Coordination-Triggered Hierarchical Folate/Zinc Supramolecular Hydrogels Leading to Printable Biomaterials
Coordination-Triggered Hierarchical Folate/Zinc Supramolecular Hydrogels Leading to Printable Biomaterials
复制标题
协调触发的分层叶酸/锌超分子水凝胶导致可打印生物材料
DOI：
10.1021/acsami.7b18155
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发表时间：
2018-02-07
影响因子：
9.5
通讯作者：
Yan, Yun
中科院分区：
文献类型：
--
作者：
Liu, Kaerdun;Zang, Shihao;Yan, Yun
生物工程中所需的可打印水凝胶对生物相容性和机械强度有极高的要求，这在由生物聚合物制成的常规水凝胶中很难实现。在这里，我们表明，就业的协调触发的层次自组装的天然小分子叶酸，超分子水凝胶具有强大的机械弹性模量合成的双网络聚合物凝胶的战略可以在浓度低于1%。这种非凡的水凝胶的形成涉及一系列分层步骤：叶酸上的petrin环通过氢键形成四聚体，四聚体通过π-π堆叠堆叠成纳米纤维，锌离子将纳米纤维交联成更大规模的原纤维，并进一步将原纤维网络交联成凝胶水。这些超分子性质赋予水凝胶剪切稀化和即时愈合能力，这使得坚固的凝胶可注射和打印成各种三维结构。由于该凝胶具有良好的生物相容性，可三维支撑细胞，可用作显像剂（Gd 3+）和化疗药物的理想载体。这种新发现的金属-叶酸超分子水凝胶具有易形成、来源丰富等特点，在生物工程技术中具有广阔的应用前景。
Printable hydrogels desired in bioengineering have extremely high demands on biocompatibility and mechanic strength, which can hardly be achieved in conventional hydrogels made with biopolymers. Here, we show that on employment of the strategy of coordination-triggered hierarchical self-assembly of naturally occurring small-molecule folic acid, supramolecular hydrogels with robust mechanical elastic modulus comparable to synthetic double-network polymer gels can be made at concentrations below 1%. A sequence of hierarchical steps are involved in the formation of this extraordinary hydrogel: petrin rings on folate form tetramers through hydrogen bonding, tetramers stack into nanofibers by pi-pi stacking, and zinc ions cross-link the nanofibers into larger-scale fibrils and further cross-link the fibril network to gel water. These supramolecular qualities endow the hydrogel with shear-thinning and instant healing ability, which makes the robust gel injectable and printable into various three-dimensional structures. Owing to the excellent biocompatibility, the gel can support cells three-dimensionally and can be used as an ideal carrier for imaging agent (Gd3+), as well as chemodrugs. In combination with its easy formation and abundant sources, this newly discovered metallo-folate supramolecular hydrogel is promising in various bioengineering technological applications.