Persistent Room‐Temperature Phosphorescent Organohydrogels Based on Nonaromatic Luminogens Crosslinked by Hydrogen Bonds

Abstract The development of persistent room‐temperature phosphorescent (pRTP) hydrogels is important for the practical applications of organic phosphors. Unfortunately, the phosphorescence emission of nontraditional luminogens (NTLs) can be strongly quenched by water in hydrogel networks. Herein, a series of pRTP organohydrogels based on NTLs are prepared by dissolving poly(vinyl alcohol) (PVA), biuret (BIU) and poly(maleic acid) (PMAc) (or other nonaromatic macromolecular acids) in a glycerol/water mixed solvent, followed by a simple freezing‐thawing treatment. Very impressively, the organohydrogel exhibits remarkable excitation‐dependent and metal cation‐responsive phosphorescence with a maximum lifetime up to 782.8 ms at ambient conditions. Moreover, the organohydrogels treated with metal cations also have excitation‐dependent phosphorescence. Multidimensional information encryption can be achieved by simply printing solutions of metal cations onto the gel surface and switching the irradiation lights, or using gel blocks prepared with different macromolecular acids. Structural characterizations, mechanical tests, and comparative studies prove that hydrogen bonding between BIU and macromolecular chains leads to rigidification of molecular conformations and the cooperative effect of the components leads to the pRTP of the organohydrogels. This work provides a reliable strategy for the preparation of nonaromatic phosphorescent hydrogels with long afterglows and greatly expands the practical applications of phosphorescent materials.