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Self-assembly post-modification has proven to be an efficient strategy to build higher-order supramolecular architectures and functional materials. In this study, we successfully realized the construction of a new family of neutral supramolecular polymeric films containing well-defined metallacycles as the main scaffolds through combination of coordination-driven self-assembly with post-electropolymerization. The obtained neutral polymeric materials were fully characterized by the cyclic voltammogram (CV), SEM, and TEM. The thickness of the films was able to be well regulated by the number of scanning cycles. Moreover, we found that the shape of the metallacycles and the number of triphenylamine moieties played important roles in the formation of the final polymer films. We believe that the introduction of the neutral metallacycles into the final polymer structures not only enriches the library of supramolecular polymeric films but also provides a new platform to study neutral molecule detection, separation, and capture.

Pillarenes (or pillararenes), as a new and rapidly developing class of covalent macrocycles, have stimulated a tremendous upsurge of interest in supramolecular chemistry because of their unique features and potentials in fabricating functional materials. In addition, metallo-supramolecular chemistry has grown steadily over the last few decades. The presence of metal in supramolecular architectures enables the systematic tuning of their properties and endows them with optical, magnetic, and electric etcetera unusual properties. The marriage of these two fields offers new possibilities for the fabrication of novel functional materials and devices. This review article provides an overview of recent advancements on pillararene-based metallic supramolecular assemblies. The fabrication and functionalities of pillararene-decorated metallic macrocycles, metal-organic frameworks (MOFs), and metal nanoparticles are comprehensively summarized and discussed.