College of Science, and Hebei Research Center of Pharmaceutical and Chemical Engineering, Hebei University of Science and Technology, Yuhua Road 70, Shijiazhuang 050080, PR China.
Nanoscale. 2019 Feb 28;11(9):4044-4052. doi: 10.1039/c8nr08532c.
Biomolecule-based hydrogels have potential use in a wide range of applications such as controlled drug release, tissue engineering, and biofabrication. Herein, driven by specific interactions between ds-DNA (double-stranded DNA) and Zn2+ based metal-complexes, we report that the use of DNA as cross-linkers can enhance interactions between self-assembling Zn2+ complexes containing terpyridine and sugar groups in the generation of bioinspired hydrogels from solutions or suspensions. The gelation process is fast and straightforward without tedious steps and happens at room temperature. Such a hydrogelation process of different Zn2+ complexes endows the visualized and selective DNA analogue discrimination. Several experiments suggest that the strong intercalation binding of Zn2+ complexes with ds-DNA results in the unzipping of ds-DNA into ss-DNA (single-stranded DNA), which further behave as linkers to enhance the intermolecular interactions of self-assembling Zn2+ complex molecules via coordination interactions. This work demonstrates an efficient and universal strategy to prepare hydrogels based on biomolecular recognition. Moreover, the DNA responsive behaviors of Zn2+ complexes are further compared with that of solutions and cells.
基于生物分子的水凝胶在药物控制释放、组织工程和生物制造等广泛应用中有潜在用途。在此,受 ds-DNA(双链 DNA)与基于 Zn2+的金属配合物之间的特定相互作用的驱动,我们报告说,使用 DNA 作为交联剂可以增强含有嘧啶和糖基的自组装 Zn2+配合物之间的相互作用,从而从溶液或悬浮液中生成仿生水凝胶。凝胶化过程快速而直接,无需繁琐的步骤,且在室温下发生。不同 Zn2+配合物的这种水凝胶化过程赋予了可视化和选择性的 DNA 类似物的区分。多项实验表明,Zn2+配合物与 ds-DNA 的强嵌入结合导致 ds-DNA 解链成 ss-DNA(单链 DNA),ss-DNA 进一步作为连接子,通过配位相互作用增强自组装 Zn2+配合物分子的分子间相互作用。这项工作展示了一种基于生物分子识别制备水凝胶的有效且通用的策略。此外,还进一步比较了 Zn2+配合物的 DNA 响应行为与溶液和细胞中的行为。