A Functioning Macroscopic “Rubik's Cube” Assembled via Controllable Dynamic Covalent Interactions

Abstract The dynamic behavior of a macroscopic adhered hydrogel stabilized through controllable dynamic covalent interactions is reported. These interactions, involving the cross‐linked formation of a hydrogel through reaction of a diacylhydrazine precursor with a tetraformyl partner, increase as a function of time. By using a contact time of 24 h and different compounds with recognized aggregation‐induced emission features (AIEgens), it proves possible to create six laminated acylhydrazone hydrogels displaying different fluorescent colors. Blocks of these hydrogels are then adhered into a structure resembling a Rubik's Cube, a trademark of Rubik's Brand Limited, (RC) and allowed to anneal for 1 h. This produces a 3 × 3 × 3 block (RC) wherein the individual fluorescent gel blocks are loosely adhered to one another. As a consequence, the 1 × 3 × 3 layers making up the RC can be rotated either horizontally or vertically to produce new patterns. Ex situ modification of the RC or application of a chemical stimulus can be used to produce new color arrangements. The present RC structure highlights how the temporal features, strong versus weak adhesion, may be exploited to create smart macroscopic structures.