Wu Xiankun, Li Min, Li Haonan, Gao Huihui, Wang Zhongkai, Wang Zhong
Biomass Molecular Engineering Center, Anhui Provincial Engineering Center for High Performance Biobased Nylons, School of Materials and Chemistry, Anhui Agricultural University, Hefei, Anhui, 230036, China.
Small. 2024 Aug;20(35):e2311131. doi: 10.1002/smll.202311131. Epub 2024 Apr 21.
High-efficient underwater self-healing materials with reliable mechanical attributes hold great promise for applications in ocean explorations and diverse underwater operations. Nevertheless, achieving these functions in aquatic environments is challenging because the recombination of dynamic interactions will suffer from resistance to interfacial water molecules. Herein, an ultra-robust and all-environment stable self-healable polyurethane-amide supramolecular elastomer is developed through rational engineering of hydrophobic domains and multistrength hydrogen bonding interactions to provide mechanical and healing compatibility as well as efficient suppression of water ingress. The coupling of hydrophobic chains and hierarchical hydrogen bonds within a multiphase matrix self-assemble to generate dynamical hydrophobic hard-phase microdomains, which synergistically realize high stretchability (1601%), extreme toughness (87.1 MJ m), and outstanding capability to autonomous self-healing in various harsh aqueous conditions with an efficiency of 58% and healed strength of 12.7 MPa underwater. Furthermore, the self-aggregation of hydrophobic clusters with sufficient dynamic interactions endows the resultant elastomer with effective instantaneous adhesion (6.2 MPa, 941.9 N m) in extremely harsh aqueous conditions. It is revealed that the dynamical hydrophobic hard-phase microdomain composed of hydrophobic barriers and cooperative reversible interactions allows for regulating its mechanical enhancement and underwater self-healing efficiency, enabling the elastomers as intelligent sealing devices in marine applications.
具有可靠机械性能的高效水下自修复材料在海洋探索和各种水下作业中具有广阔的应用前景。然而，在水环境中实现这些功能具有挑战性，因为动态相互作用的重组会受到界面水分子的阻碍。在此，通过对疏水域和多强度氢键相互作用进行合理设计，开发出一种超坚固且全环境稳定的自修复聚氨酯 - 酰胺超分子弹性体，以提供机械和修复兼容性，并有效抑制水分侵入。多相基质中疏水链和分级氢键的耦合自组装形成动态疏水硬相微区，协同实现高拉伸性（1601%）、极高韧性（87.1 MJ·m）以及在各种苛刻水性条件下的出色自主自修复能力，水下自修复效率达58%，修复强度为12.7 MPa。此外，具有足够动态相互作用的疏水簇的自聚集赋予所得弹性体在极其苛刻的水性条件下有效的瞬时粘附力（6.2 MPa，941.9 N·m）。研究表明，由疏水屏障和协同可逆相互作用组成的动态疏水硬相微区能够调节其机械增强和水下自修复效率，使弹性体成为海洋应用中的智能密封装置。
