Rapid Self‐Healing of Robust Surface‐Tethered Covalent Adaptable Coatings

This work addresses challenges with the robustness of self-healing coatings through the inclusion of surface-tethered covalently adaptable networks (CANs). Surface-initiated polymerization is combined with spray-coating to deposit polymers to produce coatings with reversible crosslinks to the tethered chains. Without this polymer brush layer, the physisorbed CAN coatings fail to self-heal completely, are labile to solvent, and exhibit shear delamination upon scratching. The utility of this tethered coating approach is highlighted through its ability to autonomously self-heal incisions within seconds at elevated temperatures, or more steadily under ambient conditions. The key to these advancements is the use of polymer brushes as a primer layer to attach the CAN to enhance healing and improve the environmental robustness of the coating.