Woven Polymer Networks via the Topological Transformation of a [2]Catenane

Weaving technology has been widely used to manufacture macroscopic fabrics to meet the artistic and practical needs of humanity for thousands of years. However, the fabrication of molecular fabrics with fascinating topologies and unique mechanical properties represents a significant challenge. Herein, we describe a topological transformation strategy to construct woven polymer networks (WPNs) at the molecular level via ring-opening metathesis polymerization (ROMP) of a zinc-template [2]catenane. The key feature of this approach is the exploitation of the pre-existing catenane crossing points that maintain the dense woven structure and the flexible alkyl chains on the [2]catenane that synergistically work with the crossing points to modulate the physicochemical and mechanical properties of the woven materials. As a result, the WPN possesses a certain degree of flexibility and stretchability, as well as high thermostability and mechanical robustness. Furthermore, we could remove the zinc ions to endow the WPN with more degrees of freedom and then enhance its mechanical behaviors by remetalation. This study not only provides a novel strategy toward woven materials with intriguing structural features and emergent mechanical adaptivities, but also highlights that mechanically interlocked molecules could offer unique opportunities for the construction of smart supramolecular materials with peculiar interlaced topologies at the molecular scale.