Thermoresponsive Polyrotaxane Aerogels: Converting Molecular Necklaces into Tough Porous Monoliths

Polyrotaxanes (PRs) are supramolecular systems that combine with several cyclic molecules threaded on a linear molecule, and have been widely applied in molecular abacus, stimuli-responsive systems, self-healing materials, etc. The fabrication of macroscopic porous PR monoliths, which is expected to impart more functions, has not been realized yet. PR aerogels featuring with high specific surface area (232 m 2 /g), high strength (74.7 MPa), and temperature-responsiveness have been synthesized in this work by introducing poly( N -isopropylacrylamide) to the molecular necklaces followed by chemical cross-linking with a rigid cross-linker and supercritical fluid drying in sequence, which might open a new door toward smart macroscopic porous materials.