Roquart Maïlie, Kharlamova Anna, Marcos Celada Lukas, Norvez Sophie, Nicolaÿ Renaud, Corté Laurent
Centre des Matériaux, MINES Paris, CNRS, PSL University, 91003 Evry, France.
Molecular, Macromolecular Chemistry, and Materials, ESPCI Paris, CNRS, PSL University, 75005 Paris, France.
Biomacromolecules. 2023 Oct 9;24(10):4454-4464. doi: 10.1021/acs.biomac.2c01265. Epub 2023 Feb 13.
We report the synthesis of networks having adjustable topologies and mechanical properties. Our approach consists of photopolymerizing poly(ethylene glycol) diacrylates (PEG-DA) in the presence of mixtures of mono- and multifunctional thiols. We show that the introduction of monothiols as non-cross-linking transfer agents provides a simple way to tune the topology of the networks and produce soft extensible networks. In a systematic study with model short PEG-DA ( = 700 g·mol), we explored how the gel point and network properties, such as the swelling ratio, the soluble fraction, the viscoelastic moduli, and the ultimate stress and strain, can be adjusted by varying the ratio of thiol to acrylate functions and the average functionality of the thiol mixture. We applied this strategy to longer chains of PEG-DA ( = 2300 and 3200 g·mol) and varied the viscoelastic and tensile responses of these networks to optimize their adhesive performance. This simple and robust approach further enriches the toolbox of thiol-acrylate polymerization and expands the application scope of PEG-based hydrogels.
我们报道了具有可调拓扑结构和机械性能的网络的合成。我们的方法包括在单官能和多官能硫醇混合物存在下光聚合聚乙二醇二丙烯酸酯（PEG-DA）。我们表明，引入单硫醇作为非交联转移剂提供了一种简单的方法来调节网络的拓扑结构并制备柔软可拉伸的网络。在对模型短PEG-DA（ = 700 g·mol）的系统研究中，我们探索了如何通过改变硫醇与丙烯酸酯官能团的比例以及硫醇混合物的平均官能度来调节凝胶点和网络性能，如溶胀率、可溶部分、粘弹性模量以及极限应力和应变。我们将此策略应用于更长链的PEG-DA（ = 2300和3200 g·mol），并改变这些网络的粘弹性和拉伸响应以优化其粘附性能。这种简单而稳健的方法进一步丰富了硫醇-丙烯酸酯聚合的工具库，并扩展了基于PEG的水凝胶的应用范围。
