Photoreversible Bond-Based Shape Memory Polyurethanes with Light-Induced Self-Healing, Recyclability, and 3D Fluorescence Encryption

Developing a shape memory polyurethane with high mechanical properties, excellent self-healing has become a huge challenge for the development of smart materials. Herein, we report the design and fabrication of a shape memory polyurethane network terminated with coumarin units (HEOMC-PU) to address this conundrum. The synthesized HEOMC-PU exhibits exceptional mechanical performance with a breaking elongation of 746% and toughness of 55.5 MJ·m–3. By utilizing the dynamically reversible behavior of coumarin units to repair the damaged network, the efficient self-healing performance (99.2%) of HEOMC-PU is obtained. In addition, the prepared network and light-induced dynamic reversibility endow the HEOMC-PU with both liquid-state remoldability and solid-state plasticity, respectively, enabling polyurethane to be recycled and processed multiple times. Furthermore, based on the fluorescence responsive characteristic of coumarin, HEOMC-PU with a fluorescent pattern can be deformed into specific three-dimensional configurations by combining photolithography, self-healing, and the shape memory effect. Such a multilevel and multidimensional anti-counterfeiting platform with rewritable fluorescent patterns and reconfigurable shapes can open up a new encryption approach for future intelligent anti-counterfeiting.