Fluorine‐ and Silicone‐Free Polymer for Smart Textile via Controlled Radical Polymerization and Its Multifunctional Applications

Superhydrophobic, scratch-healable, and sustainable coatings hold great promise for preparing smart textiles, particularly by enhancing functionality and durability while minimizing environmental impact. This study reports, for the first time, the development of a three-arm initiator (COBr₃) from castor oil (CO) and its use in reversible complexation-mediated polymerization (RCMP). A series of homo- and co-polymers, incorporating both petroleum-derived and bio-renewable monomers, are synthesized with moderate to high monomer conversions (35%-93%) and low dispersity (1.15-1.49). Specifically, star-P(SMA₄₅-r-FMA₂₂) and star-P(SMA₅₀-r-FMA₇) are synthesized and crosslinked using bis(3-ethyl-5-methyl-4-maleimidophenyl)methane (BIM) through the Diels-Alder reaction, and are applied to cellulosic substrates such as cotton cloth (CC), where SMA and FMA refer to stearyl methacrylate and furfuryl methacrylate, respectively. The coated CC demonstrates a water contact angle (WCA) of >150° and sliding at 10°, indicating superhydrophobicity. These coated CC show strong potential for oil-water separation and message encryption in anti-counterfeiting applications. Additionally, the coatings exhibit thermo-responsive scratch-healing behavior at 140°C and possess anti-staining capabilities. The coating also maintains stability across a wide range of temperatures, chemical environments, and under abrasion. This smart and sustainable textile platform is poised to benefit a range of industries-from oil remediation to functional textiles.