Tea‐polyphenols mediated interfacial modifier to integrate reinforcement, reprocessability, and shape memory properties into rubber/carbon black composites via coordination bonds

Abstract Carbon blacks are important fillers to reinforce, functionalize rubber materials and reduce their prices. However, environment‐friendly surface modification of carbon blacks is not trivial to conduct, yet challenging to effectively sever broad rubber galleries. Inspired by wet adhesion of mussel, tea polyphenols (TPs) are coated on carbon blacks by vacuum absorption method (i.e., TP@C) and then they are mixed into nitrile butadiene rubber with ZnCl₂. Specially, Zn²⁺/TP@C coordination interfaces are formed together with crosslinking structures of Zn²⁺‐CN of NBR after hot pressing. As a sequence, the rubber composites achieve superior strength and modulus reinforcement owing to strong interface interactions and good dispersion of TP@Cs. Reversible coordination crosslinking network and TP@C network topology can be rearranged at elevated temperatures, endowing the composite good plasticity and reprocessablity. Furthermore, the composites possess stable shape memory properties for five cycles and good plasticity based shape memory ability, showing great advantages in application potential of smart material fields.