Shape memory polymer (SMP)-based smart molds, which could provide high-resolution mold shape and morph in response to external stimuli for readily demolding the complex structure, attract extensive attention. However, the suitable SMP for smart molds is usually confined with low stretchability that likely causes damage during demolding. Herein, we present a cyanate ester smart composite (CESC) with a reconfigurable, solvent-processable, and near-infrared (NIR)-triggerable shape memory effect (SME), which enables the 2D sheet with a variety of morphed complex shapes through deformation in a mild situation. Notably, the reconfigurable SME and the recyclability of the shape memory cyanate ester (SMCE) were addressed for the first time, attributed to the dynamic covalent bonds of transesterification and the novel cyanurate exchange. In addition, we found that the mechanism of solvent-processable SME is attributed to the varied cross-linking density and the mobility of the polymer chain. Integrating the multiple responsive SME and reconfigurable SME, the CESC demonstrated versatile applications as a smart mold. The results demonstrate a wide scope of application of the integrated SME and provide a new design strategy for thermoset cyanate materials.
Keywords: NIR-triggerable; dynamic covalent bond; shape memory cyanate ester; smart mold; solvent-processable.