Dynamic Graftable Liquid-Like Polymer Brush Coatings with Restorable Liquid Repellency

Covalently grafted liquid-like polymer brushes are central to liquid-repellent coatings but remain extremely difficult to regenerate once abraded. Here, we present a supramolecular strategy to overcome this limitation by constructing a highly dense hydrogen-bonded matrix capable of repeated brush grafting. The matrix was formed by 2-ureido-4[1H]-pyrimidinone (UPy) functionalized polyhedral oligomeric silsesquioxane (POSS), which established a rigid yet dynamic network. Poly(dimethylsiloxane) with polar terminal groups (BHPDMS) was subsequently inserted via hydrogen bonding and dipole interactions at elevated temperatures, creating a covalent-analogous polymer brush coating that resists fluid erosion while preserving dynamically reconfigurable. This coating exhibits hardness of 0.34 GPa, modulus of 5.91 GPa, and >90% optical transparency. Its liquid-repellent performance includes water sliding angle of 1.8°, together with antismudge and antigraffiti functionality. Moreover, the coating reduces ice adhesion to 20.4 kPa and extends freezing delay more than 10-fold relative to glass. Importantly, once abraded, BHPDMS can be repeatedly reinserted into the dense UPy-POSS framework at elevated temperatures, enabling full restoration of liquid-repellent functionality. This work establishes a supramolecular design principle that reconciles covalent-analogous stability with regraftable adaptability, opening new directions for durable and sustainable surface engineering.