A Double Cation–π‐Driven Strategy Enabling Two‐Dimensional Supramolecular Polymers as Efficient Catalyst Carriers

The cation-π interaction is a strong non-covalent interaction that can be used to prepare high-strength, stable supramolecular materials. However, because the molecular plane of a cation-containing group and that of aromatic structure are usually perpendicular when forming a cation-π complex, it is difficult to exploit the cation-π interaction to prepare a 2D self-assembly in which the molecular plane of all the building blocks are parallel. Herein, a double cation-π-driven strategy is proposed to overcome this difficulty and have prepared 2D self-assemblies with long-range ordered molecular hollow hexagons. The double cation-π interaction makes the 2D self-assemblies stable. The 2D self-assemblies are to be an effective carrier that can eliminate metal-nanoparticle aggregation. Such 2D assembly/palladium nanoparticle hybrids are shown to exhibit recyclability and superior catalytic activity for a model reaction.