苯硼酸
自愈水凝胶
共价键
硼酸
化学
限制
动态共价化学
组合化学
生物化学
生物物理学
分子
有机化学
催化作用
超分子化学
生物
机械工程
工程类
作者
Yuanhui Xiang,Sijie Xian,Rachel C. Ollier,Sihan Yu,Bo Su,Irawan Pramudya,Matthew J. Webber
标识
DOI:10.1016/j.jconrel.2022.06.016
摘要
Dynamic-covalent motifs are increasingly used for hydrogel crosslinking, leveraging equilibrium-governed reversible bonds to prepare viscoelastic materials with dynamic properties and self-healing character. The bonding between aryl boronates and diols is one dynamic-covalent chemistry of interest. The extent of network crosslinking using this motif may be subject to competition from ambient diols such as glucose; this approach has long been explored for glucose-directed release of insulin to control diabetes. However, the majority of such work has used phenylboronic acids (PBAs) that suffer from low-affinity glucose binding, limiting material responsiveness. Moreover, many PBA chemistries also bind with higher affinity to certain non-glucose analytes like fructose and lactate than they do to glucose, limiting their specificity of sensing and therapeutic deployment. Here, dynamic-covalent hydrogels are prepared that, for the first time, use a new diboronate motif with enhanced glucose binding-and importantly improved glucose specificity-leveraging the ability of rigid diboronates to simultaneously bind two sites on a single glucose molecule. Compared to long-used PBA-based approaches, diboronate hydrogels offer more glucose-responsive insulin release that is minimally impacted by non-glucose analytes. Improved responsiveness translates to more rapid blood glucose correction in a rodent diabetes model. Accordingly, this new dynamic-covalent crosslinking chemistry is useful in realizing more sensitive and specific glucose-responsive materials.
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