Synergistic interfacial engineering of dynamic coordination and hydrogen bonding enables reprocessable ultra-strong rubber nanocomposites

Abstract

Designing high-strength yet reprocessable rubber materials remains a fundamental challenge, as the inherent weakness of intermolecular interactions constrains dynamic crosslinked networks. Herein, we demonstrate a facile strategy to fabricate ultrahigh-strength, reprocessable, and recyclable rubber composites through interfacial engineering of hydrogenated carboxylated nitrile rubber (HXNBR) with zeolitic imidazolate framework-67 (ZIF-67) crosslinkers. The HXNBR/ZIF-67 composites exhibit an unprecedented tensile strength of 50 MPa, coupled with remarkable durability-retaining 95% of their original strength after five reprocessing cycles. Notably, this mechanical resilience is maintained even in the presence of carbon black (N330) fillers. The composites enable full structural recovery via solvent recycling and demonstrate potential for energy applications. This simple yet effective approach establishes a promising pathway toward development of sustainable high-performance elastomers.