Robust and Flexible Rubber Composite with High Photothermal Properties Achieved by In Situ ZDMA Assisted Dispersion of Eumelanin and its Hydrophobic Photothermal Application

Abstract Eumelanin, a natural, biocompatible, and biodegradable photothermal agent derived from biomass, has attracted increasingly considerable attention due to its outstanding photothermal conversion efficiency. Unfortunately, its tendency to aggregate in flexible non‐polar polymers, owing to its abundant polar groups on the surface, severely restricted the application of eumelanin in photothermal composite field. Herein, a feasible strategy is proposed to disperse eumelanin in non‐polar rubber matrix via in situ generation of Zinc dimethacrylate (ZDMA). The graft‐polymerization of ZDMA promotes the interfacial compatibility between styrene butadiene rubber (SBR) and eumelanin, achieving a uniform dispersion of eumelanin in SBR. The rubber composite exhibits a considerable tensile strength of 11.4 MPa, acceptable elongation at break of 146%, and outstanding photothermal conversion efficiency of up to 75.2% with only 1 wt% of eumelanin. Furthermore, based on the easy‐processing of SBR matrix, the composite is treated with a sandpaper template technique and sprayed with trimethoxy(1H,1H,2H,2H‐perfluorodecyl)silane (PFDTMS) to endow the material with near superhydrophobicity (water contact angle of 147.9°) capacity. Hydrophobicity provides excellent icing resistance, with droplet surfaces extending more than twice as long to freeze. Moreover, this hydrophobic photothermal material exhibits remarkable anti‐frosting, de‐frosting, and de‐icing capabilities.