Processable and Luminescent Supramolecular Hydrogels from Complex Coacervation of Polycations with Lanthanide Coordination Polyanions

Luminescent supramolecular gels based on dynamic lanthanide coordination can be of profound interest in optical and sensing applications. However, most of the current lanthanide-based gels suffer from their poor mechanical strength and processability for practical uses. Here, we develop an effective strategy to fabricate a multifunctional robust luminescent hydrogel via the ionic coacervation of an anionic lanthanide coordination polymer with a cationic polyelectrolyte. The resultant hydrogels turn out to be moldable, self-healable, recyclable, and may be regarded as a new kind of “luminescent plastic”. Owing to the unique force-induced plastic deformation, long fibers can be directly drawn from the hydrogel reservoir at room temperature. Moreover, the dynamic nature of such a physical polymer network leads to multiple responses to various stimuli, such as temperature, salt, and sonication. The studies described herein not only enable the easy processability of luminescent hydrogels, but also provide a new strategy to prepare stimuli-responsive and self-healing lanthanide-based hydrogels as sustainable and smart materials.