Interlocked Woven COFs as Molecular Metamaterials with Snap-through and Jamming Mechanics

Interlocking architectures in three-dimensional woven covalent organic frameworks (COFs) induce interesting molecular-scale mechanical responses, programmed through reticular chemistry and topology. Here, we use atomistic simulations to investigate the topology-driven properties of a copper-templated woven framework (COF-500-Cu) and its demetalated analogue (COF-500). The computational analysis indicates that Cu-ligand coordination in COF-500-Cu pins the interlocked ribbon topology, leading to a snap-through behavior under tension. Removal of Cu(I) allows enhanced ribbon mobility while preserving the mechanical interlocking, which becomes increasingly constrained under tension and compression due to a jamming transition. These results highlight that interlocked woven COFs can function as molecular-scale metamaterials, thereby extending their use beyond conventional chemical applications.