One‐Pot Synthesis of Polyelectrolyte‐Triazine Gels Using Cation–π Interactions and Multiple Hydrogen Bonds for Adjustable Interfacial Adhesion

Abstract The poor adhesion performance of typical gels still remains a challenge to find a simple method to achieve strong and reversible adhesion with the existence of water. Here, a poly(acryloyloxyethyl trimethyl ammonium chloride‐ co ‐2‐vinyl‐4‐6‐diamino‐1,3,5‐triazine) (P(DAC‐ co ‐VDT)) gel with high and adjustable interfacial adhesion is fabricated by combining cation‐triazine π interaction and multiple hydrogen bonding and through a one‐pot route. Characterization of the gels reveals that the two types of interactions are introduced into the gel network and that the gel–gel and gel–glass interfacial adhesion can be readily adjusted in a wide range from 15.98 to 123.60 kPa. This approach enables the creation of high‐strength composites using P(DAC‐ co ‐VDT) gel as matrix, anionic monomer sodium p‐styrene sulfonate as ion concentration adjustor, and discrete quartz sands as filler with easy and repeated moldability and self‐healing capability.