It remains a challenge to use a simple approach to fabricate a multi-shape memory material with high mechanical performances. Here, we report a triple crosslinking design to construct a multi-shape memory epoxy vitrimer (MSMEV), which exhibits high mechanical properties, multi-shape memory property and malleability. The triple crosslinking network is formed by reacting diglycidyl ether of bisphenol F (DGEBF) with 4-aminophenyl disulfide, γ-aminopropyltriethoxysilane (APTS) and poly(propylene glycol) bis(2-aminopropyl ether) (D2000). The triple crosslinking manifests triple functions: the disulfide bonds and the silyl ether linkages enable malleability of the epoxy network; the silyl ether linkages impart the network with high heterogeneity and broaden the glass transition region, leading to multi-shape memory property; a small amount of D2000 increases the modulus difference between the glassy and rubbery states, thereby improving the shape fixity ratio. Meanwhile, the high crosslinking density and rigid structure provide the MSMEV with high tensile strength and Young’s modulus. Moreover, integrating carbon fibers and MSMEV results in shape memory composites. The superior mechanical properties of the composites and the recyclability of carbon fiber derived from the dissolvability of MSMEV make the composites hold great promise as structural materials in varied applications.

使用简单的方法来制造具有高机械性能的多形状记忆材料仍然是一个挑战。在这里，我们报告了一种三重交联设计，以构建一种具有高机械性能，多形状记忆性能和延展性的多形状记忆环氧微晶玻璃（MSMEV）。三联交联网络是通过双酚F的二缩水甘油醚（DGEBF）与4-氨基苯基二硫化物γ反应形成的-氨基丙基三乙氧基硅烷（APTS）和聚丙二醇双（2-氨基丙基醚）（D2000）。三重交联表现出三重功能：二硫键和甲硅烷基醚键可实现环氧网络的延展性；甲硅烷基醚键赋予网络高度的不均一性并拓宽了玻璃化转变区域，从而导致了多种形状的记忆性能。少量的D2000会增加玻璃态和橡胶态之间的模量差，从而提高形状固定率。同时，高交联密度和刚性结构为MSMEV提供了高拉伸强度和杨氏模量。此外，将碳纤维和MSMEV集成在一起会产生形状记忆复合材料。