Institute for Complex Molecular Systems, Eindhoven University of Technology, P.O. Box 513, Eindhoven, MB 5600, The Netherlands.
Laboratory of Chemical Biology, Department of Biomedical Engineering, Eindhoven University of Technology, P.O. Box 513, Eindhoven, MB 5600, The Netherlands.
Adv Mater. 2021 Sep;33(37):e2008111. doi: 10.1002/adma.202008111. Epub 2021 Aug 1.
The extracellular matrix (ECM) forms through hierarchical assembly of small and larger polymeric molecules into a transient, hydrogel-like fibrous network that provides mechanical support and biochemical cues to cells. Synthetic, fibrous supramolecular networks formed via non-covalent assembly of various molecules are therefore potential candidates as synthetic mimics of the natural ECM, provided that functionalization with biochemical cues is effective. Here, combinations of slow and fast exchanging molecules that self-assemble into supramolecular fibers are employed to form transient hydrogel networks with tunable dynamic behavior. Obtained results prove that modulating the ratio between these molecules dictates the extent of dynamic behavior of the hydrogels at both the molecular and the network level, which is proposed to enable effective incorporation of cell-adhesive functionalities in these materials. Excitingly, the dynamic nature of the supramolecular components in this system can be conveniently employed to formulate multicomponent supramolecular hydrogels for easy culturing and encapsulation of single cells, spheroids, and organoids. Importantly, these findings highlight the significance of molecular design and exchange dynamics for the application of supramolecular hydrogels as synthetic ECM mimics.
细胞外基质（ECM）通过小分子和大分子聚合物的分级组装形成，形成一种短暂的、水凝胶样的纤维网络，为细胞提供机械支撑和生化信号。因此，通过各种分子的非共价组装形成的合成纤维超分子网络是天然 ECM 的潜在合成模拟物，只要生化信号的功能化有效。在这里，采用缓慢和快速交换分子的组合，自组装成超分子纤维，形成具有可调动态行为的瞬态水凝胶网络。研究结果证明，调节这些分子之间的比例可以控制水凝胶在分子和网络水平上的动态行为的程度，这被认为可以有效地将细胞黏附功能整合到这些材料中。令人兴奋的是，该系统中超分子成分的动态特性可以方便地用于配方多组分超分子水凝胶，便于单细胞、球体和类器官的培养和封装。重要的是，这些发现强调了分子设计和交换动力学对于将超分子水凝胶用作合成 ECM 模拟物的应用的重要性。
