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 ZnCl 2 . Specially, Zn 2+ /TP@C coordination interfaces are formed together with crosslinking structures of Zn 2+ -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.
Vitrimers display great potential for application in various industries thanks to their high strength, reprocessability, and multi‐functions. However, it is still quite a challenge to fabricate rubber vitrimers as the facile designs in reversible crosslinking networks are always critical. Herein, inspired by mussel byssus, heterogeneous coordination networks are constructed in nitrile butadiene rubber (NBR) to develop novel vitrimeric structures composed of metal‐phenolic network (MPN) granules with dense zinc ions (Zn2+)–tea polyphenol (TP) bonds and a soft matrix containing few Zn2+cyano group (CN) coordination bonds. The resulting NBR composites show tunable reinforcement simply by altering the amount of Zn2+ ions. The reversibility of complexations endows the composites with good plasticity, recyclability, and stable shape memory properties. Plasticity at high temperatures changes vitrimeric networks, producing larger and spindle‐like MPN granules owing to their secondary self‐assembly. Despite these variations, the vitrimeric composites still maintain engineering plasticity‐based shape memory properties at a relatively large strain. Therefore, it is believed that the biomimetic strategies can well fabricate rubber composites with high strength, reprocessable, and shape‐memory performance.
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