Buildup of Multi-Ionic Supramolecular Network Facilitated by In-Situ Intercalated Organic Montmorillonite in 1,2-Polybutadiene

The development of a sacrificial bond provided unique inspiration for the design of advanced elastomers with excellent mechanical properties, but it is still a huge challenge to construct a homogenous polar sacrificial network in a nonpolar elastomer. In this effort, we proposed a novel strategy to engineer a multi-ionic network into a covalently cross-linked 1,2-polybutadiene (1,2-PB) facilitated by in-situ intercalated organic montmorillonite (OMMT) without phase separation. XRD, SEM, and TEM analysis were carried out to characterize the microstructure of the resulting polymers. Crosslinking density, dielectric performance, and cyclic tensile tests were used to demonstrate the interaction of zinc methacrylate (ZDMA) and OMMT. The dynamic nature of ionic bonds allowed it to rupture and reform to dissipate energy efficiently. Stretching orientation brought parallelism between polymer chains and OMMT layers which was beneficial for the reconstruction of the ionic network, ultimately resulting in high strength and a low stress relaxation rate. Overall, our work presented the design of a uniform and strong sacrificial network in the nano-clay/elastomer nanocomposite with outstanding mechanical performances under both static and dynamic conditions.