A new supramolecular hydrogel with superior self-healing and shape memory properties was synthesized via in-situ copolymerization of the adamantane-containing monomer N-adamantylacrylamide (Ad-AAm) and monomer acrylic acid (AAc) in the polycyclodextrin (PCD) aqueous solution, where PCD served as the polyfunctional physical cross-linker. The PCD-Ad hydrogels showed strength of 40 kPa with breaking strain of 600%, but small tensile loading-unloading hysteresis and residual deformation benefited from the reversible crosslinking structure. Excellent self-healing property was realized at 70 °C and humid condition. The healing percentage reached over 70% after 120 min, which showed enhanced self-healing efficiency compared with the reported supramolecular hydrogels crosslinked by CD and Ad. This may benefit from the polyfunctional PCD crosslinking reagent, which provided more host sites and binding opportunities for the complexation during the self-healing process. Shape memory behavior was also realized through the reversible second crosslinked network by the carboxyl groups of PAAc with Fe³⁺ ions. The present study provides a new method to improve self-healing ability of the supramolecular hydrogels, which will find the applications in self-healing coating, biomedical materials and soft actuators.

通过含金刚烷单体N的原位共聚合成了具有超强自愈性和形状记忆性能的新型超分子水凝胶。多环糊精（PCD）水溶液中的-金刚烷基丙烯酰胺（Ad-AAm）和单体丙烯酸（AAc），其中PCD用作多官能物理交联剂。PCD-Ad水凝胶的强度为40 kPa，断裂应变为600％，但是可逆的交联结构使拉伸和卸载的磁滞小，残余变形小。在70°C和潮湿条件下均具有出色的自愈性能。120分钟后，治愈率达到70％以上，与通过CD和Ad交联的超分子水凝胶相比，自愈效率更高。这可能得益于多官能PCD交联试剂，该试剂为自修复过程中的络合物提供了更多的宿主位点和结合机会。³⁺离子。本研究提供了一种提高超分子水凝胶自愈能力的新方法，它将在自愈涂层，生物医学材料和软致动器中找到应用。