A highly tough and conductive hydrogel with good shape memory behavior was facilely prepared via constructing the catechol-Fe³⁺ interactions in the poly(vinyl alcohol) (PVA) hydrogel matrix. The hydrophobic 5,5,6,6-tetrahydroxy-3,3,3,3-tetramethyl-1,1-spirobisindane (TTSBI) was introduced to provide the catechol ligands for Fe³⁺. The fabricated [email protected]³⁺-12 nanocomposite hydrogel performed great toughness (9.23 MJ/m³), large tensile strength (3.25 MPa) and high extensibility (752%). The distinguished mechanical performance of the composite hydrogel was contributed by the synergy of nanophase separation structure formed by TTSBI in PVA matrix, strong hydrogen bonding interaction between PVA and TTSBI, and metal coordination interaction of catechol-Fe³⁺. The introduced Fe³⁺ also imparted good conductivity to the hydrogel. Moreover, the mechanical and conductive properties of the composite hydrogel could be flexibly regulated by the pH value. The conductive hydrogel showed excellent sensitivity to stretching, bending, twist, and compression. In addition, the hydrogel exhibited multiple-stimuli responsive shape memory behaviors. This work offers a hierarchical self-assembly strategy to fabricate functional hydrogel with tailored mechanical, conductive properties and shape memory behavior for a series of promising applications such as flexible wearable electronics and intelligent actuators.

通过在聚乙烯醇（PVA）水凝胶基质中构建邻苯二酚-Fe ³⁺相互作用，可以轻松地制备具有良好形状记忆行为的高韧性导电水凝胶。引入疏水的5,5,6,6-四羟基-3,3,3,3-四甲基-1,1-螺双茚满（TTSBI）以提供Fe ³⁺的邻苯二酚配体。制成的[受电子邮件保护的] ³⁺ -12纳米复合水凝胶具有出色的韧性（9.23 MJ / m ³），大拉伸强度（3.25 MPa）和高延展性（752％）。TPSBI在PVA基质中形成的纳米相分离结构的协同作用，PVA与TTSBI之间的强氢键相互作用以及邻苯二酚-Fe ^3+的金属配位相互作用有助于形成复合水凝胶的卓越机械性能。引入的Fe ³⁺还赋予水凝胶良好的导电性。而且，复合水凝胶的机械和导电性能可以通过pH值灵活地调节。导电水凝胶对拉伸，弯曲，扭曲和压缩表现出极好的敏感性。此外，水凝胶表现出多种刺激响应的形状记忆行为。这项工作提供了一种分层的自组装策略，可以为一系列有前景的应用（例如柔性可穿戴电子设备和智能执行器）制造具有定制的机械，导电特性和形状记忆特性的功能性水凝胶。