Self‐Assembling Supramolecular Hybrid Hydrogel Beads

With the goal of imposing shape and structure on supramolecular gels, we combine a low-molecular-weight gelator (LMWG) with the polymer gelator (PG) calcium alginate in a hybrid hydrogel. By imposing thermal and temporal control of the orthogonal gelation methods, the system either forms an extended interpenetrating network or core-shell-structured gel beads-a rare example of a supramolecular gel formulated inside discrete gel spheres. The self-assembled LMWG retains its unique properties within the beads, such as remediating PdII and reducing it in situ to yield catalytically active Pd0 nanoparticles. A single PdNP-loaded gel bead can catalyse the Suzuki-Miyaura reaction, constituting a simple and easy-to-use reaction-dosing form. These uniquely shaped and structured LMWG-filled gel beads are a versatile platform technology with great potential in a range of applications.