Wang Rui, Gao Yifeng, Yu Kaixuan, Xu Ziqian, Ma Xiaofeng, Wu Linlin, Dou Qiang, Cui Sheng
College of Materials Science and Engineering, Nanjing Tech University, Nanjing, 211816, P. R. China.
College of Science, Nanjing Forestry University, Nanjing, 210037, P. R. China.
Macromol Rapid Commun. 2025 Feb;46(4):e2400832. doi: 10.1002/marc.202400832. Epub 2024 Dec 18.
Deep eutectic solvent (DES)-based eutectogels show significant promise for flexible sensors due to their high ionic conductivity, non-volatility, biocompatibility, and cost-effectiveness. However, achieving tough and stretchable eutectogels is challenging, as the highly polar DES tends to screen noncovalent bonds, such as hydrogen and ionic bonds, between polymer chains, limiting their mechanical strength. In this work, this issue is addressed by leveraging the limited solubility of zwitterionic polymers in a specific DES to induce phase separation, promoting dipole-dipole interactions between polymer chains. These interactions improve energy dissipation under mechanical stress, allowing the creation of tough and stretchable P(MAA-co-VIPS)/TBAC-EG eutectogels through a copolymerization-induced phase separation approach. Methacrylic acid (MAA) and sulfobetaine vinylimidazole (VIPS) are copolymerized within a tetrabutylammonium chloride-ethylene glycol (TBAC-EG) DES, resulting in a bicontinuous network. The bicontinuous structure consists of a PVIPS-rich phase that enhances toughness via dipole-dipole interactions, and a PMAA solvent-rich phase that enables high stretchability. The resulting eutectogel demonstrates excellent mechanical properties, including a strength of 1.76 MPa, toughness of 16.61 MJ m⁻, and remarkable stretchability of 1293%, along with self-recovery, self-healing, and shape-memory capabilities. The zwitterionic polymer-specific DES design opens up broad application potential for these eutectogels in diverse fields.
基于深共熔溶剂（DES）的低共熔凝胶因其高离子导电性、非挥发性、生物相容性和成本效益，在柔性传感器方面显示出巨大的潜力。然而，要制备坚韧且可拉伸的低共熔凝胶具有挑战性，因为高极性的DES往往会屏蔽聚合物链之间的非共价键，如氢键和离子键，从而限制了它们的机械强度。在这项工作中，通过利用两性离子聚合物在特定DES中的有限溶解度来诱导相分离，促进聚合物链之间的偶极-偶极相互作用，解决了这个问题。这些相互作用改善了机械应力下的能量耗散，从而通过共聚诱导相分离方法制备出坚韧且可拉伸的P（MAA-co-VIPS）/TBAC-EG低共熔凝胶。甲基丙烯酸（MAA）和磺基甜菜碱乙烯基咪唑（VIPS）在四丁基氯化铵-乙二醇（TBAC-EG）DES中共聚，形成双连续网络。双连续结构由通过偶极-偶极相互作用提高韧性的富含PVIPS的相和实现高拉伸性的富含PMAA溶剂的相组成。所得的低共熔凝胶表现出优异的机械性能，包括1.76 MPa的强度、16.61 MJ m⁻³的韧性、1293%的显著拉伸性，以及自恢复、自愈合和形状记忆能力。两性离子聚合物特定的DES设计为这些低共熔凝胶在不同领域开辟了广阔的应用潜力。
