Huang Zehuan, Chen Xiaoyi, O'Neill Stephen J K, Wu Guanglu, Whitaker Daniel J, Li Jiaxuan, McCune Jade A, Scherman Oren A
Melville Laboratory for Polymer Synthesis, Yusuf Hamied Department of Chemistry, University of Cambridge, Cambridge, UK.
Nat Mater. 2022 Jan;21(1):103-109. doi: 10.1038/s41563-021-01124-x. Epub 2021 Nov 25.
Supramolecular polymer networks are non-covalently crosslinked soft materials that exhibit unique mechanical features such as self-healing, high toughness and stretchability. Previous studies have focused on optimizing such properties using fast-dissociative crosslinks (that is, for an aqueous system, dissociation rate constant k > 10 s). Herein, we describe non-covalent crosslinkers with slow, tuneable dissociation kinetics (k < 1 s) that enable high compressibility to supramolecular polymer networks. The resultant glass-like supramolecular networks have compressive strengths up to 100 MPa with no fracture, even when compressed at 93% strain over 12 cycles of compression and relaxation. Notably, these networks show a fast, room-temperature self-recovery (< 120 s), which may be useful for the design of high-performance soft materials. Retarding the dissociation kinetics of non-covalent crosslinks through structural control enables access of such glass-like supramolecular materials, holding substantial promise in applications including soft robotics, tissue engineering and wearable bioelectronics.
超分子聚合物网络是通过非共价交联形成的软材料，具有独特的机械特性，如自修复、高韧性和可拉伸性。以往的研究主要集中在使用快速解离交联（即对于水性体系，解离速率常数k>10 s）来优化这些性能。在此，我们描述了具有缓慢、可调节解离动力学（k<1 s）的非共价交联剂，其可使超分子聚合物网络具有高压缩性。所得的类玻璃超分子网络具有高达100 MPa的抗压强度且无断裂，即使在93%应变下经过12个压缩和松弛循环后也是如此。值得注意的是，这些网络在室温下能快速自我恢复（<120 s），这对于高性能软材料的设计可能是有用的。通过结构控制延缓非共价交联的解离动力学，能够获得此类类玻璃超分子材料，在包括软机器人技术、组织工程和可穿戴生物电子学等应用中具有巨大潜力。
