Encapsulating Textiles with Dynamic Covalent Networks for Sustainable and Efficient Oil Spill Cleanup

ABSTRACT The development of high‐performance sorbents for oil spill remediation is highly desirable, which now calls for the integration of sustainable design in the context of advancing a circular materials economy. Here, we report a class of textile composites prepared through encapsulating industrially relevant fabrics with dynamic imine networks, which combine exceptional oil removal efficiency with intrinsic chemical recyclability. The dynamic imine networks are synthesized via a one‐pot polycondensation of terephthalaldehyde, isophorone diisocyanate, and a trifunctional amine cross‐linker. When coated onto fabrics such as PET, nylon, cotton, and polyimide, the resulting composites exhibit significant improvements in mechanical strength (8.6‐fold increase in stress at break), surface hydrophobicity (water contact angle of 123° compared to 0°), antifouling resistance, and oil sorption capacity (1.4–16‐fold increases in oil uptake). The high oil removal performance is retained across a broad temperature range (10–50 °C), and can be further improved by increasing the coating concentration, with the maximum sorption of 28.5‐fold the material's weight for silicone oil. Importantly, the coating is chemically recyclable, enabling efficient separation and recovery of both the fabrics and the dynamic networks without loss of material quality.