构、可注射性、自愈性和生理 pH 值下的糖响应性
DOI：
10.1021/acs.langmuir.8b02526
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发表时间：
2018
期刊：
影响因子：
3.9
通讯作者：
Zhang Zhenkun
中科院分区：
文献类型：
--
作者：
Zhi Xueli;Zheng Chunxiong;Xiong Jie;Li Jianyao;Zhao Chenxi;Shi Linqi;Zhang Zhenkun
随着水凝胶在生物材料、传感器、致动器和软机器人等领域的应用越来越广泛，迫切需要赋予一种凝胶多种物理化学性质，如刺激反应性、可注射性、自愈性和可调内部结构。然而，将这些备受追捧的特性同时融合到一种凝胶中是一项挑战。本文通过结合生物偶联化学、丝状病毒和动态共价键，提出了一个具有所有这些特性的概念性水凝胶系统。将定制合成的低苯基硼酸（PBA）衍生物与具有高长径比的定义良好的绿色纳米纤维M13病毒（PBA-M13）偶联，制备了具有二醇亲和力的纳米丝状生物偶联物。采用多种含二醇剂（如聚乙烯醇）通过经典的硼-二醇动态键交联PBA-M13，制备了机械强度可调的动态水凝胶。所制备的水凝胶具有良好的可注射性和自愈性，并且凝胶基质内病毒主干上的PBA片段易于化学接近。通过简单的剪切诱导病毒纳米纤维排列，将有序的内部结构传递到病毒基水凝胶中。在此基础上，利用含二醇分子扩散诱导原位凝胶法制备了独特的具有手性内部结构的水凝胶，用于固定PBA-M13病毒的手性液晶相。这种凝胶的糖反应性导致有效载荷如胰岛素的葡萄糖调节释放行为。所有这些特性都在生理pH值下实现，这将促进这些水凝胶作为生物材料的未来应用。
With expanding applications of hydrogels in diverse fields ranging from biomaterials to sensors, actuators, and soft robotics, there is an urgent need to endow one single gel with multiple physicochemical properties, such as stimuli-responsiveness, injectability, self-healing, and tunable internal structures. However, it is challenging to simultaneously incorporate these highly sought-after properties into one single gel. Herein, a conceptual hydrogel system with all of these properties is presented via combining bioconjugate chemistry, filamentous viruses, and dynamic covalent bonds. Nanofilamentous bioconjugates with diol affinity were prepared by coupling a tailor-synthesized low-pKaphenylboronic acid (PBA) derivative to a well-defined green nanofiber the M13 virus with a high aspect ratio (PBA-M13). Dynamic hydrogels with tunable mechanical strength were prepared by using multiple diol-containing agents such as poly(vinyl alcohol) to cross-link such PBA-M13 via the classic boronic–diol dynamic bonds. The as-prepared hydrogels exhibit excellent injectability and self-healing behaviors as well as easy chemical accessibility of the PBA moieties on the virus backbone inside the gel matrix. Ordered internal structures were imparted into virus-based hydrogels by simple shear-induced alignment of the virus nanofibers. Furthermore, unique hydrogels with chiral internal structures were fabricated through in situ gelation induced by diffusion of diol-containing molecules to fix the chiral liquid crystal phase of the PBA-M13 virus. Sugar responsiveness of this gel leads to a glucose-regulated release behavior of payloads such as insulin. All of these properties have been implemented at physiological pH, which will facilitate future applications of these hydrogels as biomaterials.