Self-Healing, Robust, Liquid-Repellent Coatings Exploiting the Donor–Acceptor Self-Assembly

[Image: see text] Liquid-repellent coatings with rapid self-healing and strong substrate adhesion have tremendous potential for industrial applications, but their formulation is challenging. We exploit synergistic chemistry between donor–acceptor self-assembly units of polyurethane and hydrophobic metal–organic framework (MOF) nanoparticles to overcome this challenge. The nanocomposite features a nanohierarchical morphology with excellent liquid repellence. Using polyurethane as a base polymer, the incorporated donor–acceptor self-assembly enables high strength, excellent self-healing property, and strong adhesion strength on multiple substrates. The interaction mechanism of donor–acceptor self-assembly was revealed via density functional theory and infrared spectroscopy. The superhydrophobicity of polyurethane was achieved by introducing alkyl-functionalized MOF nanoparticles and post-application silanization. The combination of the self-healing polymer and nanohierarchical MOF nanoparticles results in self-cleaning capability, resistance to tape peel and high-speed liquid jet impacts, recoverable liquid repellence over a self-healed notch, and low ice adhesion up to 50 icing/deicing cycles. By exploiting the porosity of MOF nanoparticles in our nanocomposites, fluorine-free, slippery liquid-infused porous surfaces with stable, low ice adhesion strengths were also achieved by infusing silicone oil into the coatings.