Aarts Jasper G M, Rovers Maritza M, Rutten Martin G T A, Dankers Patricia Y W
Institute for Complex Molecular Systems (ICMS), Eindhoven University of Technology, Eindhoven 5600 MB, The Netherlands.
Department of Biomedical Engineering, Eindhoven University of Technology, Eindhoven 5600 MB, The Netherlands.
J Am Chem Soc. 2025 Jun 4;147(22):18674-18684. doi: 10.1021/jacs.4c15102. Epub 2025 May 23.
Inspired by dynamic systems in nature, we can introduce dynamics into synthetic biomaterials through dynamic covalent bonds or supramolecular interactions. Combining both types of dynamic interactions may allow for advanced and innovative networks with multiple levels of dynamicity. Here we present two types of solid materials consisting of either dynamic covalent imine bonds or a combination of these dynamic covalent bonds with supramolecular hydrogen bonding ureido-pyrimidinone (UPy) units to obtain double dynamic materials. We showed the facile synthesis and formulation of both materials at room temperature. The thermal and physical properties of each material are highly tunable by altering the ratio and type of cross-linker. Interestingly, we showed that minimal amounts of UPy units result in a drastic increase in material mechanics. Furthermore, we show that both types of materials are suitable as biomaterials through functionalization with cell-adhesive peptides, through either a dynamic covalent imine bond or a supramolecular UPy moiety.
受自然界动态系统的启发,我们可以通过动态共价键或超分子相互作用将动力学引入合成生物材料中。结合这两种类型的动态相互作用可能会产生具有多层次动态性的先进创新网络。在此,我们展示了两种固体材料,一种由动态共价亚胺键组成,另一种由这些动态共价键与超分子氢键脲基嘧啶酮(UPy)单元组合而成,以获得双动态材料。我们展示了这两种材料在室温下的简便合成与配方。通过改变交联剂的比例和类型,每种材料的热性能和物理性能都具有高度可调性。有趣的是,我们发现极少量的UPy单元会导致材料力学性能急剧增加。此外,我们表明,通过用细胞黏附肽进行功能化,无论是通过动态共价亚胺键还是超分子UPy部分,这两种类型的材料都适合作为生物材料。