A biomimetic closed-loop recyclable, long-term durable, extreme-condition resistant, flame-retardant nanocoating synthesized by reversible flocculation assembly.

Flame-retardant coatings have attracted increasing attention in mitigating the fire threat of flammable polymer materials. Their durable application inevitably provides high resistance to various complex environments, however, discarded stable materials will turn into another man-made waste disaster. The paradigm shift toward a sustainable future is to combine durability and recyclability of coatings. Herein, we demonstrate a biomimetic coating that reversibly captures active flame-retardant nanomaterials by flocculation assembly using anionic polyacrylamide covering the polyurethane foam surface. Strong hydrogen bonding and microstructural interlocking provide the coating with high durability under complex harsh conditions (underwater, chemical exposure, hydrothermal aging, long-term external extrusion, ). Meanwhile, the disassembly/reorganization of the coating can be easily repeated in response to pH stimulation with a recycling rate of 97%. The experiments and theoretical calculations reveal the mechanism of the reversible flocculation assembly. This biomimetic strategy of responsive flocculation assembly opens the way for functional coatings with integrated durability and recyclability.