Antiswelling and robust supramolecular polyurea hydrogels induced by the synergy of hydrogen bond and hydrophobic interaction for constructing durable underwater anti‐oil‐fouling coatings.

Hydrogels are attractive materials for constructing underwater antifouling coatings on solid substrates. However, the application of hydrogel coatings usually faces the obstacles of complex preparation process and poor durability. Herein, we present a facile method to prepare durable hydrogel coatings on metal foils based on rationally designed supramolecular polyurea (PU) hydrogels. PU hydrogels are designed to be cross‐linked with hydrogen bonds (H‐bonds) and hydrophobic interactions in the hard segment domains by using dihydrazides with different alkyl spacer lengths ((CH2)m) as chain extender. The synergy of H‐bond and hydrophobic interaction can stabilize H‐bonds in water, as confirmed by Raman spectroscopy. As a result, PU hydrogels exhibit antiswelling capacity and robustness in both deionized water and seawater. Subsequently, PU hydrogel coatings on Cu/Al foils are prepared by convenient brush coating and subsequent swelling. The resulting hydrogel coatings exhibit excellent underwater anti‐oil‐adhesion and self‐cleaning property, and are durable enough to withstand various static and dynamic damaging tests. The good durability of PU hydrogel coatings should be ascribed to the robust adhesion interface and excellent antiswelling capacity of PU hydrogels. The combination of facile preparation and good durability makes PU hydrogel coatings promising candidates for reliable underwater antifouling. [ABSTRACT FROM AUTHOR]