Polymerization‐Induced Self‐Assembly for the Synthesis of Multi‐Responsive Micelles Hydrogel and its Versatile Applications

Poly(N-isopropyl acrylamide) (PNIPAM) is well-known for its lower critical solution temperature (LCST) and widely studied as thermo-responsive micelles for various applications. However, the synthesis of micelles with precise structures often involves complex process. Herein, we developed a novel multi-responsive micelles hydrogel GBN, which was prepared by combining the polymerization-induced self-assembly (PISA) of poly(N-isopropyl acrylamide)-poly (glycerol methacrylate) (PGMA_x-PNIPAM) and B─O crosslinking the micelles. The yielded micelles with stable worm-like structures, easily form a hydrogel through significant entanglement. The thermo-responsiveness of these micelles facilitates a reversible gel-sol transition, accompanied by changes in transparency, making them suitable for thermal management in smart window applications. Additionally, the glucose responsiveness associated with the dynamic B─O bonds address the incompatibility of PNIPAM's LCST temperature for drug release applications. Importantly, we discovered that the GNB hydrogel can also function as sealing material; its thermo-responsiveness enables the formation of liquid gaskets that uniformly fill rough surfaces. In its gel state, it exhibits stable load-bearing capacity, sealing strength, and consistent friction coefficients, making it applicable in both static and dynamic sealing scenarios to tackle sealing challenges in extreme environments. Thus, this work offers a novel approach for fabricating stimulus-responsive materials, broadening the application scope of PNIPAM in various fields.